&EPA
United States       Office of Air Quality       EPA-453/R-00-005
Environmental Protection  Planning and Standards     . June 2000
Agency          Research Triangle Park, NC 2771 1




Deposition of Air Pollutants


to the  Great Waters



Third Report to Congress

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                                ACKNOWLEDGMENTS

       The report was prepared by the Office of Air Quality Planning and Standards of the U. S.
Environmental Protection Agency (EPA). The Project Leads were Gail Lacy and Dale Evarts. Completion
of this report could not have been possible without significant contributions from the wider community of
scientists and environmental experts involved with the programs and issues described in the report.  In
particular, EPA would like to thank those persons who provided peer review of the draft report:
       Mary Ann Allan
       Dr. Caroline Currin
       Elisabeth Galarneau
       Dr. Louis Guillette
       Dr. Michael Murray
                     Electric Power Research Institute, Palo Alto, California
                     National Marine Fisheries Service, Beaufort, North Carolina
                     Atmospheric Environment Service, Ontario, Canada
                     Department of Zoology, University of Florida
                     National Wildlife Federation, Ann Arbor, Michigan
Dr. Hans Paerl Institute of Marine Sciences, University of North Carolina
Dr. Joseph Scudlark   College of Marine Sciences, University of Delaware
       In addition, EPA would like to acknowledge the substantive review and contributions provided by
Richard Artz and Margaret Kerchner of the Air Resources Lab of the National Oceanographic and
Atmospheric Administration, by Bob Larson of the National Atmospheric Deposition Program, and by
many staff of State, local and tribal agencies.

       Within EPA, we would like to acknowledge the contributions of the Agency work group members
and others involved in the development of the report, including staff (too numerous to name) in the Offices
Air and Radiation, Water, Research and Development, Solid Waste and Emergency Response, Prevention,
Pesticides, and Toxic Substances, and General Counsel, as well as in the Great Lakes National Program
Office, the Chesapeake Bay Program Office, the Gulf of Mexico Program Office, EPA Regions IV and V,
and the National Estuary Program.
                                            Cover photo credits:
                                            S.C. Delaney/EPA
                                                              S.C. Delaney/EPA
                                            S.C.
                                            Delaney/EPA
                                                  S.C. Delaney/EPA
Carole Y. Swinehart/
Michigan Sea Grant
Extension
                                                         S.C. Delaney/EPA

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                                                                                       Errata
                                        ERRATA
Page II-7, Table II-l, Rows 8 and 12:

"Chlor-alkali" row (Row 8) should be removed because it is a duplicate with Row 5, "Chlor-alkali
Production."  "Others (<1 percent each)" row (Row 12) should be revised to read 10 tons/year and <
percent. The  corrected table is included below.

                                          Table 11-1
                      National Anthropogenic Mercury Air Emissions
                      (Based on 1994-1995 Inventory; U.S. EPA 1997e)
Source Category
Utility boilers: coal combustion, oil, and natural gas
Municipal waste combustion
Commercial/industrial boilers: coal and oil
Medical waste incineration
Chlor-alkali production
Hazardous waste combustors
Portland cement, excluding hazardous waste-fired
Residential boilers: oil and coal
Pulp and paper manufacturing
Others (<1 percent each) a
Total U.S. Anthropogenic Mercury Air Emissions
1994-1995
Anthropogenic Air
Emissions (tons/year)
52
30
28
16
7
7
5
4
2
10
158b'c
Percent Contribution to
Total U.S. Anthropogenic
Air Emissions
33
19
18
10
4
4
3
2
1
6
100b,c
1A list of the source categories that contribute less than 1 percent to total U.S. emissions is provided in Appendix B.
b This value represents anthropogenic mercury air emissions in the U.S. only.
0 Values do not add exactly due to rounding.
Page 11-51, Paragraph 3, Sentences 4 and 5:

Replace original sentences with revised sentences provided below. Also, one new reference should be
added, and one reference should be revised.

Original Text:  "It should be noted, however, that ADN accounts for roughly only 1 percent of nitrogen
              loadings  in the Mississippi River basin, which has highly diverse sources of
              anthropogenic nitrogen (Goolsby et al. 1998, as cited by Paerl 1999).  The ADN is also
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Errata
Revised Text:
likely to be a relatively less important contributor to nitrogen loadings in Pacific coast
Great Waters than is the case in the east and Gulf coast areas, due to the prevailing
westerly winds over Pacific coastal waters and their watersheds, originating from
unpolluted ocean areas."

"In the Mississippi River basin, ADN accounts for at least 10 percent of nitrogen
loadings in the Mississippi River basin, which has highly diverse sources of
anthropogenic nitrogen (Goolsby et al. 1999; Alexander et al. 2000).  The ADN is likely
to be a relatively less important contributor to nitrogen loadings in Pacific coast Great
Waters than is the case in the east and Gulf coast areas, due to the prevailing westerly
winds over Pacific coastal waters and their watersheds, originating from unpolluted
ocean areas."
New Reference:                     :

Alexander, R.B., R.A. Smith, and G.E. Schwarz. 2000. Effects of stream channel size on the delivery of
nitrogen to the Gulf of Mexico. Nature.  403:758-761.

Revised Reference:

Goolsby, D.A., W.A. Battaglin, G.B. Lawrence, R.S. Artz, B.T. Aulenbach, R.P. Hooper, D.R. Kenney,
and G.J. Stensland. 1999. Flux and sources of nutrients in the Mississippi-Atchafalaya River Basin.
Topic 3 Report for the Integrated Assessment on Hypoxia in the Gulf of Mexico: NOAA Coastal Ocean
Program, Decision Analysis Series No. 17.
Page 2
      Deposition of Air Pollutants to the Great Waters - 3  Report to Congress 2000

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                           EXECUTIVE  SUMMARY
       With section 112(m) of the 1990 Clean Air Act (CAA), Congress directed the U.S.
Environmental Protection Agency (EPA), in cooperation with the National Oceanic and Atmospheric
Administration (NOAA), to identify and assess the extent of atmospheric deposition of air pollutants to
the Great Lakes, the Chesapeake Bay, Lake Champlain, and coastal waters, collectively known as the
Great Waters.  Further, section 112(m) directed EPA to report its findings to Congress in periodic
reports. This is EPA's third Report to Congress on the deposition of air pollutants to the Great Waters.
The first report was published in May 1994, and the second report was published in June 1997.

       The goals of the Third Great Waters Report to Congress are to discuss the current state of
knowledge regarding atmospheric deposition of pollutants to the Great Waters based on new research
and program activities undertaken since the Second Report to Congress and to describe any necessary
revisions to requirements, standards, and limitations under the CAA or other Federal laws. This report is
not intended to be a comprehensive summary of all relevant scientific research and activities. Instead, it
summarizes and highlights major trends and key findings, and builds on conclusions presented in the
First and Second Reports to Congress.

How does deposition  of air pollutants affect public health and the
health of the Great Waters ecosystems?
       A rapidly growing number of atmospheric
deposition monitoring and modeling studies confirm
that, along with runoff and discharges of pollution into
waterways, atmospheric deposition is a significant
pathway of pollutant inputs to the Great Waters. These
studies show that the contribution of atmospheric
deposition to overall pollutant loadings varies greatly by
pollutant and location.  For example, studies show that
atmospheric deposition contributes from less than 5 to
100 percent of dioxins and furans entering the Great
Lakes, depending on the location of the monitoring site,
and from 2 to 38 percent of the nitrogen load to certain
coastal waters. Given this variability in contributions,
the improvement of the quality of the Great Waters
environments requires an understanding of all of the
sources of the pollutants into a waterbody, including
runoff from urban areas and farms, discharge from point
sediments, as well as atmospheric deposition.
       Great Waters Pollutants of Concern

    Cadmium and cadmium compounds
    Chlordane
    DDT/DDE
    Dieldrin
    Hexachlorobenzene
    a-Hexachlorocyclohexane
    Lindane (v-hexachlorocyclohexane)
    Lead and lead compounds
    Mercury and mercury compounds
    Polychlorinated biphenyls
    Polycyclic organic matter
    Tetrachlorodibenzo-p-dioxin (dioxins)
    Tetrachlorodibenzofuran (furans)
    Toxaphene
    Nitrogen compounds
sources, and seepage from contaminated
       Like the First and Second Reports to Congress, this report focuses on 15 pollutants of concern,
including certain pesticides, metal compounds, chlorinated organic compounds, and nitrogen compounds
(see sidebar). Some of these pollutants are single compounds while others represent categories of several
or even hundreds of individual compounds. They are emitted into the air by a wide range of sources,
including industries and other human activities, natural sources, and re-emissions of these pollutants from
soil and water. What is known about their emission rates, concentrations in the environment,
transformation processes, deposition rates and pathways, and health and environmental effects varies
widely. Nevertheless, recent research has added to our knowledge of the adverse human health and
ecological effects of these pollutants. At certain levels, these pollutants are associated with adverse
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Executive Summary
effects on many target organs in humans and animals, including the liver, kidney, nervous system,
endocrine system, reproductive organs, and immunological system. Research since the Second Report to
Congress provides additional evidence that some of the pollutants are likely "endocrine disrupters,"
meaning they may interfere with the action of hormones in wildlife and humans.

       A number of regional and national assessments and monitoring programs described in this report
suggest that, while environmental conditions are improving in general, the current concentrations of
pollutants of concern continue to impair the ecological health of many Great Waters. For example, the
NOAA Estuarine Eutrophication Surveys indicate that approximately 89 percent of the Great Waters that
are coastal estuaries show some degree of adverse effects associated with amounts; of nitrogen in excess
of natural levels.  (Nitrogen is a natural component of these waterbodies, but excess amounts can also be
introduced through natural and human activities such as runoff from urban and agricultural areas and
atmospheric deposition.) Because of long-range atmospheric transport and certain chemical properties
(e.g., persistence, mobility, bioaccumulation, and bioconcentration), the pollutants of concern may
contribute to ecological impairment far from known emission sources and long after releases.

       At current levels of contamination, pollutants of concern in the Great Waters pose potentially the
greatest health risks to individuals who consume fish from contaminated waters for subsistence or
cultural reasons, women of child-bearing age, the developing fetuses of pregnant women, and young
children who consume fish from contaminated waters. For mercury in particular, exposures do not
appear to pose a health risk to people consuming average amounts of fish, but sensitive sub-populations
(e.g., young children, and pregnant women and their developing fetuses) with higher than typical fish
consumption may be at risk.  Also at risk are subsistence fish-eating populations who consume large
amounts offish. The extent of risk for these groups depends on the amount offish consumed and the
mercury concentrations present in the fish.                                  :

What  are the recent and anticipated trends  in emission and
deposition  of Great Waters pollutants of concern and their
concentrations in the Great Waters environment?

       Where monitoring trends information exists, either nationally or locally, atmospheric deposition
of pollutants of concern to the Great Waters has declined or remained relatively constant in recent years,
as described in Chapter n.  Specifically, deposition of lead, cadmium, polycyclic organic matter (POM) -
which includes a group of compounds known as polycyclic aromatic hydrocarbons (PAHs) -
polychlorinated biphenyls (PCBs), and some banned or restricted use pesticides is declining in the Great
Lakes. Other Great Waters have also shown decreasing trends of some of the pollutants of concern, such
as lead in Long Island Sound. Deposition of nitrogen in the U.S. has remained fairly constant. These
trends may reflect the results of emission reduction programs established under the CAA, pesticide bans,
as well as other local, tribal, State, Federal, and international pollution control efforts, many of which are
described in this report. There is considerable uncertainty in the trends estimates, however, because
limited monitoring capability, technological barriers, and variable collection and analysis methods make
it difficult to adequately characterize historical or current conditions.  In addition, these estimates do not
address all Great Waters waterbodies for all pollutants of concern.

       Emissions of mercury to the atmosphere come from human-made sources, natural emissions, and
re-emission from biologic and geologic processes. Emissions of mercury have been on a downward trend
since 1990, due chiefly to the phase-out of mercury in many products.  Nevertheless, monitoring suggests
that atmospheric deposition is a significant contributor of mercury to the Great Waters. At EPA's current
reference dose for mercury, levels in some lakes and streams remain sufficiently high to pose adverse
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                                                                            Executive Summary
 human health and ecological risks and to result in fish consumption advisories for mercury in many Great
 Waters.

        Lead air emissions, ambient air concentrations, and deposition levels in the Great Lakes region
 have also decreased in recent years.  Cadmium emissions in the Great Lakes region, on the other hand,
 increased in the 1980s and have not shown a trend since then, while cadmium deposition in the Great
 Lakes region is believed to have decreased in recent years. In the Chesapeake Bay, trends in atmospheric
 deposition of lead and cadmium are difficult to discern with current information, but total inputs of both
 lead and cadmium in some eastern parts of the bay have increased in recent years due to the increase in
 population and industrial activities. In some areas of the Chesapeake Bay, levels of these metals may be
 high enough in sediments to cause adverse ecological effects.

        Air emissions of dioxins, furans, and POM (including PAHs) in the U.S. are from both natural
 and human-made combustion and incineration processes.  Emissions have declined for dioxins and
 furans, while trends for POM are not known. A large degree of variation has been observed in deposition
 levels  of dioxins and furans over time within and between the Great Lakes.  Deposition levels of these
 compounds are related to the pattern of industrialization and population density. In many instances, long
 term monitoring indicates that concentrations of dioxins and furans in biota in the Great Waters have
 declined over time.  Analytical results indicated that levels in aquatic species are declining steadily and
 in several Great Waters, no dioxin was found in fish samples taken between 1987 and 1994.

        Although CAA programs have had a major impact on nitrogen oxide (NOJ emissions, the
 emission reductions have been balanced approximately equally with emission increases attributable to
 economic growth, resulting in a relatively flat trend since 1980. Deposition monitoring data suggest that
 the deposition rates of inorganic nitrogen (e.g., NOX, ammonia) to many of the Great Waters watersheds
 have also been relatively constant for the past two decades, though some increases have been noted
 downwind of areas where population or livestock operations are growing. The EPA expects that
 additional NOX  controls to be implemented under the CAA will slightly outpace emission increases
 associated with economic growth, resulting in a net decreasing trend in NOX emissions through 2005.
 Emissions are expected to remain steady at that level until 2010.  Research is ongoing into the lesser
 known, but apparently important, forms of nitrogen deposition (e.g., dry deposition, organic nitrogen).
 Current and anticipated nitrogen deposition rates are significantly greater than natural rates, and
 combined with nitrogen inputs from runoff from farms and cities, have the potential to overwhelm the
 capacities of surface waters to assimilate the additional nitrogen.

       Manufacture of PCBs in the U.S. no longer occurs; however, releases into the environment
 continue to occur because of PCBs in electrical transformers and capacitors that are still in use, releases
 from soils and sediments contaminated with PCBs, and releases during some combustion processes. The
 number and magnitude of PCB  sources in the U.S. has decreased 20-fold in the past 20 years.
 Furthermore, deposition of PCBs in the Great Lakes has decreased and a net loss of PCBs has been
 observed in the  Chesapeake Bay. Overall, PCB concentrations in the environment appear to have
 declined but are still present and continue to result in the need for fish consumption advisories in many
 Great Waters.

       Based on recent academic research on atmospheric pollutant concentrations in the Great Lakes
 region, DDT and DDE, followed by dieldrin and chlordane, are estimated to fall below current detection
 limits in the atmosphere between 2010 and 2020. Hexachlorocyclohexane and hexachlorobenzene are
 projected to be eliminated in the atmosphere by 2030 and 2060, respectively. These estimates assume
 current rates of long-range transport of these pollutants into the region and do not mean that
 concentrations would be eliminated in deposited media (water and sediments) by these dates. However,
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Executive Summary
these estimates indicate that reduction strategies in the Great Lakes, along with the original bans and
restrictions on the use of these substances, are having the intended effect.

What actions are EPA and others taking to address atmospheric
deposition?

       Chapter IE of this report describes more than 60 programs under way from the local to
international levels that directly or indirectly contribute to reducing atmospheric deposition of pollution
to the Great Waters or to understanding its effects. Although EPA leads or supports many of these
programs, which often use multimedia and cross-program approaches to control pollution, other Federal
agencies, State and tribal organizations, industry groups, and Canada have also initiated and implemented
many important activities. Examples of EPA's cross-program and multimedia approaches include the
pulp and paper industry "cluster rule" that for the first time integrates, coordinates, and streamlines
applicable requirements of the Clean Water Act and the CAA.  The EPA's air and water programs are
also working together to address the contribution of air deposition into water quality protection under
total maximum daily load (TMDL) determinations. This also includes coordinated activities such as the
Persistent Bioaccumulative Toxics Initiative, Clean Water Action Plan, and Contaminated Sediment
Management Strategy.  Several State organizations have successfully worked with industry and
municipalities to develop pollution prevention programs and programs to collect banned and restricted
use pesticides.  Tribes are working to reduce exposure of indigenous populations to pollutants of concern
through a variety of efforts, and industry has initiated efforts to reduce the use of pollutants of concern in
products and processes. Canada has implemented a variety of programs, some of which are joint efforts
with the U.S., like the Binational Toxics Strategy which seeks to  eliminate pollutants of concern from the
Great Lakes environment.

       These coordinated Agencywide efforts demonstrate EPA's commitment to implement the
strategic directions discussed in the First and Second Reports to Congress and in the section 112(m)(6)
adequacy determination, and to pursue all authorities available for addressing atmospheric deposition and
Great Waters pollutants of concern.  In addition, developing and implementing these and other programs
and initiatives described in this report have not required revisions to requirements,' standards, and
limitations in accordance with the CAA and other Federal laws which provide protection of human health
and the environment from atmospheric deposition to the Great Waters.

What  are EPA's findings and conclusions from this Third Report
to Congress?

       The new scientific and programmatic information presented in this report supports and builds on
the three  broad conclusions presented in the First and Second Reports to Congress.

•      Atmospheric deposition from human activities can be a significant contributor of toxic  chemicals
       and nitrogen compounds to the Great Waters. The relative importance of atmospheric loading
       for a particular chemical in a given waterbody depends on many factors, including characteristics
       of the waterbody, properties  of the chemical, and the kind and amount of atmospheric or water
       discharges.

•      A plausible link exists between emissions into the air of Great Waters toxic pollutants of
       concern, the atmospheric deposition of these pollutants (and their transformation products), and
       the concentrations of these pollutants found in water, sediments and biota; especially fish and
       shellfish.  For mercury, fate and transport modeling and exposure assessments predict that the
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                                                                             Executive Summary
        anthropogenic contribution to the total amount of methylmercury in fish is, in part, the result of
        anthropogenic mercury releases from industrial and combustion sources increasing mercury body
        burdens (i.e., concentrations) in fish. Furthermore, the consumption offish is the dominant
        pathway of exposure to methylmercury for fish-consuming humans and wildlife. However, what
        is known about each stage of this process varies with each pollutant (for instance, the chemical
        species of the emissions and its transformation in the atmosphere).

 •       Airborne emissions from local as well as distant sources, both within and outside the U.S.,
        contribute pollutant loadings to waters through atmospheric deposition.  Determining the relative
        roles of particular sources- - local, regional, national, and possibly global, as well as
        anthropogenic, natural, and re-emission of pollutants — contributing to specific waterbodies is
        complex, requiring careful monitoring, atmospheric modeling, and other analytical techniques.

        Actions taken by EPA and others to control sources of Great Waters pollutants of concern appear
 to have positively affected trends in pollutant concentrations measured in air, water, sediment, and biota.
 Overall deposition rates of pollutants of concern have declined slightly or remained constant.  Several
 pollutants of concern continue to enter the Great Waters primarily through atmospheric deposition.  In
 addition, long-range  transport of pollutants of concern from other U.S. regions or other countries is
 estimated to contribute significantly to atmospheric loadings to the Great Waters. For example, the
 global reservoir of mercury (which includes mercury from both U.S. and foreign sources) is estimated to
 contribute about 40 percent of the total mercury deposition to U.S. lands and waters.

        Concentrations of some pollutants of concern in the water, sediment, and biota  of the Great
 Waters declined in recent years, whereas others were constant or variable. Concentrations of most
 pollutants of concern still pose potential adverse ecological and human health effects. For example,
 approximately 5 percent of the Nation's coastal and inland watersheds include "areas of probable
 concern," meaning a watershed that is associated with a certain number of monitoring sites with sediment
 contamination at levels likely to cause adverse effects.  Water quality data also indicate that water quality
 standards in place for drinking water supplies in the Great Waters are not being exceeded for the
 pollutants of concern, but that surface water quality guidance and criteria are being exceeded for some of
 the Great Waters. In addition, nationally, fish consumption advisories were in place for 39 of 56 Great
 Waters waterbodies as of 1997.

        Based on current trends, EPA expects atmospheric deposition to remain a significant source of
 several pollutants of concern to the Great Waters for the foreseeable future.  In addition, because of the
 ability of these pollutants to persist and bioaccumulate, they are expected to remain in the water,
 sediments and biota for much longer.

        Implementation of existing EPA regulations is expected to further reduce emissions of mercury,
 NOX, POMs, dioxins  and furans, cadmium, and hexachlorobenzene. The EPA continues to'implement
 programs under CAA authorities and expects that pollutant emissions will be further controlled by
 several rules scheduled to take effect in coming years. As a result, atmospheric deposition and loadings
 of these pollutants may be significantly reduced. In addition, actions taken to voluntarily reduce
 chemical use, implement pollution prevention initiatives, advance technology (e.g., alternative fuel
 vehicles), and implement pollution control laws issued by States and other nations will further reduce
 pollutant loadings to  the Great Waters.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Executive Summary
What future directions will EPA follow to implement section
       The EPA developed six key recommendations that will assist in meeting the objectives and
requirements of the CAA related to the Great Waters program.

•      The EPA will continue to support the maintenance and expansion of efforts to monitor Great
       Waters pollutants of concern in order to evaluate the relative contributions of local, regional, and
       long-range transport to deposition in the U.S., as well as natural versus human-made sources.

•      The EPA will continue to develop and implement regulations and pollution prevention programs
       regionally and nationally, including multimedia programs, in order to reduce the impact of
       sources of Great Waters pollutants of concern within the U.S.

       For Great Waters pollutants emitted by sources outside the U.S., EPA will work within
       international frameworks to reduce sources of these pollutants.

       The EPA will support model development and research that establish and clarify the linkages
       from emissions to atmospheric deposition to waterbody loadings to adverse public health and the
       environmental effects of Great Waters pollutants of concern in order to enable effective risk
       management decisions.

•      The EPA will encourage and support the establishment of common baselines and measures of
       progress in order to better assess trends and health of Great Waters and other waterbodies
       affected by atmospheric deposition.

       The EPA will work to increase public awareness of risks of exposure to Great Waters pollutants.

       These key recommendations build on the strategic themes identified in the First and Second
Reports to Congress: (1) continued implementation of the CAA to directly control emissions of Great
Waters pollutants of concern; (2) use of an integrated multimedia approach throughout the Agency,
including coordination of clean air programs with programs available under other Federal laws (e.g.,
Clean Water Act); and, (3) continued support of research activities that address the goals of the Great
Waters program.

       In support of the first strategic theme, EPA will develop or assess the need for new rules and
programs under the CAA, including maximum achievable control technology (MACT) standards, section
 1 12(c)(6) standards, as well as standards that could stem from the residual risk program, the utility air
toxics determination, and the integrated urban air toxics strategy.  As appropriate, EPA will consider the
impacts of atmospheric deposition in developing standards under these authorities:  In addition, EPA will
ensure the timely implementation of NOX control programs already in place and will encourage
innovative, nonregulatory approaches to reducing NOX emissions and other sources of atmospheric
nitrogen.

       This report describes a number of multimedia and cross-program initiatives (e.g., Clean Water
Action Plan, Persistent Bioaccumulative Toxics Initiative) that are in line with EPA's second strategic
theme for the Great Waters program.  Some of these initiatives, such as the pulp and paper cluster rule,
will produce tangible environmental benefits within the near future. Other initiatives, such as
development of multimedia models in support of TMDL determinations and completion of the
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                                                                              Executive Summary
 Contaminated Sediment Non-point Source Inventory, will provide tools and data resources that will help
 EPA target future pollution control activities.

        There has been substantial progress in research activities relevant to the Great Waters program
 since the Second Report to Congress.  However, important information gaps remain, and there are critical
 limitations to current atmospheric monitoring and modeling capabilities. Consistent with the third
 strategic theme, therefore, EPA will initiate and continue to support scientific research to fill these
 critical gaps, including the following activities:

 •       Support research to examine and quantify the ecological effects of atmospheric deposition and to
        better quantify the water quality benefits of air pollution controls;

 •       Expand the geographic coverage and consistency of waterbody monitoring to enable more
        accurate characterizations of the extent of contamination and ecosystem effects due to
        atmospheric deposition;

        Encourage and support interagency coordination to better quantify the indirect loadings of
        atmospheric deposition to the Great Waters through the development of tools that can quantify
        watershed transport of pollutants of concern;

        Continue to support the development of modeling tools which address the transport and fate of
        pollutants in ecosystems and characterize risk, including research to clarify mechanisms of
        mercury methylation so as to better predict and manage ecosystems at risk;

 •       Develop reliable approaches for quantifying and monitoring nitrogen dry deposition and wet
        organic nitrogen deposition;

        Support joint work with States and industry to fill gaps in emissions information for MACT
        source categories and further refine emissions measurement methods, inventories, and modeling
        for Great Waters pollutants of concern;

 •       Support research on viable prevention and controls for sources of pollutants of concern;

 •       Encourage and support greater coordination and expansion of monitoring networks to assess
        deposition of pollutants to coastal waters, to assess the contribution of long-range transport to
        deposition in the U.S., and to evaluate the impact of agricultural and urban sources;

        Develop standard methods to monitor pollutants of concern to enable the comparison of data and
        trends analyses;

        Support international efforts to quantify the transboundary contributions of pollutants of concern
        and to share technology, information, and expertise with other countries on reducing releases to
        the environment and on cost-effective alternatives to their use;

 •       Working closely with other EPA and inter-governmental efforts to address, in particular,
        persistent bioaccumulative toxic pollutants, and to identify and evaluate additional pollutants
        which may be of concern to the Great Waters;

 •       Continue research to identify additional endocrine disrupting chemicals and their associated
        effects; and,
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Executive Summary
•      Continue coordination and support of efforts to improve the consistency of fish consumption
       advisories and the awareness and understanding of advisories among populations most at risk to
       exposure to the Great Waters pollutants of concern.                     •

       The EPA is committed to continuing to address air deposition of pollutants into the Nation's
waters as a priority matter. To that end, and to assure continued coordination of the many related tasks
involved and outlined in this report, EPA will develop a detailed biennial work plan for implementation
actions beginning this year and updated every two years. As EPA develops and implements plans,
programs and initiatives with NOAA and its other Federal, State, tribal, industry and community
partners, we expect to make significant, measurable progress toward our goal of assuring the protection
of human health and the environment from adverse effects attributable to atmospheric deposition of
pollution to the Great Waters.
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                           TABLE OF CONTENTS
                                                                                   PAGE
ACKNOWLEDGMENTS

EXECUTIVE SUMMARY	i

LIST OF TABLES	xii

LIST OF FIGURES	xiv

LIST OF ABBREVIATIONS AND ACRONYMS	 xv

I.     INTRODUCTION AND BACKGROUND	1-1
       A. Overview of the Great Waters Program	1-3
              Definition of Great Waters  	1-3
              Program Participants and Organizations	1-3
              Government Goals Supported by the Great Waters Program and Its Partners	1-6
       B. Pollutants of Concern	1-7
       C. Goals of the Third Report to Congress	1-13

II.     ENVIRONMENTAL PROGRESS	  II-l
       Pollutant-Specific Changes	  0-3
              Mercury and Compounds	  H-4
              Other Metals (Lead and Cadmium)	  11-19
              Combustion Emissions	  II-31
              Nitrogen and Compounds  	  11-40
              Banned and Restricted Use Substances	  11-58
       Cross-Pollutant Trends	  II-67
              Fish Consumption Advisories ..	  11-68
              Water Quality Assessments	  11-69
              NOAA's National Status and Trends Program	  11-70
              National Sediment Quality Survey  	  11-73
              Chesapeake Bay Program  	  11-73
              Lake Champlain Sediment Toxics Assessment Program 	  11-75
              San Francisco Estuary Regional Monitoring Program for
                     Trace Substances  	  II-76

III.    MAJOR PROGRAMS AND ACTIVITIES	HI-1
       A. National Programs and Activities	ni-3
              Multimedia Activities 	ni-4
              Hazardous Air Pollutant (HAP) Controls  	III-l 1
              Stationary Source Controls Addressing NOX	111-17
              Mobile Source Program Activities  	111-29
              Ozone and PM NAAQS and Proposed Regional Haze Rule	111-30
              Other National Programs	111-30
       B.  Regional and Waterbody-Specific Programs  	111-34
              Great Lakes Program	 IH-35
              Lake Champlain Basin Program  	111-37
              Chesapeake Bay Program 	111-38
              Gulf of Mexico Program	111-41
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              National Estuary Program	111-42
              NOAA Activities	HI-48
              Ozone Transport Commission (OTC)	111-49
       C. State, Local, and Tribal Activities	IH-51
              State and Local Activities 	111-51
              Tribal Activities	111-60
       D. Industry Activities	111-63
              Chlor-alkali Industry Mercury Reduction Goal	111-63
              Voluntary Mercury Agreement with Northwest Indiana Steel Mills  	111-64
              American Hospital Association MOU	:	111-64
              Electric Power Research Institute Studies	'•.	111-65
       E. Work with Other Countries	HI-66
              Canada-U.S. Binational Toxics Strategy	111-66
              International Joint Commission	;	111-69
              United Nations Economic Commission for Europe LRTAP Protocols
                     on Heavy Metals and POPs  	111-70
              United Nations Environment Program Global POPs Initiative	111-71
              NAFTA Commission on Environmental Cooperation Sound Management
                   of Chemicals Program	111-71
              U.S.-Canada Air Quality Agreement	in-72

IV.    SCIENCE AND TOOLS . . .	IV-1
       What Major Advancements Have Occurred Since  the Second Report?	IV-2
              Emission Inventories	IV-2
              Ambient Air and Deposition Monitoring Networks  	!	IV-4
              Other Environmental Monitoring Networks and Databases	:	IV-8
              Environmental Transport and Fate  	IV-11
              Measuring and Monitoring Techniques	IV-20
              Exposure and Effects Research	IV-21

V.     NEXT STEPS FOR THE GREAT WATERS PROGRAM	  V-l
       A. Pollutant Sources  	  V-4
              Findings and Conclusions 	  V-4
              Recommendations for Continued and Further Action	  V-5
       B. Contribution of Atmospheric Deposition to Pollutant Loadings in the Great Waters ....  V-8
              Findings and Conclusions 	  V-8
              Recommendations for Continued and Further Action	 V-10
       C. Environmental and Public Health Effects	:	,	 V-l 1
              Finding and Conclusions	 V-l 1
              Recommendations for Continued and Further Action	V-l2
       D. Exceedances of Water Quality or Drinking Water Standards	 V-14
              Finding and Conclusions	'	 V-14
              Recommendations for Continued and Further Action	 V-14
       E. Summary and Key Recommendations	:	 V-16

REFERENCES

INDEX OF WATERBODIES
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                                                                       Table of Contents
APPENDIX A:

APPENDIX B:


APPENDIX C:

APPENDIX D:
Major Sources of Information - Publications and Internet Sites

Detailed Breakdown of Air Emissions Inventory by Pollutant for Source
Categories Emitting Less than One Percent of Total U.S. Emissions

Fish Consumption Advisories Issued for the Great Waters

Names of Numbered Sites from Figure 11-17: Locations of Watersheds
Designated as Areas of Probable Concern
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Table of Contents
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                                   LIST OF TABLES

 CHAPTER I                                                                          PAGE

 Table 1-1:      Uses/Sources and U.S. Regulatory Status of Great Waters Pollutants of
                  Concern	I_9
 Table 1-2:      EPA Multimedia and Cross-program Management of the Great Waters
                  Pollutants of Concern	1-10
 Table 1-3:      Great Waters Pollutants of Concern Addressed by Selected Waterbody, Regional,
                  and International Activities	1-12

 CHAPTER II

 Table II-1:     National Anthropogenic Mercury Air Emissions 	 n-7
 Table II-2:     Preliminary Estimates of Total Atmospheric Mercury Deposition to
               Lake Michigan	  H-13
 Table II-3:     Mercury Sources Identified in Mass Balance Studies (By Percent Contribution)  ..  11-14
 Table II-4:     National Anthropogenic Lead Air Emissions  	  11-23
 Table II-5:     National Anthropogenic Cadmium Air Emissions 	  11-25
 Table II-6:     Trace Metals Inputs to the Chesapeake Bay	  11-26
 Table II-7:     Direct Atmospheric Deposition of Lead and Cadmium to Massachusetts
                  Bay	  n-27
 Table II-8:     Temporal Changes in Metal Concentrations in Chesapeake Bay
                  Tributaries Based on Sediment Cores	  11-29
 Table II-9:     Cadmium and Lead in Sediments of the Chesapeake Bay Mainstem	  11-30
 Table 11-10:    Lead and Cadmium in Horseshoe Crab Eggs from Delaware Bay	  11-30
 Table 11-11:    National Anthropogenic Dioxin and Furan TEQ Air Emissions	  11-32
 Table 11-12:    Current Rates of Dioxins and Furans Accumulation in Great Lakes
                  Sediments  	  H-33
 Table 11-13:    Modeled Air Deposition, Depositional Flux, and Waterborne Inputs of Dioxins
                  and Furans to the Great Lakes	  11-33
 Table 11-14:    National Anthropogenic 16-PAH Air Emissions	  11-35
 Table 11-15:    Sum of Wet and Dry Deposition of PAHs onto Massachusetts Bay  	  11-38
 Table 11-16:    Estimates of PAH Inputs to the Chesapeake Bay  	  11-39
 Table 11-17:    Annual PAH Inputs to and Losses from the Chesapeake Bay	  11-39
 Table 11-18:    Common Forms of Atmospheric Nitrogen 	  II-42
 Table 11-19:    Transfer of Atmospheric Deposition Nitrogen (ADN) from Various Watershed
                  Areas	  H-52
 Table 11-20:    Transfer of Atmospheric Deposition Nitrogen (ADN) from Watersheds to
                  Several Bays and Estuaries	  H-52
 Table 11-21:    Atmospheric Nitrogen Loads Relative to Total Nitrogen Loads in Selected
                  Great Waters	  H-53
 Table 11-22:    National Anthropogenic PCB Air Emissions  	  11-59
 Table 11-23:    IADN Loading Estimates of PCBs (wet and dry) for the Great Lakes	  11-60
 Table 11-24:    IADN Loading Estimates of DDT (wet and dry) to the Great Lakes  	  11-64
 Table 11-25:    Current and Maximum Rates of Toxaphene Accumulation in Great Lakes
                  Sediments  	  H-66
 Table 11-26:    Modeled Air Deposition, Depositional Flux, and Waterborne Inputs of HCB to
                  the Great Lakes	  11-67
 Table 11-27:    Trends of Pollutant Concentrations in Mussel Watch Project (1986-1996)	  11-72
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List of Tables
                                                                                       PAGE

Table 11-28:    Percentages of 1996 Samples that Exceeded Guidelines in the San
                  Francisco Estuary	 11-76

CHAPTER HI

Table ni-1:    Source Categories With Effective Compliance Dates and Anticipated Reductions
                  of HAP Emissions	HI-11
Table III-2:    Proposed and Final Rules Affecting Pollutants of Concern	Ill-13
Table III-3:    Emission Reductions Expected from Control Equipment Used to Retrofit A
                  Typical Existing MWC Plant	in-17
Table III-4:    Emission Reductions Expected from Existing HMIWI	,	Ill-18
Table III-5:    Emission Reductions Expected at New HMIWI after 5 Years of NSPS
                  Implementation .	• • • • HI-19
Table III-6:    Recent Regulations Affecting Stationary Source NOX Emissions	111-20
Table III-7:    Pounds of Pesticides Collected through Clean Sweep Programs
                  Nationwide  	111-57
Table III-8:    U.S. BNS Challenge Goals and Activities for Level I Substances 	111-68
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                                LIST OF FIGURES
CHAPTER I
  PAGE
Figure 1-1:     Pollutant Transport Pathways to Waterbodies	1-1
Figure 1-2:     Locations of the Great Waters	1-3

CHAPTER II

Figure II-1:    Atmospheric Release, Transport, and Deposition Processes	 II-2
Figure II-2:    Monitoring Sites of the Mercury Deposition Network - 1999 	 11-10
Figure II-3:    1993 Lead Emissions in the Great Lakes Region 	 11-22
Figure II-4:    1982 Lead Emissions in the Great Lakes Region 	 11-22
Figure II-5:    1993 Cadmium Sources in the Great Lakes Region 	 11-23
Figure II-6:    Chesapeake Bay Tidal and Non-tidal Waters  	 11-26
Figure II-7:    LADN Loading Estimates of B[a]P to the Great Lakes	 11-37
Figure II-8:    National NOX Emission Trends, 1985-1996 		 11-45
Figure II-9:    1996 NOX Emissions by State  	 H-46
Figure 11-10:   1996 National Anthropogenic NOX Emissions by Principle Source
                  Category  	 11-45
Figure II-11:   Estimated Nitrogen Emissions to Air by Principle Source Category in North
                  Carolina - Anthropogenic and Biogenic	 11-47
Figure 11-12:   Estimated Inorganic Nitrogen Wet Deposition, 1997 	 11-48
Figure 11-13:   Nitrogen Wet Deposition in the Chesapeake Bay Watershed	 11-50
Figure 11-14:   Nitrogen Wet Deposition in the Great Lakes Watersheds	 11-50
Figure 11-15:   Nitrogen Wet Deposition in the Lake Champlain Watershed	 11-50
Figure 11-16:   Expected Year that Great Waters Pesticides will be Below Current Detection
                  Limits in the Great Lakes Atmosphere	 11-64
Figure 11-17:   Locations of Areas of Probable Concern Within Watersheds	 11-74

CHAPTER III

Figure III-l:   Projected National NOX Emission Trends, 1996-2010  	HI-19
Figure III-2:   The 43 Areas of Concern in the Great Lakes Basin 	111-36

CHAPTER IV

Figure IV-1:    Monitoring Sites of Ambient Air and Deposition Monitoring Networks Measuring
                  Pollutants of Concern  	IV-5
Figure IV-2:   Revised Principal Airshed for the Chesapeake Bay 	IV-15
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List of Figures
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                 ABBREVIATIONS AND ACRONYMS

 ADN            Atmospheric deposition nitrogen
 AEOLOS        Atmospheric Exchange Over Lakes and Ocean Surfaces
 AIEO            American Indian Environmental Office
 AILESP          American Indian Lands Environmental Support Project
 AIRMoN        Atmospheric Integrated Research Monitoring Program
 AOC            Areas of concern
 APC            Areas of probable concern
 AQC            Air Quality Committee
 ARL            Air Resources Laboratory
 ATSDR          Agency for Toxic Substances and Disease Registry
 BACT           Best available control technology
 BASMAA        Bay Area Stormwater Management Agencies Association
 BNS            Binational Toxics Strategy
 BRACE          Bay Regional Atmospheric Chemistry Experiment
 CAA            Clean Air Act
 CASTNet        Clean Air Status and Trends Network
 CBADS          Chesapeake Bay Atmospheric Deposition Study
 CBEP            Community-Based Environmental Program
 CBP            Chesapeake Bay Program
 CBPO            Chesapeake Bay Program Office
 CEC            Commission on Environmental Cooperation
 CENR           Committee on Environment and Natural Resources
 CHPAC          Children's Health Protection Advisory Committee
 CMAQ           Community multi-scale air quality
 CTDEP          Connecticut Department of Environmental Protection
 CVAFS          Cold vapor atomic fluorescence spectrometry
 CWA            Clean Water Act
 CZM            Coastal zone management
 DC              District of Columbia
 DDD            1,1 '-(2,2-dichloroethylidene)bis(4-chlorobenzene)
 DDE            1,1 '-(dichloroethenylidene)bis(4-chlorobenzene)
 DDT            1,1 '-(2,2,2-trichloroethylidene)bis(4-chlorobenzene)
 DIN/SRP         Dissolved inorganic  nitrogen to soluble reactive phosphorus
 DNREC          Department of Natural Resources and Environmental Conservation
 EAGLE          Effects on Aboriginals from the Great Lakes Environment
 EDSTAC         Endocrine Disrupter Screening and Testing Advisory Committee
 EEGLE          Episodic Events/Great Lakes Experiment
 EGU            Electric generation units
 EMAP           Environmental Monitoring and Assessment Program
 EPCHC          Environmental Protection Committee of Hillsborough County
 EOM            Extractable organic matter
 EPA             Environmental Protection Agency
 EPRI            Electric Power Research Institute
 FAMS            Florida Atmospheric Mercury Study
 FCP             Fish Contamination Program
 FDEP            Florida Department of Environmental Protection
 FIFRA           Federal Insecticide, Fungicide, and Rodenticide Act
 FIP              Federal implementation plan
 FR              Federal Register
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Abbreviations and Acronyms
g                Gram
GIS              Geographic Information System
GLNPO          Great Lakes National Program Office
GLWQA         Great Lakes Water Quality Agreement
GMPO           Gulf of Mexico Program Office
GPRA           Government Performance and Results Act
HAP             Hazardous air pollutant                                 ;
HCB             Hexachlorobenzene
HCH             Hexachlorocyclohexane
HMIWI          Hazardous/medical/infectious waste incinerators
HNO3            Nitric acid
HYSPLIT        Hybrid single particle Lagrangian integrated trajectory
IADN            Integrated Atmospheric Deposition Network               ;
IAQAB          International Air Quality Advisory Board
IBI              Index of Biotic Integrity
IDEM           Indiana Department of Environmental Management
IJC              International Joint Commission
INC             International Negotiating Committee
kg               Kilogram
LaMP            Great Lakes Lakewide Management Plans
LAER           Lowest achievable emission rate
LCBP            Lake Champlain Basin Program
LISS             Long Island Sound Study
LMMBS         Lake Michigan Mass Balance Study
LRTAP          Europe Long-Range Transboundary Air Pollution
MACT          Maximum achievable control technology
MCL            Maximum contaminant level
MCM            Mercury cycling model
MDEQ          Michigan Department of Environmental Quality
MDN            Mercury Deposition Network
MOU            Memorandum of Understanding
MPCA          Minnesota Pollution Control Agency
MTRL          Maximum tissue residue level
MWC           Municipal waste combustors
N               Nitrogen
NAAEC         North American Agreement on Environmental Cooperation
NAAQS         National ambient air quality standard
NADP           National Atmospheric Deposition Program                :
NADP-MDN     National Atmospheric Deposition Program - Mercury Deposition Network
NADP-NTN      National Atmospheric Deposition Program - National Trends Network
NAFTA         North American Free Trade Agreement
NCSU           North Carolina State University
NDAMN        National Dioxin Air Monitoring Network
NEP             National Estuary Program
NERRS         National Estuarine Research Reserve System
NESCAUM      Northeast States and Eastern  Canadian Provinces Mercury Study
NH3             Ammonia
NH4+            Ammonium
NHX             Reduced nitrogen compounds (e.g., ammonia, ammonium)
NLFWA         National Listing of Fish and Wildlife Advisories
 Pagexviii
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                                                                Abbreviations and Acronyms
 NLEV            National low emission vehicle
 NO              Nitric oxide
 NO2              Nitric dioxide
 NO3              Aerosol nitrate
 NOAA           National Oceanic and Atmospheric Administration
 NOEL            No observed effects level
 NOX              Oxides  of nitrogen
 NS&T            National Status and Trends
 NSI              National Sediment Inventory
 NSPS            New source performance standards
 NSQS            National Sediment Quality Survey
 NTI              National Toxics Inventory
 NORBIC          North Business-Industrial Council
 OAP             Office of Atmospheric Programs
 OAQPS           Office of Air Quality Planning and Standards
 OAR             Office of Radiation
 OC              Organochlorine chemical
 OCHP            Office of Children's Health Protection
 QMS             Office of Mobile Sources
 OPPTS           Office of Pollution Prevention and Toxics
 ORD             Office of Research and Development
 OTAG            Ozone Transport Assessment Group
 OTAQ            Office of Transportation and Air Quality
 OTC             Ozone Transport Commission
 OTR             Ozone Transport Region
 OW              Office of Water
 PAH             Polycyclic aromatic hydrocarbon
 PBT              Persistent bioaccumulative toxic
 PCB              Polychlorinated biphenyl
 PCDD            Polychlorinated dibenzo-p-dioxin
 PCDF            Polychlorinated dibenzofuran
 PEL              Probable effects level
 PM              Particulate matter
 POM             Polycyclic organic matter
 POP              Persistent organic pollutant
 RACT            Reasonably available control technology
 RADM            Regional Atmospheric Deposition Model
 RAP              Regional action plan
 RELMAP         Regional Lagrangian Model of Air Pollution
 R-EMAP          Regional Environmental Monitoring and Assessment Program
 REMSAD         Regulatory Modeling System for Aerosols and Deposition
 SAB              Science  Advisory Board
 SAV              Submerged aquatic vegetation
 SFEI              San Francisco Estuary Institute
 SFEP             San Francisco Estuary Project
 SIP               State implementation plan
 SMOC            Sound management of chemicals
 SoFAMMS        South Florida Atmospheric Mercury Monitoring Study
 SVOC            Semi-volatile organic compound
 SWFWMD .       Southwest Florida Water Management District
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Abbreviations and Acronyms
SWMP           System-Wide Monitoring Program
TBNEP          Tampa Bay National Estuary Program
TEQ             Toxic equivalent quantity
TLRJ            Toxics Loading and Release Inventory
TMDL           Total maximum daily load
tpy              Tons per year
TRANSCO       Transfer coefficient
TRI              Toxic Release Inventory
TRIM            Total Risk Integrated Methodology
TSCA            Toxic Substances Control Act
UNC-CH         University of North Carolina at Chapel Hill
UN-ECE         United Nations Economic Commission for Europe
UNEP            United Nations Environment Program
US              United States
USGS            U.S. Geological Survey
VOC            Volatile organic compound
WLSSD          Western Lake Superior Sanitary District
WMNP          Waste Minimization National Plan
WMPT          Waste Minimization Prioritization Tool
WQB            Water Quality Board
WRDA          Water Resources Development Act
yr               Year
Page xx
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                                     CHAPTER I
                INTRODUCTION AND BACKGROUND
        Although water quality has improved in past years, ongoing research indicates that many of the
 Nation's waterbodies, including the Great Waters, are impacted by degraded water quality and associated
 adverse health and ecological effects. These impacts are due, in part, to inputs of pollutants from a
 variety of sources and through multiple pathways, including atmospheric deposition (Figure 1-1). The
 role of air pollution as an important contributor to water pollution has long been recognized and, in
 recent years, has been the subject of growing scientific study and concern to regulatory agencies. Section
 112 of the CAA provides the statutory basis for hazardous air pollutant (HAP) programs directed by
 EPA.  In response to mounting evidence that air pollution contributes to water pollution, Congress
 included section 112(m), Atmospheric Deposition to Great Lakes and Coastal Waters, in the 1990
 Amendments to the CAA to establish research, reporting, and potential regulatory requirements related to
 atmospheric deposition of HAPs to the "Great Waters."

                                          Figure 1-1
                       Pollutant Transport Pathways to Waterbodies
                   .  . Air
                    deposition
       This report fulfills the requirements in section 112(m)(5), which direct EPA, in cooperation with
NOAA, to periodically submit a Report to Congress including information on pollutant sources and
emissions, loadings, effects, and exceedances of guidelines in the Great Waters.  The biennial report is
required under section 112(m) of the CAA to cover the following:

1.      The contribution of atmospheric deposition to pollution loadings in the Great Waters;

2.      The environmental and public health effects of any pollution attributable to atmospheric
       deposition to these waterbodies;

3.      The sources of any pollution attributable to atmospheric deposition to these waterbodies;
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter I
Introduction and Background
4.     Whether pollution loadings in these waterbodies cause or contribute to exceedances of drinking
       water or water quality standards or, with respect to the Great Lakes, exceedances of the specific
       objectives of the Great Lakes Water Quality Agreement; and,

5.     Descriptions of any revisions of the requirements, standards, and limitations of relevant CAA
       and Federal laws to ensure protection of human health and the environment.

       The First and Second Great Waters Reports to Congress on atmospheric deposition to the Great
Waters were published in May 1994 (U.S. EPA 1994) and June 1997 (U.S. EPA 1997b). The first two
reports presented the programmatic background and covered the scientific issues that are addressed by
the Great Waters program. The Third Great Waters Report to Congress provides an update to the
information presented in previous reports and specifically highlights progress made since the Second
Report to Congress, including changes in pollutant emissions, deposition, and effects, as well as recent
advancements in the scientific understanding of relevant issues.  In addition, the report discusses recent
activities and accomplishments of the many different initiatives that help protect the Great Waters from
pollutants deposited from the atmosphere.
Page 1-2
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                                                                                 Chapter I
                                                               Introduction and Background
LA   OVERVIEW OF THE GREAT WATERS PROGRAM

DEFINITION OF GREAT WATERS

       The waterbodies collectively referred to as the "Great Waters" in this report are the Great Lakes,
Lake Champlain, Chesapeake Bay, and specific coastal waters defined in the statute as coastal waters
designated through the National Estuary Program (NEP) and the National Estuarine Research Reserve
System (NERRS).  Figure 1-2 displays the locations of these waterbodies. Examples of some of the
coastal waters designated as Great Waters include Tampa Bay, Santa Monica Bay, San Francisco Bay,
Puget Sound, Galveston Bay, Casco Bay, the New York Bight, and Albemarle-Pamlico Sounds.

                                         Figure 1-2
                              Locations of the Great Waters
           + Great Waters designated by name
           • EPA National Estuary Program (NEP) Site
           • NOAA NERRS Designated Site

           D EPA NEP Site and NOAA NERRS Designated Site
NOAA—National Oceanic and Atmospheric Administration
NERRS—National Estuanrine Research Reserve System
PROGRAM PARTICIPANTS AND ORGANIZATIONS

       The EPA's Great Waters program was established to implement the provisions of section 112(m)
of the CAA.  In partnership with NOAA, this program is charged with examining the sources and impacts
of air pollutant deposition to the Great Waters and recommending potential solutions in Reports to
Congress.  In addition to these two agencies, other international, national, regional, and local
organizations are engaged in activities that seek to reduce sources and quantities of pollution to the Great
Waters and also contribute to the body of science relevant to the Great Waters program.  This Report to
Congress, like the first two reports, describes the most recent activities of these programs, both within
and outside of EPA.
Deposition of Air Pollutants to the Great Waters - 3  Report to Congress 2000
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Chapter I
Introduction and Background	__^_	

       Increasingly, EPA is utilizing cross-program teams and partnerships with other agencies and
organizations to study and solve complex, "multimedia" environmental issues (i.e., issues that cut across
air, water, land, and biological resources). For example, the Clean Water Action Plan, issued by EPA in
1998, which includes many activities relevant to the Great Waters program, is a coordinated Federal
effort involving EPA and the Departments of Agriculture, Defense, Interior, and Commerce, all of which
have authorities affecting the quality of the Nation's water resources. This Report to Congress describes
several such collaborative efforts that support targeted data gathering and decision making for multiple
objectives, including those of the Great Waters program.

       Because deposition of atmospheric pollutants to the Great Waters is a multimedia problem,
several media-based and geographically-based programs are part of EPA's integrated efforts to address
pollution in the Great Waters, including the following.

•      Office of Air and Radiation (OAR) administers the Great Waters program along with other
       programs under the CAA that affect the Great Waters. For example, air regulations and
       programs developed by OAR reduce emissions of air toxics and nitrogen from many mobile and
       stationary sources of Great Waters pollutants of concern.  Offices within OAR responsible for
       air pollution control programs include (1) the Office of Air Quality Planning  and Standards
       (OAQPS), which has overall responsibility for the Great Waters, air toxics, and air quality
       management programs; (2) the Office of Atmospheric Programs (OAP), which manages the
       acid rain and global climate change programs; and, (3) the Office of Transportation and Air
       Quality (OTAQ; formerly the Office of Mobile Sources or OMS), which is responsible for
       regulating on- and off-road vehicles and fuels.

•      Office of Research and Development (ORD) undertakes and coordinates research and
       monitoring programs that provide information for assessment of human health and
       environmental risks associated with exposures to  pollutants of concern in the Great Waters  as
       well as for risk management decisions.  The ORD is the lead EPA office in developing a mercury
       research strategy and is working closely with EPA's Office of Prevention, Pesticides and Toxic
       Substances (OPPTS) in preparing a dioxin reassessment.

•      Office of Water (OW) leads numerous activities that are integral to the Great Waters program.
       For example, OW provides data on trends in fish and sediment contamination in the Great
       Waters and is working to factor atmospheric deposition into waterbody-specific water pollution
       standards.  In addition, OW manages the Non-Point Source Control Program under section 319
       of the Clean Water Act. Within OW, the Office of Wetlands, Oceans and Watersheds is
       responsible for, among other things, coastal protection (e.g., the National Estuary Program) and
       the TMDL determination. The Office of Science and Technology provides critical tools to help
       understand and reduce water pollution, and, in cooperation with NOAA and other Federal and
       State and tribal agencies, reviews and monitors fish and shellfish contamination across the U.S.

•      National Estuary Program (NEP), which is managed by OW, was established by EPA in  1987
       to implement section 320 of the Clean Water Act. The purpose of the NEP is to restore and
       enhance nationally significant estuaries that are threatened or impaired by pollution,
       development, or overuse.  Management decisions are made by conferences composed of EPA
       and local stakeholder groups. The NEP currently includes 28 estuaries, several of which have
       identified air deposition as a concern and have received Great Waters program funding to address
       the problem.
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                                                                                    Chapter I
                                                                 Introduction and Background
•      Chesapeake Bay Program Office (CBPO) represents EPA as a partner in the Chesapeake Bay
       Program. This program was created in 1983 by an agreement between EPA, the State of
       Maryland, the Commonwealths of Virginia and Pennsylvania, and the District of Columbia. The
       Chesapeake Bay Program uses a cooperative, watershed approach to research and resolve public
       health and environmental issues affecting the bay.

•      Great Lakes National Program Office (GLNPO) is responsible for EPA activities specific to
       the Great Lakes, including responsibilities defined by the Great Lakes Water Quality Agreement
       with Canada, Great Lakes Program requirements under section 118 of the Clean Water Act, and
       the Great Lakes Critical Programs Act of 1990. The GLNPO also supports EPA's OAQPS and
       Region V activities specific to the Great Lakes for the air toxics program under section 112 of
       the CAA.  In addition, GLNPO conducts and funds monitoring research in support of the Great
       Waters program.

•      Gulf of Mexico Program Office (GMPO) is a nonregulatory organization that sets
       environmental goals and implements projects to protect the environmental resources of the Gulf
       of Mexico. Partners in the GMPO include EPA, other governmental agencies (Federal, State,
       and local), private and non-profit sector stakeholders, and interested citizens.  The Gulf of
       Mexico shoreline includes a substantial percentage of the Nation's estuaries and other significant
       coastal ecosystems.

•      EPA Regional Offices (Regions I-X) are responsible for working directly with States, tribes,
       and regional organizations to implement national environmental programs, including the Great
       Waters program. For instance, Region I and Region II work with the States in the Northeast to
       address pollution in the Lake Champlain Basin, as well as the National Estuary Programs from
       Maine to New Jersey.

       In addition to the EPA Offices listed above, many others contribute to the integrated efforts as
well. For example, the Office of Solid Waste and Emergency Response (OSWER) provides Agencywide
policy, guidance, and direction for the EPA's solid waste program and emergency response program.
The Office of Enforcement and Compliance Assurance is responsible for leading the Agency in ensuring
compliance with the rules that limit pollution. The OPPTS leads the Agency  in pollution prevention
activities, among many other activities.  Chapter III discusses many of the programs led by these and
other offices.

       The NOAA administers the 23 National Esruarine Research Reserves System (NERRS) sites -
all are coastal Great Waters - which were created in 1972 by the Coastal Zone Management Act. The
NERRS sites, which were selected to be representative of various regions and estuary types, are managed
cooperatively with the States to provide opportunities for long-term research, education, and stewardship.
Research conducted at NERRS sites includes studies of the impacts of toxic pollutants deposited from
the atmosphere.

       The NOAA also conducts or funds several other monitoring and research programs that
contribute to the Great Waters program. For example, the Atmospheric Integrated Research Monitoring
Program (AIRMoN) conducts daily deposition monitoring, the National Status and Trends Program
gathers and maintains data on the environmental quality of U.S. estuaries and coastal waters, and the
NERRS System-wide Monitoring Program currently gathers water quality and weather data. In addition,
NOAA plays a critical role in working with EPA to jointly assess the transport and deposition of nitrogen
and other pollutants on surface waters.
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Chapter I
Introduction and Background	  ,	

       Other involved participants include State, tribal, and local agencies, non-profit organizations,
private sector groups, industry and industry groups, universities, other countries, and international
research organizations. Relevant research and other activities of these partners are described throughout
the report. The combined activities of all of these partners are responsible for progress to date in
identifying, assessing, and resolving Great Waters problems, including problems associated with
pollutants deposited from air pathways.

GOVERNMENT GOALS SUPPORTED  BY THE GREAT WATERS
PROGRAM AND  ITS PARTNERS

       The EPA's Strategic Plan (U.S. EPA  1997c) defines ten strategic goals used by the Agency for
planning and resource allocation, as required by the Government Performance and Results Act (GPRA).
The efforts by EPA, NOAA, and partners support the following GPRA goals:

1.     Clean Air -- "The air in every American community will be safe and healthy to breathe ...
       Reducing air pollution will also protect the environment, resulting in many benefits, such as
       restoring life in damaged ecosystems and reducing health risks to those whose subsistence
       depends directly on those ecosystems."

2.     Clean and Safe Water —  "All Americans will have drinking water that is clean and safe to
       drink. Effective protection of America's rivers, lakes, wetlands, aquifers, and coastal and ocean
       waters will sustain fish, plants, and wildlife, as well as recreational, subsistence, and economic
       activities..."

3.     Preventing Pollution and Reducing Risk in Communities, Homes, Workplaces and
       Ecosystems — "EPA will safeguard ecosystems and promote the health of natural communities
       that are integral to the quality of life in this Nation ..."

4.     Reduction of Global and Cross-Border Environmental Risks — "The U.S. will lead other
       nations hi successful, multilateral efforts to reduce significant risks to human health and
       ecosystems..."
                                                                       i
5.     Sound Science, Improved Understanding of Environmental Risk, and Greater Innovation
       to Address Environmental Problems — "EPA will develop and apply the best available
       science for addressing current and future environmental hazards, as well as new  approaches
       toward improving environmental protection."

       These efforts support these goals either directly or by contributing information on atmospheric
deposition helpful to EPA's place-based (i.e., geographically-based programs, such as GLNPO) or
media-oriented programs (e.g., programs in OW that focus on water resources).  Specifically, the Great
Waters program and its partners help the Agency achieve atmospheric deposition objectives outlined in
the clean air and clean and safe water goals and the atmospheric transport and deposition component
related to international pollution transport goal. Furthermore, the aspects of the work  devoted to
investigation and assessment of atmospheric deposition support EPA's efforts under the  sound science
goal to provide the best available science on which to base decisions on how best to reduce the presence
and effects of this pollution. As shown in later sections of the report, progress toward each of these goals
involves and emphasizes multimedia and multiprogram collaboration.
Page 1-6
Deposition of Air Pollutants to the Great Waters - 3 Report to Congress 2000

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                                                                                   Chapter I
                                                                Introduction and Background
I.B   POLLUTANTS OF CONCERN

       This report focuses on the 15 pollutants of concern addressed in the First and Second Great
Waters Reports to Congress. The general types of emission sources and uses (and use restrictions) of
these pollutants are summarized in Table 1-1. In general, sources of these pollutants can include U.S.
short-range and long-range transport from stack emissions, natural emissions, re-emitted emissions from
natural and human-made sources, long-range transport from foreign countries, and cycling within the
global pool of each pollutant.

       As in the two previous reports, these pollutants are organized into the following pollutant groups
(with one change):

•      Mercury and Mercury Compounds

•      Other Metals

       — Cadmium and cadmium compounds
       — Lead and lead compounds

•      Combustion Emissions

       — Polycyclic organic matter (POM), including polycyclic aromatic hydrocarbons (PAHs)
       — Dioxins (tetrachlorodibenzo-p-dioxin, 2,3,7,8-TCDD) and furans (tetrachlorodibenzofuran,
       2,3,7,8-TCDF)
       — Hexachlorobenzene (HCB)1

•      Nitrogen Compounds (including NOX, ammonia and ammonium, and organic nitrogen)

•      Banned and Restricted Use Substances

       — Polychlorinated biphenyls (PCBs)
       -- Pesticides
              - Chlordane
              - DDT/DDE
              - Dieldrin
              - Hexachlorobenzene (HCB)1
              - Hexachlorocyclohexane (cc-HCH)2
              - Lindane (y-hexachlorocyclohexane, or Y-HCH)2
              - Toxaphene

       This last revised grouping is based on the fact that the use and manufacture of these pollutants
have either been banned or severely restricted under other Federal statutes, such as the Federal
Insecticide, Fungicide, and Rodenticide Act (FIFRA) and the Toxic Substances Control Act (TSCA).
       1 HCB is a product of incomplete combustion as well as a pesticide. In Chapter II of this report, HCB is
discussed under the pesticides pollutant group.

       2 There are different isomers of HCH of concern that can transform into other HCH isomers that have
different persistence and toxicity characteristics.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page 1-7

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Chapter I
Introduction and Background	____^_	

With these pollutants, in general, historical contamination (e.g., in sediments and landfills), and not
current national releases from U.S. industrial or agricultural activities, appears to be the problem. For the
most part, the sources of these pollutants to the Great Waters today include resuspension of contaminated
sediments, releases from contaminated soils, atmospheric deposition from long-range transport of
pollutants from foreign countries where uses are still permitted, and accidental releases from stockpiles
or intentional dumping.  The revised grouping helps to organize research into these pollutants of concern
and management of the reduction of the risks they pose to the Great Waters (e.g., work under
international frameworks to reduce global releases, activities to remediate contaminated sediments).

       Many programs and activities address these pollutants  of concern either directly or indirectly and
through statutory requirements or voluntary initiatives.  The above pollutants are of concern to multiple
programs because they share the problematic characteristics of toxicity, persistence, and/or potential for
long-range transport in the environment (e.g., via the atmosphere). Because of these properties, many of
these contaminants are ubiquitous in the environment and may accumulate to potentially harmful
concentrations in water, sediments, soil, or the food web. This presents difficult challenges and places a
premium on multimedia, interdisciplinary approaches for solving problems associated with these
pollutants.

       Table 1-2 provides examples of how the Great Waters pollutants of concern are being addressed
in the U.S. by closely related multimedia programs and other activities authorized by the CAA. All of
the programs and activities identified in this table, along with several others, are discussed later in the
report. Collectively, these programs and activities demonstrate EPA's holistic perspective and steps
toward approaching the goals of clean air, clean water, and healthy ecosystems in an integrated manner.

       Building strong partnerships with other governmental agencies and stakeholders is a  guiding
principle of EPA's Strategic Plan and one of five key attributes of EPA's reinvention plan (U.S. EPA
1997c). This report describes several ways in which EPA's progress toward the Great Waters program
goals can be attributed to the collective efforts of many partners at the local, tribal, State, Federal, and
international levels. Table 1-3 identifies some of the programs at different levels that address Great
Waters pollutants of concern. Each of these programs and activities is described later in this report.
Page 1-8
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                                      Chapter I
                                                                  Introduction and Background
I.C   GOALS OF THE THIRD REPORT TO CONGRESS

        The goals of the Third Report to Congress are to discuss the current state of knowledge regarding
atmospheric deposition of pollutants to the Great Waters based on the information available and program
activities since June 1996 (the end of the timeframe for information presented in the Second Report to
Congress) and to describe any necessary revisions to requirements, standards, and limitations pursuant to
the CAA and other Federal laws. The report is organized into four chapters that summarize the
following:

•       Observed and anticipated spatial and temporal changes in airborne emissions, loadings, and
        effects of pollutants of concern (Chapter II);

•       Programs and activities that have been undertaken to address pollutants of concern since the
        Second Report to Congress (Chapter III);

•       Advancements in scientific research methods, environmental models, and data sources that
        improve our understanding of and abilities to address the public health and environmental risks
        posed by the pollutants of concern in the Great Waters (Chapter IV); and,

•       Conclusions and recommendations to help further national, regional, and waterbody-specific
        activities related to the Great Waters program (Chapter V).

In addition, this report identifies important remaining uncertainties, such as those that limit EPA's ability
to assess the links between pollutant sources, loadings, and effects. The research findings, conclusions,
and recommendations presented in this report will be  used to further understand and promote reductions
of overall contaminant loadings to the Great Waters.

        The report focuses on the scientific and programmatic progress that has occurred since the
previous report and presents information according to the major issues of concern (e.g., trends in
loadings and effects, program progress, scientific tools) from a national perspective. Regional or
waterbody-specific examples are presented in the context of a national-level picture of progress toward
the goals of the Great Waters program. For more detail on specific regions or waterbodies, readers are
referred to the many other publications or Internet sites that specifically address those areas (see
Appendix A).  In addition, the report includes an index of waterbodies to enable readers to identify all
information related to a specific waterbody that is presented in this report.

        The information in this report was collected from several sources.  The references cited are
generally from published peer-reviewed journals, government reports, and conference proceedings.  The
report uses a variety of sources that provide relevant new information on Great Waters issues and
generally addresses information released in the past 2 years.  In some cases, large summary reports were
used and, therefore, primary sources of information are not cited. In general, literature published from
the summer of 1996 to the fall of 1998 is included.

        In addition to literature searches for updated information, EPA obtained current scientific and
programmatic information about atmospheric deposition to the Great Waters through personal interviews
with and direct input from various researchers and program participants.  Many of the waterbody-specific
activities highlighted in this report, for example, were provided by the EPA offices that coordinate
investigation, restoration, and maintenance efforts of the waterbody (e.g., Great Lakes National Program
Office, EPA Region V Air and Radiation Division, Chesapeake Bay Program Office, Gulf of Mexico
Program Office).
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page 1-13

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                                      CHAPTER II
                       ENVIRONMENTAL PROGRESS
   Pollutant-Specific Changes 	II-3
     
-------
Chapter H
Environmental Progress
biologic/geologic processes for previously deposited pollutants). Examples of human-made emissions
are those associated with industrial stacks, municipal waste incinerators, agricultural activities (e.g.,
pesticide applications, manure management), and vehicle exhaust. Examples of natural emissions
include those associated with volcanic eruptions, windblown gases and particles from forest fires,
windblown dust and soil particles, and sea spray. In many cases, however, it is difficult to determine if
the pollutant inputs are from natural or anthropogenic sources.

                                           Figure 11-1
                Atmospheric Release, Transport, and Deposition  Processes
                                                                                   Wet
                                                                                 Deposition
                                    Particulate
                                      Matter
              Sources of Pollutants
Anthropogenic Sources          Natural Sources
                                   Air Masses
                          - Local or long-distance
                            transport
                          - Changes in chemical/
                            physical forms
                                                     Dry :•':    ''
                                                   Particle
                                                  Deposition
                                                                                      Air/Water
                                                                                        Gas
                                                                                      Exchange
        Airborne releases or emissions of pollutants can be transported away from the source to other
locations. Depending on the weather conditions and the chemical and physical properties of the
pollutant, air pollutants can be transported varying distances and may undergo physical, chemical, and/or
biological transformations during transport (U.S. EPA 1997b).  As mentioned in Chapter I, all of the
Great Waters pollutants of concern are known to be subject to long-range transport.

        Pollutant loadings to waterbodies can occur through many different pathways, including
connecting streams and rivers, groundwater inflow, land surface runoff, rerelease of pollutants from
sediments, and atmospheric deposition processes. Atmospheric inputs to waterbodies also occur through
several mechanisms (Figure II-l). Pollutants that are released to the air can be deposited to land areas,
tributaries, or directly to the waterbody by wet or dry deposition. The process of wet deposition refers to
the removal of air pollutants from the air by a precipitation event, such as rain or snow. The process of
dry deposition refers to the removal of aerosol pollutants through eddy diffusion and impaction, large
particles through gravitational settling, and gaseous pollutants through direct transfer from the air to the
water (i.e., gas exchange). Air pollutants can also enter the waterbody through indirect deposition which
occurs when an air pollutant is deposited to a land area or tributary and is then carried into a waterbody
by other routes, such as storm water runoff or inflow from tributaries. Therefore, in these mechanisms,
loadings to a waterbody are both directly and indirectly affected by air pollutant emission levels.

        Loadings can be expressed as the total amount of a pollutant entering a waterbody over a
specified time period (e.g., kg/year) or as a loading rate (e.g., ug/m2/year).  The tendency of a specific
pollutant to enter a waterbody through wet deposition, dry deposition, or gas exchange is related to the
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                                                                                     Chapter II
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physical and chemical properties of the pollutant as well as to current and local meteorology.
Determining the relative atmospheric loading - how the loading from atmospheric deposition compares
to that from other pathways, such as groundwater seepage and inflow from connecting surface
waterbodies, where portions of the pollutant load may not be of atmospheric origin - is as important as
determining total loading. Uncertainties exist, however, in loadings estimates because of errors inherent
in sampling methodologies and the assumptions about a specific chemical's behavior that are used to
develop deposition estimates.  Furthermore, monitoring networks have spatial and temporal limitations,
making it difficult to accurately and reliably quantify atmospheric deposition inputs.

        Air pollutant loadings to the waterbody may contribute to environmental and public health
effects, such as when water quality and drinking water standards are exceeded (where such standards
exist). These standards provide a measure of degradation and possible exposures of plants, animals, and
humans to potentially harmful levels of pollutants. The number and magnitude of water quality and
drinking water standard exceedances in a waterbody may be affected, in part, by changes in pollutant
loadings from the atmosphere, which in turn, are affected by changes in atmospheric emissions of those
pollutants.  Potential ecological and human health effects from exposures to the Great Waters pollutants
of concern  are not discussed comprehensively in this report because the Second Report to Congress
focused on effects from exposures. This report focuses more on recent literature on trends, such as
contaminant levels found in biota as well as fish consumption advisories. In many cases, however,
information on trends in exposure levels or observed effects was not available. Therefore, surrogate
measures of exposure, such as trends in concentration levels in environmental media or biota, are
presented.  Note that the presence of a pollutant in the environment only translates into an exposure for
humans and/or biota if an exposure pathway exists.

        The understanding of how the pieces of this complex puzzle fit together continues to increase,
although uncertainty and gaps in information remain. This chapter reports on new information that helps
to establish the links between emissions, transport and transformation, loadings, and effects. It also
includes information on the various elements that contribute to establishing these links. For example, it
includes inventories of emission sources, which are essential inputs to models that predict pollutant
loadings to waterbodies.

POLLUTANT-SPECIFIC CHANGES

        For each pollutant or pollutant group, information on sources  and emissions is presented first,
followed by new loadings information, and then by new information on exposure and effects. If no new
information is available on one of these topics for a particular pollutant or pollutant group, that topic
simply is not addressed. The second part of this section, Cross-Pollutant Changes, summarizes results
from several EPA and other agency programs and projects that are not limited to individual pollutants,
but rather provide information on many pollutants  in a manner making it more appropriate to present the
information as a cohesive piece as opposed to dividing the information among the pollutant groups.

        Although a large amount of research has been and continues to be conducted related to the
release, transport, loadings, exposure, and effects of Great Waters pollutants of concern, information
gaps and uncertainties remain. In general, the information presented below consists of the highlights of
the studies, and details on assumptions and uncertainties are not always presented. However, most if not
all of the studies discussed below are associated with some type of uncertainty (e.g., related to the
number of measurements, the time period of the study, or the lack of standard measurement methods).
The original study should be consulted for these details for a better understanding of the assumptions
used and resultant uncertainties.  While uncertainties and information gaps continue to exist, it should be
noted that research is ongoing to attempt to reduce them.
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Chapter II
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MERCURY AND  COMPOUNDS

       Mercury is a cationic metal — it has
characteristics of both a metal and an organic
compound (e.g., it is persistent in the
environment, bioaccumulates in the food chain,
and vaporizes at low temperatures). Mercury is
an excellent conductor of electricity and is
widely used in products such as batteries,
electric switches, thermostats, thermometers, and
barometers as well as a number of industrial
processes including pharmaceutical preparations
and the production of caustic soda and chlorine.

       Mercury can exist in three oxidation
states: Hg° (metallic), Hg22+ (mercurous), and
Hg24 (mercuric). The oxidation state strongly
influences the properties and chemical behavior
of mercury.  For example, mercurous and
mercuric mercury can form numerous inorganic
and organic chemical compounds; however,
mercurous mercury is rarely stable under
ordinary environmental conditions. Most of the
mercury encountered in water, soil, sediment,
and biota is in the form of inorganic mercuric
salts and organomercurics (i.e., chemical
compounds with a covalent Hg-C bond, rather
than inorganic mercury compounds that simply
associate with organic material in the
environment). The mercury  compounds most
likely to be found under environmental
conditions include the following: the mercuric
salts HgCl2, Hg(OH)2, and HgS; the   :
methylmercury compounds,  methylmercuric
chloride (CH,HgCl) and methylmercuric
hydroxide (CH^HgOH); and, in small fractions,
other organomercurics  (i.e., dimethylmercury
and phenylmercury) (U.S. EPA 1997e).  The
mercury compounds that are of highest concern  in terms of exposure and toxicity to humans and biota are
the methylated mercury compounds. The Mercury Study Report to Congress (U.S. EPA 1997e) provides
additional background  information on mercury and mercury compounds.

       Sources of mercury emissions to the air in the U.S. are ubiquitous and can be broadly classified
as belonging to one of three types:

1.     Re-emitted mercuiy - the re-emission of mercury to the atmosphere by biologic and geologic
       processes from mercury that was previously deposited to the earth's surface following either
       anthropogenic  or natural releases.  For example, a large portion of the deposited mercury is the
       result of past human-made releases as well as releases from natural sources that previously were
       sequestered (e.g., arctic tundra, ice sheets, oceans and wetlands);
                                             HIGHLIGHTS
                                               Mercury

                             >•  Sources.  The largest human-made sources of
                             mercury emissions in the U.S. are coal-fired utility
                             boilers, medical waste incinerators, and municipal
                             waste combustors. Mercury can also be emitted
                             from natural sources, such as volcanic activities.
                             Mercury releases from human activities today are
                             adding to the  global reservoir of mercury cycling
                             between land, water, and air that is the result of
                             natural releases and past human activities. Human-
                             made emissions of mercury have declined since
                             1990, due chiefly to the phase-out of mercury-
                             containing products.

                             >•  Loadings. Atmospheric deposition is a principal
                             source of mercury to several Great Waters, followed
                             by riverine inputs. Urban areas in proximity to the
                             Great Waters can also contribute significantly to
                             loadings via the atmosphere and urban runoff.
                             Deposited mercury that is buried or immobilized in
                             soils and sediments can be transported to
                             waterbodies by high streamflow events like storms
                             and snowmelt. Forested watersheds retard mercury
                             transport to the waterbody compared to agricultural
                             or urban watersheds.

                             >• Human and Ecological Exposure and Effects.
                             Consumption of contaminated fish represents the
                             dominant pathway for both human and wildlife
                             exposures to  methylmercury. The typical U.S.
                             consumer offish from restaurants and grocery stores
                             is not believed to be at risk. Rather, consumers who
                             eat more fish  than is typical or fish that are more
                             contaminated than typical fish may be at risk of
                             adverse effects. Because the developing fetus is
                             regarded as the most sensitive to the effects of
                             methylmercury, women of childbearing age are the
                             population of  greatest concern.  State and tribal fish
                             consumption  advisories have been implemented to
                             warn people about the related risks.  Measurements
                             of mercury in  loons  indicate up to 30 percent of
                             male loons in the northeastern U.S. have mercury
                             levels sufficiently high to cause adverse effects.
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                                                                                     Chapter II
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2.     Natural mercury emissions - the mobilization or release of geologically-bound mercury by
       natural processes; or

3.     Anthropogenic mercury emissions - the mobilization or releases of mercury by human activities.

       Atmospheric deposition of mercury occurs primarily through two processes:  scavenging of
particulate matter by precipitation and conversion of elemental mercury (Hg°) to ionic mercury during
rain formation. Dry deposition of reactive gaseous (Hg2"1") and particulate mercury is also thought to be
an important process.  The three dominant mercury forms act differently in the environment:

•      Hg° can be transported in the atmosphere for thousands of miles around the globe and deposits
       very inefficiently because it is insoluble in water and is less chemically reactive;

•      Hg2+ in the gas-phase may be removed from the atmosphere within a few ten to a few hundred
       miles of the source because it is highly water soluble and reactive; and,

•      Particulate-phase mercury may be deposited at intermediate distances from the source, depending
       on the size of the aerosol  (Schroeder and Munthe 1998).

       Current anthropogenic mercury emissions are only one component of the global mercury cycle.
The amount of mercury in the land, water, and air at any one location is comprised of mercury from the
natural global cycle, the global cycle perturbed by human activities, as well as regional sources and local
anthropogenic sources. In addition to air emissions, other sources of mercury include direct water
discharges or past uses of mercury, such as fungicide application to crops. Current research continues to
indicate that natural sources, industrial sources, and recycled anthropogenic mercury each contribute to
about one-third of the current mercury burden in the global atmosphere (Pirrone et al. 1996). However,
as discussed further in Chapter IV, new measurement methods suggest that natural mercury emissions
rates from mercury-rich soils and bedrocks may be larger than past estimates. It is important to
understand the source of mercury and the amount of mercury contributed by each source type so that the
most efficient control strategies can be devised.

       Given the complexities of the global mercury cycle,  much of the research in recent years focused
on the environmental fate of mercury and the extent of current contamination in the environment. The
state of the science at this time does not provide a complete answer to the question of whether the
problem is improving. There is a general downward trend in anthropogenic mercury emissions in the
U.S., although emissions from many  CAA source categories are not included in this assessment.
Atmospheric deposition of mercury to an adjacent waterbody is primarily a function of the amount of
particulate-phase and reactive gaseous mercury emitted, the proximity of the source to the waterbody,
and meteorological conditions. The National Atmospheric Deposition Program - Mercury Deposition
Network (NADP-MDN) has been used to collect weekly wet deposition data for the past 4 years in some
locations; however, these early data are not robust enough to discern trends. Additional monitoring data
(which includes both wet and dry deposition measurements)  from high quality stations over a longer
period are necessary for effective  trends analyses.  These measurements must be performed to allow for
meteorological analysis and identification of source contributions to the measured mercury. In general,
the  research described in this section represents an important step forward in understanding the fate of
mercury in the environment and will  continue to form the scientific basis for measures taken to address
the  problem.
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Mercury Emissions

       Estimates of the global contribution of mercury emissions to the atmosphere from anthropogenic
sources are 2,000 to 4,000 tons per year (tpy) and from natural sources are 2,200 to 4,000 tpy, resulting
in total mercury air emissions of 4,200 to 8,000 tpy (Pirrone et al. 1998). In comparison, U.S. mercury
air emissions for the 1994-1995 timeframe are 158 tpy, as reported in EPA's Mercury Study Report to
Congress (Table II-l) (U.S. EPA 1997e).  Roughly 87 percent of national mercury emissions in the U.S.
are from combustion sources, including waste and fossil fuel combustion.

       A recently identified source of mercury to the atmosphere is emissions of elemental mercury gas
(Hg°) from soils that have been amended with municipal sewage sludge. Carpi and Lindberg (1997),
using a field chamber and soil amended with sewage sludge, found that sludge application to soil
increased soil Hg° releases by up to two orders of magnitude. The researchers estimated that land
application of sewage sludge in the U.S. and European Union may account for approximately 5 x 106
g/year (5 metric tons/year) of Hg° released to the atmosphere based on the area of land amended each
year and measured Hg° emission rates.

       While there is a growing body of data on the total amount of mercury emitted from different
source types, data on the form (or species) of mercury emitted remain a critical research need.  The
Mercury Study Report to Congress (U.S. EPA 1997e) estimated that anywhere from 0 to 73 percent  of
the mercury emitted from different source categories is in the form of divalent mercury (Hg2+), the form
that deposits and contributes the most to methylmercury concentrations in soil, water, sediment, and
biota. There is, however, considerable uncertainty about the amounts of different mercury species
emitted from some industrial sources.

       The emission inventories provide  a snapshot of recent emissions and indicate a downward trend
in U.S. emissions between 1990 and 1995. This  downward trend follows a general decline in domestic
mercury uses and reduced emissions from waste  combustion sources (including municipal waste
combustors and medical waste incinerators).  Industrial demand for mercury peaked in 1964 and fell 75
percent between 1988 and 1996. This decline largely reflects the phaseout of mercury in household
batteries and paint.  The rate of decline, however, has slowed since 1990.  Future trends in mercury
emissions from fossil fuel combustion sources, which currently represent a large portion of national
mercury emissions, are dependent on future energy needs and fuel use.  Mercury emissions from
municipal waste combustors and medical waste incinerators, which also are large national sources of
mercury emissions, are expected to continue to decline from 1995 through 2000 due to new regulations
(see Chapter III) (U.S. EPA 1997e).

       It should be noted that several uncertainties exist with the mercury emissions inventory. For
example, not all source categories are included (e.g., landfills), and recent data submitted to EPA by the
Chlorine Institute indicate that current emissions may be underestimated.  Furthermore, mercury
emissions from coal-fired electric utilities are expected to increase in future years, based on estimated
changes in  emissions from implementation of the acid rain program and projected trends in fuel choices
and electric power demands in the year 2010 (U.S. EPA 1998p).  As noted earlier in this section, the
speciation of mercury emitted is important in determining its transport and fate, yet remains a key
uncertainly. The EPA has worked with the Department of Energy and the American Society for Testing
and Materials to develop a standard method for measuring speciated mercury from utility boilers.  The
EPA is also working to refine this method for other  source categories, such as incinerators. The electric
utility industry is currently conducting speciated mercury emission testing on a  subset of coal-fired
facilities, as discussed in the hazardous air pollutant section of Chapter III. Finally, in order to better
understand the relative contribution of mercury to the environment from anthropogenic sources, further
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                                                                                     Chapter II
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 research is needed into the level of natural emissions as well as the amount and original source of
 mercury that is re-emitted to the atmosphere after being deposited to soils, watersheds, and ocean waters.
 Although considerable uncertainty still exists, it has become increasingly evident that anthropogenic
 emissions of mercury to the air rival or exceed natural inputs (U.S. EPA 1997e).

                                           Table 11-1
                       National Anthropogenic Mercury Air Emissions
                      (Based on 1994-1995 Inventory; U.S. EPA 1997e)
Source Category
Utility boilers: coal combustion, oil, and natural gas
Municipal waste combustion
Commercial/industrial boilers: coal and oil
Medical waste incineration
Chlor-alkali production
Hazardous waste combustors
Chlor-alkali
Portland cement, excluding hazardous waste-fired
Residential boilers: oil and coal
Pulp and paper manufacturing
Others (<1 percent each) a
Total U.S. Anthropogenic Mercury Air Emissions
1994-1995
Anthropogenic Air
Emissions (tons/year)
52
30
28
16
7
7
7
5
4
2
3
158b'c
Percent Contribution to
Total U.S. Anthropogenic
Air Emissions
33
19
18
10
4
4
4
3
2
1
2
100b'°
 A list of the source categories that contribute less than 1 percent to total U.S. emissions is provided in Appendix B.
b This value represents anthropogenic mercury air emissions in the U.S. only.
0 Values do not add exactly due to rounding.

Mercury Deposition in the  U.S.

       Once in the air, mercury can be deposited locally or widely dispersed and transported long
distances from emission sources.  How far it travels and where it is deposited depends in part on the
chemical and physical form of the mercury emitted. Elemental mercury may be transported in the
atmosphere for relatively long periods (approximately 1 year), allowing its distribution over long
distances, both regionally and globally, before being deposited to the earth. In contrast, the residence
tune of mercuric (Hg2+) compounds in the atmosphere is generally believed to be a few days or less,
resulting in deposition closer to sources. Mercury also differs from other metals because it is readily re-
emitted to the atmosphere following deposition and chemical transformation. In summary, principal
factors that contribute to the modeled and observed patterns of mercury deposition are (1) the emission
source locations and characteristics (e.g., stack height); (2) the amount of Hg24" and particulate mercury
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Chapter H
Environmental Progress
emitted; (3) atmospheric chemical and physical properties; (4) uncertainties associated with the
emissions inventories, both in the magnitudes and the chemical forms emitted; (5) climate and
meteorology, and (6) treatment of natural sources and re-emission within the modeling domain.

       Because of the influence of the above six factors on mercury deposition, modeling of mercury
transport and deposition at different spatial scales (e.g., national, regional, and local) results in slightly
different information appropriate to each scale. Modeling at the local scale (i.e., approximately 100 km),
can provide more specific deposition estimates for a specific waterbody, but requires meteorological
modeling at the appropriate scale  and up-to-date information on the amount of divalent and particulate
mercury emitted from the local sources. Recent studies in the Great Lakes region and in Florida show
that mercury emissions on local scales can greatly influence loadings in some locations when local
sources have significant emissions of divalent and particulate forms of mercury. For example, the South
Florida Atmospheric Mercury Monitoring Study (SoFAMMS) collected daily event precipitation samples
at 17 sites for 1 month and, using a suite of chemical and meteorological data, was able to demonstrate
that local anthropogenic sources strongly influence mercury wet deposition levels (see Section III.C for
additional information on SoFAMMS) (Dvonch et al. 1998). National modeling of emissions and
meteorology, on the other hand, can assist in answering some questions, but should not be applied to
regional or local analyses without critical review. The various forms of mercury in emissions are all
important in predicting atmospheric transport and deposition patterns, and care must be taken in
estimating local deposition or longer range impacts.

        For the Mercury Study Report to Congress, EPA used the Regional Lagrangian Model of Air
Pollution (RELMAP) to model mercury emissions from the continental U.S. to estimate the amount of
mercury being deposited to the U.S. The model inputs included meteorological data from  1989, the U.S.
emissions inventory of 158 tons/year (U.S. EPA 1997e), and assumptions about the chemical species of
mercury emitted from various source types. The results showed total deposition (i.e., wet and dry
deposition of all forms of mercury) to be over 10 Fg/m2 throughout most of the continental U.S. east of
the Mississippi River, with values over 30 Fg/m2 for the northeast corridor and other urban areas. The
highest mercury deposition rates were predicted to occur in the southern Great Lakes and Ohio River
valley, the Northeast, and scattered areas in the South (with highest deposition rates in the Miami and
Tampa areas).  Deposition of mercury is strongly influenced by the magnitude of emissions, the chemical
species of the emitted mercury (ionic and particulate-bound forms of mercury being the most readily
deposited), ozone and soot concentrations, and total annual precipitation.

        On a national basis, the computer simulation suggested that about one-third (~ 52 tpy) of U.S.
anthropogenic mercury emissions is deposited within the lower 48 States.  The remaining two-thirds (~
107 tpy) of mercury emissions are transported beyond U.S. borders. In addition, the simulation suggests
that another 35 tpy of mercury from the global reservoir (which includes mercury from U.S. emissions)
are deposited in the U.S., resulting in a total deposition of roughly 87 tpy.  Note, however, that the results
of the simulation include some uncertainty, as discussed in more detail in the following paragraph.
According to the simulation, 98 percent of the deposited mercury of anthropogenic origin was emitted in
the form of ionic mercury or particulate mercury. The emissions inventory and estimated
chemical/speciation profiles indicate that of all combined ionic and particulate mercury emissions, 29
percent is from coal-fired electric utility boilers, 25 percent is from municipal waste combustion, 18
percent is from medical waste incineration, 16 percent is from coal-fired commercial and industrial
boilers, and 12 percent is from all other modeled sources.  The methods for developing these mercury
emission estimates and speciation profiles are described in detail in volumes I and II of EPA's Mercury
Study Report to Congress (U.S. EPA 1997e).
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        As the Mercury Study Report to Congress explains, there are a number of uncertainties in the
 RELMAP analysis, with a large degree related to the state-of-the-science on chemical and physical forms
 of mercury air emissions and their chemical and physical transformations in the atmosphere. The model
 seems most sensitive to the speciation of mercury emissions. Speciated emissions data remain a critical
 research need, as discussed above in the section on mercury emissions. In addition, atmospheric
 chemistry data are incomplete in the model. Furthermore, there is inadequate information on the
 atmospheric processes that affect wet and dry deposition (U.S. EPA 1997e). (Note that other sections of
 this report describe additional research and model development activities in these areas.)

        To test the validity of the model, the wet deposition results from the RELMAP simulation were
 compared to limited measured data from the Mercury Deposition Network (MDN). The RELMAP
 estimates agreed with actual measurements within a factor of two in most cases and tended to
 underestimate measured wet deposition. Overall, the RELMAP model seemed to produce reasonable
 spatial patterns of annual wet deposition. Better spatial coverage by a long-term deposition network is
 needed to better evaluate the model. In addition, the high deposition rates estimated for some urban areas
 could not be verified because measurement data in urban areas are lacking (U.S. EPA 1997e).
                                                      Mercury Emission Inventory by Percent
                                                    Contribution by Source Category for Eight
                                                               Northeast States

                                                    Municipal waste combustion — 45 percent
                                                    Non-utility boilers -18 percent
                                                    Electric utility boilers -13 percent
                                                    Manufacturing sources — 7 percent
                                                    Area sources — 6 percent
                                                    Sewage sludge incineration - 6 percent
                                                    Medical waste incineration — 5 percent

        In addition to the Mercury Study Report
 to Congress, there have been a number of other
 recent modeling and monitoring studies of
 mercury deposition. For example, a regional-
 scale analysis, performed by the Northeast States
 and Eastern Canadian Provinces in collaboration
 with EPA, also illustrates the importance of local,
 regional, and global sources to mercury
 deposition levels (NESCAUM 1998). The
 purpose of this study was to determine whether
 deposition in the Northeast could be attributable
 to sources within the region or to long-range
 transport of mercury from upwind States. In this analysis, a RELMAP simulation suggested that
 approximately 47 percent of the modeled deposition in the Northeast is attributable to sources in the
 region, while approximately 30 percent is attributable to sources located outside the region. The
 remaining 23 percent was estimated to be from the global atmospheric reservoir, which includes mercury
 from U.S. emissions. The accompanying text box lists the source categories contributing to mercury
 emissions in the Northeast.  As with the national EPA study, combustion sources account for more than
 85 percent of the mercury emissions. Note, however, that the results of the simulation include
 considerable uncertainty.

       The modeling predictions described above are based on average emissions over a year and as
 such do not provide an indication of trends over time. Two ways to assess trends in emissions and
 deposition are to consistently measure deposition over a wide geographic area over a long period of time,
 or to analyze sediment cores. Mercury monitoring of wet deposition at a number of sites began recently,
 and there are not enough data at present to evaluate trends over a widespread area.  The Mercury
 Deposition Network (MDN), which began as a transition network of 17 sites in 1995, became an official
 subnetwork of NADP in 1996. Currently, nearly 40 sites are in operation throughout the U.S. and
 Canada, with sites concentrated on the east coast and in the Great Lakes basin (Figure II-2). However,
the network is relatively sparse in its overall coverage, introducing uncertainty into trends analyses. The
 objective of the MDN is to develop a long-term database of weekly total mercury concentrations in
precipitation and the annual and seasonal flux of total mercury in wet deposition. The present sites were
not selected to be representative of the region and, in some cases, are highly influenced by local emission
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                                                                                      Page II-9

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                                                                                                      U)
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                                                                                     Chapter II
                                                                        Environmental Progress
 sources. Site sponsors consist of U.S. and Canadian government agencies, State government agencies,
 universities, associations, and consulting firms.  Currently, MDN data are available for 1996 and 1997.

        Available MDN monitoring data from 1996 and 1997 indicate that the volume-weighted mean
 concentration of total mercury in precipitation from 22 sites ranged from 6.0 to 18.9 ng/L and annual
 deposition of mercury ranged from 2.1 to 25.3 ug/m2 (or 2,100 to 25,300 ng/m2). In 1997, average
 mercury concentrations in rain ranged from 6.2 to 18.3 ng/L at the 21 sites that had a full year of
 monitoring data and the average concentration for all sites was 10.6 ng/L. In 1996, average mercury
 concentrations at nine sites with a full year of data ranged from 6.0 to 14.1 ng/L with an average for all
 sites of 10.2 ng/L.  In 1997, the annual average wet deposition of mercury for 21 sites ranged from 4.3 to
 25.3 ug/m2 (or 4,300 to 25,300 ng/m2), whereas in 1996, the annual average wet deposition of mercury
 for nine sites ranged from 6.3 to 19.7 ug/m2 (or 6,300 to 19,700 ng/m2). In the eastern U.S., average
 summer mercury concentrations are more than double winter concentrations and average summer
 deposition values are more than three times winter values. This can be explained by higher
 concentrations of mercury in the rain and higher rainfall amounts during the summer. One interesting
 finding from the 1996 and 1997 MDN data is that several individual weeks were associated with
 unusually high mercury deposition amounts as a result of heavy rainfall and above average mercury
 concentrations. Based on National Weather Service information, the storms that contributed the
 precipitation in these weeks tracked along the east coast, including New Jersey, New York City,
 Providence, and Boston.  Therefore, it is likely that emissions of mercury from these urban centers
 entered the air mass of the storm and were deposited at these MDN sites (Sweet et al. 1999).

        While the MDN monitoring sites have not been in operation long enough to discern any temporal
 trends in mercury levels, one monitoring station has been in operation in the Lake Champlain basin at
 Underbill, Vermont since 1992.  This is now the longest continuous monitoring program in the world for
 total mercury wet deposition, ambient particulate phase mercury, and ambient total gas phase mercury.
 Results do not show long-term trends in atmospheric mercury concentrations except perhaps for a
 downward trend for vapor phase mercury. Based on monitoring of wet deposition  and modeling of dry
 deposition, total annual deposition of mercury in  1993 was estimated at 15.1 ug/m2 (or 15,100 ng/m2).
 However, research suggests that the dry deposition flux of mercury may be much greater and re-emission
 of mercury from forest ecosystems may be significant, introducing considerable uncertainty in the total
 wet plus dry deposition estimates (Hanson et al. 1995, Rea et al. 1998, Scherbatskoy et al. 1999, 1998,
 1997).

        The Underbill monitoring data collected between December 1992 and December 1997 also show
 seasonal variations. Deposition peaked in summer months when mercury concentrations in precipitation
 are highest, while the concentration of mercury vapor in the air showed only slight seasonal variation.
 The seasonal variations observed in mercury deposition at Underbill were similar to those observed in the
 Great Lakes basin (Hoyer et al. 1995, Burke et al. 1995).  Concentration of particulate-associated
 mercury in the air in 1993-94 tended to be greatest in winter months at this site. Concurrent monitoring
 of mercury concentrations in stream water in a nearby forested catchment in the Lake Champlain basin
 showed dissolved concentrations to be fairly constant, but found that total mercury (dissolved plus
 particulate) was strongly correlated with flow rates. Thus, high flows may re-mobilize mercury adsorbed
 to sediment and organic matter. Also, maximum  stream flows were often associated with spring
 snowmelt, which appears to be an important regulator of annual transport patterns of mercury within the
 Lake Champlain basin (Scherbatskoy et al. 1999, 1998, 1997, Shanley et al. 1999).

        In another recent analysis, Pirrone et al. (1998) estimated atmospheric emissions and deposition
 of mercury in North America and compared these estimates to vertical profiles of mercury accumulation
 rates in sediment cores from four Great Lakes sites . The results of this analysis illustrate that
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atmospheric deposition has been significant since the 1900s and still is the major contributor of mercury
to the Great Lakes, although a variety of other sources (including direct discharges) also contribute to
mercury inputs in the Great Lakes. Based on sediment core data and emissions estimates, Pirrone et al.
calculated the atmospheric deposition flux of mercury to North America as a whole to be between 14.3
and 19.8 ug/m2/yr (1.43 to 1.98 ng/cm2/yr), whereas in the Great Lakes region, the atmospheric
deposition flux of mercury was calculated to be higher, at 135 ug/m2/yr (13.5 ng/cm2/yr). This difference
is likely due to local anthropogenic emissions and subsequent deposition of mercury in the Great Lakes
region.  Furthermore, mercury accumulation rates in sediment cores from the Great Lakes from pre-
industrial to modern times increased from 0.7 to 235 ng/cm2/yr in Lake Ontario, from 0.8 to 65 ng/cm2/yr
in Lake Michigan, and from 3 to 175 ng/cm2/yr in Lake Erie. All of these values are larger than those
reported in sediment cores from small remote lakes in the northeastern U.S,, indicating local and regional
sources of mercury are deposited in the Great Lakes region rather than simply from the regional
background in the northeastern U.S.

        Engstrom and Swain (1997) analyzed sediment core data to detect recent trends in mercury
emissions in the upper Midwest and found that, for a number of Minnesota lakes, mercury deposition
peaked in the 1960s and 1970s and then declined.  These declines were not seen in remote lakes in
southeastern Alaska, indicating that deposition from the global pool had not declined. The decline in
deposition inputs to Midwestern lakes can be attributed to reduced emissions from regional and local
sources, which are thought to be largely due to pollution controls (particularly on waste incinerators) and
a shift from coal to natural gas for residential and commercial heating.

Moss Balance Studies of Mercury

        Preliminary results of the Lake Michigan Mass Balance Study (LMMBS; described in the
Second Great Waters Report to Congress) are becoming available. Results from two studies (Hurley et
al. 1998b, Landis 1998), which are discussed below, show varying results. The study by Hurley et al.
(1998b) involved sampling eleven tributaries that are representative of a variety of watersheds as part of
the LMMBS. For example, land-use patterns included agricultural, forest, wetland, and urban. Ten of
the 11 tributaries sampled are associated with areas of concern due to past contamination. Sediment core
and sediment trap analysis is still being conducted by EPA for the LMMBS samples; however, tributary
sample analysis has been completed. The mean mercury concentration in the 11 tributaries was 6.9 ng/L,
with the highest concentrations in the rivers running through the urban areas. The highest mean mercury
concentration (36.0 ng/L) was observed on the Fox River running through Green Bay, while the lowest
mean concentration (1.0 ng/L) was observed on the Muskegon River. In general, the northern rivers had
lower tributary inputs than the more industrialized southern rivers.

        Hurley et al. (1998b) calculated tributary loading to Lake Michigan from each river as the
product of the daily average water discharge and the daily mercury concentration. The estimated annual
tributary mercury flux was 230 kg/year. The total annual mercury input into Lake Michigan from the
atmosphere and the tributaries during the LMMBS was estimated to be 1,419 kg/year. Atmospheric
deposition was determined to be the dominant source of mercury inputs to Lake Michigan, contributing
approximately 84 percent (1,189 kg/year) of the annual total.

        The study by Landis (1998) involved a hybrid-modeling framework based on monitoring data in
the Great Lakes region. Annual deposition estimates from Landis (1998) are provided in Table II-2. In
addition, the Landis modeling effort indicated that the Chicago/Gary urban area was responsible for at
least 19 percent of the total atmospheric deposition to Lake Michigan. It should be noted that reactive
mercury deposition is not included in this estimate of the urban influence and, thus, likely represents an
underestimate of the true impact of the  Chicago/Gary urban area.
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                                           Table 11-2
     Preliminary Estimates of Total Atmospheric Mercury Deposition to Lake Michigan
Deposition
Wet
Aerosol Dry
Reactive Gaseous Mercury3
Dissolved Gaseous Mercuryb
Total
Annual Total (kg)
614 ±186
69 ±38
506
-460
729
Annual Mean (pg/m2)
10.6 ±3.2
1.2 ±0.7
8.8
-8.0
12.6
               1 Reactive gaseous mercury (RGM) deposition values do not include error bars because they
               reflect a sensitivity analysis performed on a single measurement in place of direct measurements
               since no measurement method was available for RGM at the time of the study.
               b Dissolved gaseous mercury (DGM) deposition values do not include error bars because the
               values reflect a single measurement taken to establish modeling parameters.
               Source: Landis 1998

        In another effort, Hurley et al. (1998a) collected and analyzed field samples from the Fox River
in Wisconsin, which is located in a highly industrialized area and feeds into Green Bay, and ultimately,
Lake Michigan. While total mercury in this river is high relative to other tributaries feeding into Lake
Michigan, most of the mercury is bound to sediments.  In the Fox River, resuspended sediments appear to
be the predominant source of mercury into Green Bay. However, in the Lower Fox River and Green Bay,
methyhnercury concentrations are relatively low, suggesting that particulate-bound mercury has limited
bioavailability (Hurley et al. 1998a).

        As part of the Chesapeake Bay Atmospheric Deposition Study (CBADS), mercury wet
deposition, dry deposition, and gas exchange were measured at sampling sites in the Chesapeake Bay
representative of regional background levels.  Total atmospheric deposition of mercury to the
Chesapeake Bay was estimated to be 80 kg/year. Wet deposition of mercury to the Chesapeake Bay
surface waters was estimated to be 162.1  kg/year (± 10-20 percent). Dry deposition was estimated to be
32.4 kg/year (accurate within a factor of two or three).  Gas exchange was a net output that was estimated
to be -115 kg/year (± 40 percent). Note that to develop these estimates, it was assumed that 10 percent of
the surface waters below the fall line (see Figure II-5) are impacted by urban deposition and that the
loading estimates are sensitive to this assumed percentage value (Chesapeake Bay Program 1999a).

        Several additional mass balance studies are ongoing in Lake Michigan, Long Island Sound, and
the Chesapeake Bay to characterize mercury inputs to as well as losses from these systems (Table II-3).
In Long Island Sound, Fitzgerald (1998) collected and analyzed precipitation, air, surface water, and
biota samples to develop a mass  balance for mercury. In the Chesapeake Bay, Mason et al. (1997)
developed a mercury mass balance based on precipitation, throughfall, and stream water samples. The
mass balance study of Lake  Michigan by Mason and Sullivan (1997) is a smaller effort than the LMMBS
and is primarily a mass-balance modeling exercise based on data extracted through a literature review.

        Similarities among the various mass balance studies include the finding that atmospheric
deposition is a pathway with enough relative contribution in these waters to be of consideration (e.g.,
from 10 to greater than 80 percent). Furthermore, several of these studies indicate that air-water
exchange (through net volatilization) and sediment burial are two major loss pathways.
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                                         Table 11-3
                   Mercury Sources identified in Mass Balance Studies
                                 (by percent contribution)
Location
Lake
Michigan "
Chesapeake
Bay"
Long Island
Sound c
Atmospheric
Deposition
(%)
-80
>50
(Wet 47-53)
(Dry 9-11)
-10
Urban Area
(%)
-30
(Chicago)
Baltimore
(percent not
known)
New York
New Jersey
(percent not
known)
Riverine
-17
-33-49
-52
Ground-
water
<1
Not
reported
Not
reported
Direct
Discharge
Not
reported
Not
reported
-36
Comments
Air-water exchange
and sediment burial
account for the major
loss pathways from
the lake, but
atmospheric
deposition dominates
inputs
Over 90 percent of the
mercury entering the
watershed is retained
in the terrestrial
system and does not
reach the aquatic
system
Tidal exchange,
sediment burial, and
air-water exchange
are major loss
pathways. 45 percent
of the mercury
entering the Sound is
re-emitted
" Mason and Sullivan (1997).
b Mason etal. (1997).
c Fitzgerald (1998).

Factors Affecting Mercury Fate and Transport in Watersheds and
Tributaries

       Recent research illustrates that a number of factors influence whether mercury that is deposited
to watersheds or tributaries will be transported to the lake itself. The principal factors that affect mercury
loading to the aquatic ecosystem appear to be (1) the amount of annual precipitation; (2) the influence of
the urban air plume (in terms of local deposition of the contaminated plume);  (3) storms and other events,
like snowmelt, which influence stream flow and the resuspension of particle-bound mercury in
sediments; and,  (4) prevailing land use (e.g., forestry, agriculture, urban).  Some of these factors appear
to influence the  amount of mercury in throughfall (i.e., precipitation that has washed through the forest
canopy) and litterfall (i.e., fallen leaves) as well as the amount of mercury that is sequestered in organic
soils which prevent its transport through the watershed.

       Rea et al. (1996) found that throughfall and litterfall are the dominant components of mercury
deposition in forested areas of the Lake Champlain basin. Monitoring during  a 6-week period in August
and September 1994 produced estimates of annual throughfall and litterfall deposition of 11.7 u,g/m2/yr
and 13 /ig/m2/yr, respectively. Thus, the total below-canopy deposition rate was estimated to be 24.7
ug/m2/yr, considerably greater than the 15.1 ug/m2/yr wet plus dry deposition estimated by Scherbatskoy
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 et al. (1997). In the former study, precipitation deposition accounted for just 32 percent (or 7.9 ug/m2/yr)
 of this estimated below-canopy deposition.

         Several recent studies related to mercury cycling in the Lake Champlain basin, which focused
 primarily on forested systems, suggest that urban and agricultural systems may retain less atmospheric
 mercury than forested systems. For example, an analysis of mercury deposition and stream export (i.e.,
 transport of mercury out of the basin through streamflow) in an 11 hectare, deciduous forested catchment
 (i.e., a portion of the larger watershed) in the Lake Champlain basin based on field sampling showed net
 annual stream export of mercury was less than 10 percent of wet deposition.  Consistent with an earlier
 study  in the basin, stream export was  strongly related to flow and dominated by mercury in particulate
 form (i.e., mercury complexed with organic material). In 1 year of the study, fully one-half of the total
 annual export occurred on the single day of peak snowmelt.  A more recent stream water sampling and
 deposition monitoring study also showed that most of the mercury transported in stream water is in the
 particulate phase, with the dissolved phase contributing only about 30 percent of the annual export.
 Analysis of soil water mercury reported in this study suggested that the transport of dissolved mercury in
 shallow soil water may be the primary mechanism for mercury movement from the forest floor to
 streams. These studies showed that the forested catchment is a net sink for atmospheric mercury and
 indicated that forests in the Lake Champlain basin help reduce the movement of mercury to the lake
 because the mercury is bound to soil organic matter. Some portion of the mercury is mobilized, however,
 and undergoes three possible fates: transport to streams through groundwater and overland (flood) flow,
 incorporation into vegetation by root uptake, or volatilization back to the atmospheric pool (Scherbatskoy
 et al. 1998, 1997, Shanley et al. 1999) .

 Mercury Exposure and Effects

        Once deposited, mercury may enter terrestrial and aquatic food chains. Mercury concentrations
 increase at successively higher levels  in the food chain such that predators at the top of these food chains
 are potentially at risk from consumption of mercury in contaminated prey. Of the various forms of
 mercury in the environment, methylmercury has the highest potential for bioaccumulation in the food
 chain.  In the Mercury Study Report to Congress, the Agency concluded that fish-eating birds and
 mammals are particularly at risk from mercury emissions and exposures. Ecosystems most at risk from
 airborne releases of mercury exhibit one or more of the following characteristics:

 •      Located in areas where atmospheric deposition of mercury is high;

 •      Include surface waters that are already impacted by acid deposition;

 •      Possess characteristics other than low pH (e.g., high organic content, long aquatic food chains)
       that result in high levels of bioaccumulation; and/or,

 •      Include sensitive species (U.S. EPA 1997e).

       Although a large body of research exists on mercury exposure and effects, as discussed below
 and in  previous Great Waters Reports to Congress, areas of uncertainty remain, particularly with respect
 to mercury methylation processes and their implications for exposure levels. The EPA and others are
 currently planning and conducting research projects to address the fate and transport of mercury
 compounds and subsequent exposures to methylmercury. Some examples of research under way related
 to methylmercury include investigations of the following:
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•      The role of a variety of biogeochemical parameters in watersheds, wetlands, and marine
       environments on mercury bioavailability, bioconcentration, and methylation;

       The effects of anthropogenic ecosystem changes on methylation rates, such as increased sulfate
       deposition, increased nutrient loads, and increased loadings of mercury due to soil disturbance;

       The role of sulfur (especially sulfide) hi mercury methylation in watersheds as related to
       microbial activity; and

•      The effects of agricultural sulfur on methylmercury in soils and wetland areas.

       Effects of mercury can be two-fold. First, mercury in lower-level organisms can impact the
health of those organisms. Next, these organisms become prey for higher-level organisms, resulting in
higher-level organisms having higher concentrations of mercury than the lower-level organisms.
Concentrations of methylmercury in fish tissue have been measured at levels one million times greater
than the mercury concentration in the surrounding water column, illustrating the extent to which
methylmercury can be concentrated in organisms.

       Principal factors affecting the bioavailability of mercury in the waterbody include (1) whether it
is bound to organic matter (which would inhibit bioavailability); and, (2) characteristics of the lake itself,
such as surface area to volume ratio (with more shallow lakes having more bioavailable mercury). When
conditions in a waterbody change (i.e., pH), the bioavailability of a compound can change without a
change in the concentration of the compound.

       Analyzing sediments for mercury concentrations can reveal the extent to which bottom dwelling
organisms are exposed. Eskin et al. (1996) compiled and analyzed sediment contamination data from the
Chesapeake Bay and its tributaries from 1984 to 1991.  The potential for sediment contamination to
impact aquatic life was evaluated by comparing median and maximum contaminant concentrations to no
observed effects levels (NOELs) for aquatic biota, probable effects levels (PELs) for aquatic biota, or
other aquatic health benchmarks.  The NOELs are concentrations above which impacts  on aquatic life are
judged to  be possible. Aquatic life impacts are considered probable at concentrations above the PELs.
For toxic effects to occur, metals must not only be present at concentrations above aquatic life
benchmarks, but must also be bioavailable.

       Where data were available for comparison, sediment mercury concentrations in the Chesapeake
Bay, in general, were lower in 1991 than in previous years. The median and maximum concentrations of
mercury at all locations in the mainstem of Chesapeake Bay were 0.08 and 0.8 ppm, respectively, which
are below the mercury PEL of 1.4 ppm for aquatic biota. However, because maximum concentrations of
mercury in all segments of the bay exceeded the mercury NOEL of 0.1 ppm for aquatic biota, adverse
impacts are still possible. The median and maximum mercury concentrations in tributaries were 0.1 and
4.66 ppm, respectively. Mercury concentrations were highest in the Middle River, other northwestern
tributaries, and near the Sewells Point Naval Complex on the James River. Median mercury
 concentrations exceeded the mercury NOEL for aquatic biota in several tributaries, including the James
 and Potomac Rivers. The PEL concentration for mercury was exceeded only in the James River at
 stations near the Sewells Point Naval Complex.

        Sources with episodic emissions or releases of mercury and other pollutants to the Delaware Bay
 influence concentrations in biota.  Horseshoe crab eggs are of particular importance for monitoring
 efforts because they are a major food source for many species of migrating shore birds during the spring
 migration. While measurements of mercury levels in the eggs of horseshoe crabs from Delaware Bay,
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New Jersey in 1993, 1994, and 1995 do not indicate any temporal trend, levels of mercury varied
markedly among years, with the highest values in 1994 (Burger 1997).  The variations in mercury levels
and the peak in 1994 highlights the importance of episodic sources of pollutants to the Delaware Bay,
which is situated downstream from highly industrialized areas in Trenton, New Jersey; Wilmington,
Delaware; and, Philadelphia, Pennsylvania. Burger (1997) also analyzed mercury concentrations in
female horseshoe crab leg muscle tissues from the Delaware Bay and found that mercury concentrations
were higher in leg muscle tissues than in eggs and were indicative of few adverse effects to developing
horseshoe crabs.

        In an evaluation of higher level organisms, Brazner and DeVita (1998) detected mercury in
yellow perch and spottail shiners from 23 sites in Green Bay, Lake Michigan. The overall distribution of
mercury tissue concentrations was fairly uniform within the bay, indicating that mercury contamination
originates primarily from non-point sources, including atmospheric deposition.  Certain sites exhibited
unusually high mercury residues in fish, however, suggesting these sites may be associated with direct
discharges of mercury nearby.  The mercury residue levels of 9.4 to 31.0 ng/g in yellow perch and 10.5 to
33.5 ng/g in spottail shiners were well below the International Joint Commission Aquatic Life Guideline
for total mercury of 500 ng/g. Furthermore, these mercury levels were similar to or below the most
recently reported (i.e., 1993, 1985) mercury levels in fish in most of the locations in the Great Lakes.

        Mercury levels apparently decreased in yellow perch taken from the St. Lawrence River, which
drains the Great Lakes, in 1991-1992 and were compared to results from a 1975 study (Ion et al. 1997).
Mercury was detected in all yellow perch samples taken from various sites along the river. Comparison
of average mercury concentrations to historical levels in St. Lawrence River fish indicates a two- to
three-fold decrease since  1975. Because mercury contamination and bioaccumulation can vary
considerably from site to  site and species to species, additional studies of this type are needed for trends
analysis of mercury levels in fish.

        Fish-eating birds  are of particular interest for evaluating the effects of mercury because relative
to their body weight, exposures can be very high. Hughes et al. (1997) detected significant differences in
mercury concentrations in both osprey eggs and chick feathers from nests  at four Great Lakes study areas
in Ontario (three natural lakes and one reservoir) and two Delaware Bay sites in New Jersey. Overall,
eggs from the Ogoki Reservoir and chick feathers from St. Mary's River (Ontario) and the  Ogoki
Reservoir had significantly higher mercury concentrations than the eggs and feathers sampled from the
other locations. Despite these geographic variations, mercury levels in osprey eggs, chick feathers, and
adult feathers at all locations were below the levels associated with toxic reproductive effects, such as
reduced number of eggs, decreased hatchability, increased hatchling mortality, and altered reproductive
behavior. Fish sampled at each site also exhibited significant differences in mercury levels with a clear
spatial pattern, similar to that observed for chick feathers. However, the study did not assess the relative
impact of point source discharges and atmospheric deposition on spatial variation.

        In a recent study that attempted to link spatial variations in mercury levels in biota with
variations in atmospheric deposition of mercury, Evers et al. (1998a) found that mercury concentrations
in the feathers and blood of adult and juvenile common loons from sites within five regions across North
America (Canadian Maritimes, New England, Upper Great Lakes, northwestern U.S., and Alaska)
increased significantly from western regions to eastern regions.  Adults had average blood mercury levels
which were 10 times higher than juveniles. Feather mercury levels increased significantly over a 4-year
period, probably due to bioaccumulation of mercury over that time period. At some of the study
locations where exposure is high (e.g., some eastern North American locations), the loon's natural
mechanisms to excrete excess mercury (e.g., feathers,  eggs, demethylation and storage in the liver and
kidney) may not be sufficient to balance current exposure levels. The researchers note that the observed
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geographical gradient agrees with EPA's Regional Environmental Monitoring and Assessment Program
(R-EMAP) modeling of atmospheric deposition of mercury and predicted high impact areas (U.S. EPA
1997e) and the Northeast States and Eastern Canadian Provinces Mercury Study (NESCAUM 1998).
Within the upper Great Lakes region (nine sites total), blood mercury levels were influenced the most by
lake biogeochemistry and hydrology, rather than atmospheric deposition. Significantly higher
concentrations from sites in north-central Wisconsin and central Ontario were detected.  The authors
conclude that loons breeding on low-pH lakes in the upper Great Lakes and in all lake types in
northeastern North America are the most at risk from mercury contamination. A comparison of the
measured blood mercury concentrations to health threshold levels determined from laboratory studies
indicate that 12 to 31 percent of New England's breeding loon population exceed these levels (Evers
1998b). Based on feather mercury levels, over 30 percent of the male loons exceed threshold levels for
health effects.

       Like wildlife, fish consumption represents the dominant pathway for human exposure to
methylmercury.  Given the current scientific understanding of the environmental fate and transport of this
element, it is not possible to quantify how much of the methylmercury in fish consumed by the U.S.
population is contributed by U.S. emissions relative to other sources of mercury (such as natural sources
and re-emissions from the global pool). As a result, it cannot be assumed that a change in total mercury
emissions will be linearly related to any resulting change in methylmercury in fish, nor over what time
period these changes would occur.  This is an area of ongoing study.

       The effects of methylmercury on humans and especially the developing fetus are well known and
have been described in detail in earlier Reports to Congress.  The critical target for methylmercury
toxicity for humans is the nervous system. The factors that affect whether the mercury exposure is
sufficient to cause health effects depend primarily on the species of fish consumed, the concentration of
methylmercury in the fish, the quantity of fish consumed, and how frequently fish is eaten. The 1997
EPA Mercury Study Report to Congress includes a detailed analysis of potential public health impacts
relating to fish consumption.  This analysis was based on information on the mercury levels in various
types offish, dietary surveys, and EPA's current reference dose (RfD) for methylmercury. The RfD is an
estimated daily ingestion level anticipated to be without adverse effect to persons, including sensitive
subpopulations, over a lifetime. Note that the National Academy of Science is currently reviewing more
recent mercury health effects studies and will recommend whether the EPA should revise its RfD for
methylmercury.  This review and recommendation is expected to be completed by mid-2000.

       The Mercury Study report concluded that the typical U.S. consumer eating fish from restaurants
and grocery stores was not in danger of consuming harmful levels of methylmercury from fish and is not
advised to limit fish consumption on the basis of mercury content. However, eating more fish than is
typical or eating fish that are more contaminated than typical fish can change the advice. Because the
developing fetus is regarded as the most sensitive to the effects of methylmercury, women of
child-bearing age are the population of greatest concern.

        In addition,  for cultural or economic reasons,  some people in certain ethnic groups (e.g., Asians,
Pacific Islanders, Native Americans) and subsistence fishers eat substantially more fish than the average
consumer. Because of the higher amounts offish in their diets, people in these groups, especially the
women of child-bearing age, need to be aware of how much mercury is in the fish they consume. The
Mercury Study report has more detailed information about amounts of mercury found in various types of
fish.

        The Food and Drug Administration (FDA) and State, local, and tribal agencies issue advisories
that suggest limiting the consumption of contaminated fish. Mercury fish advisories in the U.S. have been
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 issued by 40 States and some tribes.  Eleven States have Statewide advisories for mercury in freshwater
 lakes or rivers, and five States have Statewide advisories for mercury in coastal waters.  Based on data
 from December 1997, 20 of 56 Great Waters are associated with mercury fish consumption advisories
 (U.S. EPA 1998m). The EPA is sponsoring work with the State of Wisconsin to assess current methods
 of communicating fish consumption advisories and to recommend improvements.

        Despite this advice, a recent survey on awareness and effectiveness offish advisories found that
 only half of the Great Lakes sport fish consumers were aware of health advisories related to fish
 consumption (Tilden et al. 1997). While one study of Lake Ontario anglers concluded that the angler
 subpopulation's health does not significantly differ from those experienced by the general North
 American population (Cole et al.  1997), a different study concluded that the consumption of
 contaminated fish affected time-to-pregnancy (i.e., the amount of time between when a women plans to
 become pregnant and the date of pregnancy). The study also  found that 42 percent of the women
 surveyed reported consumption of contaminated fish from Lake Ontario,  despite highly publicized
 advisories against the consumption offish from Lake Ontario by women  of reproductive age (Buck et al
 1997).

        According to Tilden et al. (1997), the most widely accepted advisory recommendation was
 cleaning and cooking methods. While cooking methods are effective to reduce PCB exposure, mercury
 concentrations will actually increase, on a per weight basis, with all cooking methods (including pan
 frying, deep-frying, baking, boiling, and smoking) because of the moisture and fat lost during cooking
 (Morgan et al. 1997). Unlike PCBs which accumulate in fatty tissue that can be removed prior to
 consumption, mercury accumulates in the muscle tissue or filet portion.

        Studies of mercury exposure in U.S. populations are limited, particularly for the general
 population. However, research is being planned as part of EPA's draft Mercury Research Strategy (see
 Chapter III) to address this need.  A number of studies have been conducted involving sport fisherman
 and Native peoples, which have shown high levels offish consumption in a number of populations; but,
 risk of exposure is dependent, in large part, on the level of contamination in the fish (U.S. EPA 1997e).
 A recent study of Ojibwa tribal members from the Great Lakes region indicates that mercury
 concentrations in Ojibwa populations are low; however, researchers identified several individuals with
 elevated levels of mercury (Gerstenberger et al. 1997).

 OTHER METALS (LEAD AND  CADMIUM)


 Sources and Emissions of Lead and Cadmium

       Lead and cadmium are naturally-occurring trace metals and, therefore, are expected to be
 detected at some background level in the environment, depending on the location.  Furthermore, because
 lead  and cadmium are metals, they are by nature persistent compounds that may cycle between
 environmental compartments.  Therefore, while it is possible to estimate lead and cadmium emissions
 from anthropogenic sources, it is difficult to determine which  sources (e.g., specific human-made
 sources, natural sources, cycling) contribute to total and atmospheric deposition inputs to the Great
 Waters.

       Based on a study of lead, cadmium, and other trace metals emissions and air concentrations in
 the Great Lakes region from 1982 to 1993, (1) sources of lead in 1993 included steel manufacturing, coal
 combustion, non-ferrous metal production, and waste disposal (Figure II-3), and (2) sources of cadmium
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in 1993 included coal combustion,
solid waste and sewage sludge
incineration, iron-steel
manufacturing, non-ferrous metals
production, and several smaller
sources (Figure II-5) (Pirrone and
Keeler 1996).

        A review of cadmium and
lead emission sources on a national
scale, based on EPA's National
Toxics Inventory for the time period
from 1990-1993 (1990-1993 NTI),
provides a somewhat different
picture compared to regional
sources for the Great Lakes (Tables
II-4 and II-5).  The larger national-
level sources of lead air emissions
are mobile sources, including non-
road vehicles and equipment
(aircraft) and on-road vehicles. The
larger national-level sources of
cadmium air emissions are
secondary lead smelting, primary
copper smelting, and primary lead
production (U.S. EPA 1999a). The
NTI data for lead air emissions also
indicate that there are many source
categories that are emitting similar
amounts of lead compounds, rather
than there being a few source
categories contributing the majority
of the air emissions. The              .^	
differences observed between the
local (Figures II-3 and II-5) and
national (Tables II-4 and II-5) source characterizations for these pollutants highlight the importance of
examining both local sources and regional sources, as well as the need to consider the influence of urban
areas on nearby waterbodies.

        A study of lead emissions and air concentrations indicates that, overall, U.S. lead emissions have
decreased since the 1970s, primarily due to the phaseout of leaded gas. Lead emissions in the Great
Lakes region decreased steadily from 1982 to  1993 at a rate of about 6.4 percent per year. Lead
emissions in the Great Lakes region in 1988 were estimated to be 4,430 tpy.  Lead concentrations in
ambient air also showed steady declines over the entire region between 1982 and 1993. The regional
decrease in lead emissions and air concentrations is correlated to the reduction of lead in gasoline (from
0.28 g/1 in 1982 to 0.026 g/1 in 1989) and an increase in unleaded gasoline use  in both the U.S. and
Canada since  1981.  Sources of lead emissions also shifted over this time period. As shown in Figures II-
3 and II-4, about 80 percent of lead emissions were from leaded gasoline use in 1982 compared to 1993
when most lead emissions were  from four major industrial sources in the Great Lakes region (Pirrone and
Keeler  1996). Another study of lead deposition  to sediments in Central Park Lake in New York City


Page H-20           Deposition of Air Pollutants  to the Great Waters - 3rd Report to Congress 2000
                       HIGHLIGHTS
             Other Metals (Lead and Cadmium)

>• Sources. In some urban locations, local sources (versus
regional sources) are primarily responsible for atmospheric
deposition of lead and cadmium to the Great Lakes, whereas the
opposite is true in some more remote locations.  The largest
national sources of lead air emissions are mobile sources, including
non-road vehicles and equipment (aircraft) and on-road vehicles.
Emissions and ambient air concentrations of lead have continued to
decrease since the 1970s. The largest national sources of
cadmium air emissions include secondary lead smelting, primary
copper smelting, and primary lead production. Cadmium air
emissions increased from 1982 to 1988 in the Great Lakes region
and have not shown a trend since 1988.

>• Loadings.  In the Great Lakes region, lead deposition
decreased from 1988 to 1994, and cadmium deposition may have
decreased from 1992 to 1994.  In the Chesapeake Bay,
atmospheric deposition of cadmium  and lead contributes no more
than 5 to 7 percent, respectively, to total loadings.  Total inputs from
all pathways of lead and cadmium increased in the eastern section
of the bay from 1966 to 1995 due to the increase in human
population and industrial activities. However, trends in the relative
contribution  of atmospheric deposition of lead and cadmium to the
Chesapeake Bay have not been discerned.  In the Long Island
Sound, lead inputs have been decreasing since  1980 and
atmospheric deposition contributes 70-90 percent of total lead
inputs.

>• Environmental Concentrations.  Sediment contamination
studies in the Chesapeake Bay provide conflicting results - one
study found  increased lead and cadmium levels, possibly due to an
increase in population, industrial activities, and agricultural activities,
whereas another found decreasing levels. Lead and cadmium
levels in Chesapeake Bay sediments, in general, were between the
aquatic biota NOEL and PEL; however, bioavailability of these
metals  is low.  In the Delaware Bay, lead levels decreased in
horseshoe crab eggs in recent years, but cadmium levels were
more variable.

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                                                                                     Chapter II
                                                                        Environmental Progress
 using sediment cores indicates, however, that municipal solid waste incineration contributed a large
 portion of the lead deposited during the same time period that lead from leaded gasoline was deposited.
 Furthermore, lead emissions from municipal solid waste incinerators decreased beginning in 1966 due to
 progressive facility closures following regulations. Therefore, although it is clear that lead emissions and
 deposition have decreased, it is possible that solid waste incineration has been underestimated as a source
 of atmospheric lead in the past, particularly to urban areas (Chillrud et al. 1999).

        In contrast to lead emissions and ambient air concentrations, cadmium emissions in the Great
 Lakes region increased from 1982 to 1988 at a rate of 5.2 percent per year, with a peak in 1988 at 150
 tpy. Since 1988, emissions of cadmium have not increased or declined (Pirrone and Keeler 1996).

 Deposition of Lead and  Cadmium.

        Data collected under the Integrated Atmospheric Deposition Network (IADN), a joint U.S.-
 Canada program that monitors pollutant levels in air and precipitation at remote sites in the Great Lakes
 region, by Eisenreich and Strachan in 1992 and Hoff et al. in 1994 show that total deposition of lead
 decreased from 1988 to 1994 in each of the Great Lakes.  Paode et al. (1998) found that measured
 average lead fluxes in Chicago, Illinois were 0.07 mg/m2/day, whereas over Lake Michigan, lead fluxes
 were 0.003 mg/m2/day, demonstrating the urban influence of Chicago on atmospheric deposition of lead
 onto Lake Michigan. Dry deposition of cadmium in the Great Lakes region decreased from 1992 to
 1994; however, this decrease may be due to improved averages in the particulate air concentrations of the
 metals (Hoff et al. 1996). Sweet et al. (1998) estimated annual wet and dry deposition rates to Lake
 Michigan, Lake Erie, and Lake Superior using air and rain concentrations of lead and cadmium measured
 at three U.S. IADN sites and found that lead and cadmium deposition levels were similar at all lakes.
 Since the IADN sites are situated in remote locations, this finding indicates regional atmospheric
 deposition, rather than local emissions, is the source of lead and cadmium at the remote sites on these
 three lakes.

        Estimates of total inputs of trace metals  to the Chesapeake Bay indicate that inputs of trace
 metals from the non-tidal watershed are much higher than trace metal inputs to tidal waters from point
 source discharges, urban storm water inputs, and direct atmospheric deposition to the tidal waters. The
 boundary for the non-tidal and tidal waters in the Chesapeake Bay region is indicated in Figure II-6.

        Inputs from the non-tidal watershed to the Chesapeake Bay consist of all point and non-point
 sources, including atmospheric deposition. Atmospheric  deposition (measured as direct deposition to
 water surfaces based on monitoring data) of cadmium and lead contributes approximately 4.6 and 5.6
 percent, respectively, to total inputs to the Chesapeake Bay (Table II-6). Note that these percentages may
 be underestimates because the monitoring site locations do not reflect the urban influences of Baltimore,
 Maryland on the Chesapeake Bay. However, these percentages are similar to those for other metals but
 are much less than percentages for polycyclic aromatic hydrocarbon (Eskin et al. 1996).
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Chapter II
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                                     Figure 11-3
                   1993 Lead Emissions in the Great Lakes Region
                              (Pirrone and Keeler 1996)
                                                        Non-ferrous metal production


                                                        Steel manufacturing

                                                        Waste disposal

                                                        Coal combustion
                                                    S!H Other
                                     Figure II-4
                    1982 Lead Emissions in the Great Lakes Region
                              (Pirrone and Keeler 1996)
                                                                 Leaded Gas
                                                                 Other
Page 11-22
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                                                                              Chapter II
                                                                  Environmental Progress
                                       Figure 11-5
                    1993 Cadmium Sources in the Great Lakes Region
                               (Pirrone and Keeler 1996)
                                                            Coal Combustion
                                                            Incineration
                                                            Iron-Steel Manufacturing

                                                            Non-Ferrous Metals Production

                                                            Other
                                       Table II-4
                      National Anthropogenic Lead Air Emissions
                 (Based on EPA's 1990-1993 National Toxics Inventory)
Source Category
Mobile sources: non-road vehicles and equipment - aircraft
Mobile Sources: on- road vehicles
Primary lead
Steel wire and related products manufacturing
Mobile sources: non-road vehicles and equipment - other
Primary copper smelting
Pulp and paper: combustion
Lead oxide in pigments
Secondary lead smelting
Anthropogenic
Air Emissions
(tons/year)
619
418
259
163
158
152
150
136
106
Percent Contribution
to Total U.S.
Anthropogenic Air
Emissions
18.7
12.6
7.8
4.9
4.8
4.6
4.5
4.1
3.2
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Chapter n
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Source Category
Municipal waste combustion
Non-stainless steel manufacture - EAF
Utility boilers: coal combustion, all types
Secondary copper smelting
Medical waste incineration
Hazardous waste incineration
Secondary nonferrous metals production
Pressed and blown glass and glassware manufacturing
Storage batteries manufacturing
Portland cement manufacture: hazardous waste-fired
Primary nonferrous metals production
Paint application: no spray booth
Others (< 1 percent each) a
Total U.S. Anthropogenic Lead Air Emissions
Anthropogenic
Air Emissions
(tons/year)
80
79
72
71
63
56
55
52
51
41
40
35
454
3,31 Ob
Percent Contribution
to Total U.S.
Anthropogenic Air
; Emissions
2.4
2.4
2.2
2.2
1.9
1.7
1-7
1.6
1.5
1.2
1.2
1.1
13.7
100"
* A list of the source categories that contribute less than 1 percent to total U.S. emissions is provided in Appendix B.
b This value represents anthropogenic lead air emissions in the U.S. only.
Source: U.S. EPA 1999a
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                                                                                 Chapter II
                                                                    Environmental Progress
                                        Table 11-5
                    National Anthropogenic Cadmium Air Emissions
                 (Based on EPA's 1990-1993 National Toxics Inventory)
Source Category
Secondary lead smelting
Primary copper smelting
Primary lead
Hazardous waste incineration
Petroleum refining: catalytic cracking units
Municipal waste combustion
Medical waste incineration
Cadmium refining and cadmium oxide production
Secondary copper smelting
Industrial inorganic chemical manufacturing
Sewage sludge incineration
Cadmium stabilizers production
Pulp and paper: combustion
Portland cement manufacture: hazardous waste-fired
Inorganic pigments: cadmium pigments in plastics
Primary nonferrous metals production
Others (<1 percent each) a
Total U.S. Anthropogenic Cadmium Air Emissions
Anthropogenic
Air Emissions
(tons/year)
84
16
16
9
7
5
5
5
5
4
4
4
3
2
2
2
28
201b
Percent Contribution
to Total U.S.
Anthropogenic Air
Emissions
42.2
8.1
7.9
4.3
3.3
2.5
2.4
2.3
2.3
2.2
1.9
1.8
1.7
1.2
1.1
1.0
13.8
100"
' A list of the source categories that contribute less than 1 percent to total U.S. emissions is provided in Appendix B.
b This value represents anthropogenic cadmium air emissions in the U.S. only.
Source: U.S. EPA1999a
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Chapter II
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                                          Figure 11-6
                        Chesapeake Bay Tidal and Non-tidal Waters
                                (Tributary basins are shaded)
                    James
                    River
                    Basin
                                         Fallllne'
                                                                  Chetapeake
                                                                  Bay
Note: Fall line is the upper boundary of the tidal waters of the Chesapeake Bay.
Source: Chesapeake Bay Program 1994

                                           Table II-6
                    Trace Metal Inputs to the Chesapeake Bay (kg/year)
Trace
Metal
Cadmium
Lead
Total Inputs to
Chesapeake
Bay3
27,800
275,300
Direct
Atmospheric
Deposition to
Tidal Waters
1,200
14,500
Direct Atmospheric
Deposition to Tidal
Waters as Percent of
Total Inputs
-4.6
-5.6
                 1 Includes inputs from the non-tidal watershed (including atmospheric
                 deposition to the watershed), storm water inputs to the tidal waters, point
                 source inputs to the tidal waters, and direct atmospheric deposition to the
                 tidal waters.
                 Source: Eskin etal.  1996
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                                                                                     Chapter II
                                                                        Environmental Progress
        Data collected by the Chesapeake Bay Atmospheric Deposition Study (CBADS),1 as presented in
 the Chesapeake Bay Program's 1999 Toxics Loading and Release Inventory (TLRI), result in estimates of
 total inputs to the Chesapeake Bay for cadmium and lead (42,600 and 254,000 kg/year, respectively) that
 are similar to the Eskin et al. (1996) values. Inputs of lead and cadmium via atmospheric deposition to
 the tidal waters of the Chesapeake Bay as a percentage of the total inputs are 7 percent and 3 percent,
 respectively. Inputs from the non-tidal watershed dominate for lead and cadmium (Chesapeake Bay
 Program 1999a, 1994).

        A study on the eastern shore of the Chesapeake Bay in Maryland using sediment cores found that
 lead deposition rates range from 0.32 ± 0.20 to 13.60 ± 0.98 mg/m3/yr, and cadmium deposition rates
 range from 0.01 ± 0.01 to 0.43 ± 0.04 mg/nf/yr. Total inputs of both lead and cadmium from all
 pathways increased from 1966 to 1995 due to the increase in human population and industrial activities
 (Karuppiah and Gupta 1998).

        Direct atmospheric deposition rates of lead and cadmium to the Massachusetts Bay based on
 monitoring data are presented in Table II-7. In general, deposition of lead and most other metals is
 higher at the monitoring site closer to Boston due to higher urban area emissions. However, deposition
 of cadmium is similar at both the urban and rural locations. While there is not a seasonal trend for trace
 metal deposition in general, higher dry deposition of lead has been observed in the winter (Golomb et al
 1997a).

                                           Table 11-7
                   Direct Atmospheric Deposition of Lead  and Cadmium
                              to Massachusetts Bay (ug/m2/yr)
Trace Metal
Cadmium
Lead
Total
Urban
260
2,300
2,560
Rural
280
1,400
1,680
                          Source: Golomb etal.1997a

        In Long Island Sound, sediment cores from salt marshes indicate that lead inputs reached a
maximum between 1970 and 1980 at approximately 62 ug/cm2/yr and have been decreasing since that
time at most sites. Atmospheric deposition to the water surface of Long Island Sound contributes
approximately 90 percent of total lead inputs.  At sites closer to New York City, cores show that
atmospheric deposition accounts for approximately 70 percent of lead inputs, suggesting that non-
atmospheric sources (e.g., direct discharges, storm water runoff) play a larger role near the urban areas
(Cochran et al. 1998).
       1 CBADS measurements include wet deposition, dry deposition, and gas exchange of pollutants at rural
sites, with estimations for urban areas.
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Chapter II
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Lead and Cadmium Levels in the Environment

        Lead and cadmium levels have been measured in a variety of environmental media and in a wide
range of geographic locations in the Great Waters.  The concentrations that are observed in the
environment are a result of atmospheric deposition from both domestic and international sources as well
as from non-atmospheric sources, including storm water runoff and direct discharges to waterbodies and
tributaries.
                                             Seasonal Variation in Cadmium Concentrations

                                        A monitoring study of the St. Lawrence River, which connects
                                        the Great Lakes with the Atlantic Ocean, emphasized the
                                        importance of seasonal variation on the concentration and
                                        distribution of metals.  Quemerais and Lum (1997) collected
                                        water from sites in the river and four of its tributaries from
                                        March to November 1991  and April to June 1992 and analyzed
                                        the samples for dissolved and particulate cadmium. The mean
                                        dissolved cadmium concentration for the basin (10 + 5 ng/L)
                                        was in the same range as that measured for rivers considered
                                        pristine environments. The mean particulate cadmium
                                        concentration (1.3 ±1.1 ug/g) was also relatively low in
                                        comparison to other waterbodies. Dissolved cadmium
                                        concentrations exhibited a seasonal trend; concentrations
                                        increased in spring and autumn and decreased in summer.
                                        The trend was attributed to increased runoff and leaching from
                                        soil during spring snowmelt and rainfall events in autumn as
                                        well as uptake by surface water microorganisms during
                                        summer. The seasonal variation of particulate cadmium was
                                        not as apparent, probably due to the negative influence of
                                        suspended particulate matter, which is higher in spring and
                                        autumn as a result of snowmelt and rainfall patterns.
       A recent study in the
Chesapeake Bay found an increase in
lead and cadmium concentrations in
and toxicity of the sediments and pore
water (i.e., interstitial water of
sediments) of two tributaries
(Wicomico River and Pocomoke River)
in comparing sediment cores from
1966-1975 to sediment cores from
1986-1995 (Table II-8).  The authors
examined the historical land use of
areas adjacent to these rivers and
concluded that the increases were likely
due to a variety of pathways.
Specifically, (1) increases in metal
concentrations in Wicomico River
sediments and pore water are probably
due to an increase in population,
industrial activities, and the volume of
the sewage treatment plant influent; (2)
increases in metal concentrations in
Pocomoke River sediments and pore water are probably due to the increased runoff from agricultural
areas, including poultry farms;  and, (3) increases in lead concentrations in Wicomico River sediments
and pore water are possibly due to an increase in various industrial activities, commercial facilities that
use lead compounds, and atmospheric deposition (Karuppiah and Gupta 1998).

       Other studies have found that sediment concentrations of lead and cadmium are declining,
however.  Sediment concentration data from the Chesapeake Bay Program from 1984 to 1991, for
example, indicate that lead and cadmium concentrations in sediments are declining in some areas of the
Chesapeake Bay (Eskin et al. 1996).

       An analysis of spatial trends shows that metals concentrations in sediments of the mainstem of
the bay were lowest at the head of the bay and in the extreme lower bay.  The highest metals
concentrations were detected in sediments of the segment of the bay closest to Baltimore, the largest
urban center on the bay. Lead  contamination trends were somewhat different when concentrations were
normalized by the fine particle content of the sediment. In particular, normalized sediment
concentrations of lead gradually declined toward the mouth of the bay, suggesting that the Susquehanna
River is the primary source of lead. Lead concentrations were highest in the Middle River, other
northwestern tributaries, and near the Sewells Point Naval Complex on the James River. The distribution
of cadmium contamination was different from other contaminants, where the highest concentrations were
located in the sediments of the James  (near the Sewells Point Naval Complex) and Patuxent Rivers and in
some of the southeastern tributaries (Eskin et al. 1996).
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                                                                                   Chapter II
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                                          Table 11-8
        Temporal Changes in Metal Concentrations in Chesapeake Bay Tributaries
                                 Based on Sediment Cores
Sediment
Core Depth
(cm)
Estimated
Period
(year)
Lead
Sediment
(mg/kg)
Pore Water
(mg/L)
Cadmium
Sediment
(mg/kg)
Pore Water
(mg/L)
Wicomico River
0-7.5
7.5-15.0
15.0-23.0

0-7.5
7.5-15.0
15.0-23.0
1986-1995
1976-1985
1966-1975
18.01
7.60
7.43
5.12
0.54
0.42
0.49
0.48
0.37
0.026
0.008
0.007
Pocomoke River
1986-1995
1976-1985
1966-1975
5.14
3.51
2.35
0.74
0.59
0.59
0.28
0.24
0.20
0.025
0.003
0.002
     bource: Karuppiah and Gupta 1998

        The potential for sediment contamination to impact aquatic life was evaluated by comparing
median and maximum sediment contaminant concentrations to aquatic health benchmarks in both the
mainstem of the Chesapeake Bay and its tributaries (Table 11-9).  Maximum concentrations of cadmium
and lead in the mainstem of Chesapeake Bay were below PEL concentrations for aquatic biota.
However, impacts must be considered possible because maximum lead and cadmium concentrations
exceeded the aquatic biota NOEL in most of the upper half of the bay and at the mouth of the Potomac
River (Eskin et al. 1996).

        In the Chesapeake Bay tributaries, median and maximum lead concentrations in sediments were
31 and 343 parts per million (ppm), respectively.  Median lead sediment concentrations exceeded the
lead NOEL in northwestern tributaries, but the aquatic biota PEL for lead was exceeded only near the
Sewells Point Naval Complex.  The median and maximum cadmium sediment concentrations were 0.6
and 6.0 ppm, respectively. The distribution of cadmium contamination was different from other
contaminants, where the highest concentrations were located in the James (near the Sewells Point Naval
Complex) and Patuxent Rivers and in some of the southeastern tributaries. Median cadmium sediment
concentrations in several of the western and northwestern tributaries exceeded the aquatic biota NOEL;
however, the maximum concentrations did not exceed the PEL for aquatic biota (Eskin et al. 1996).

       For toxic effects to be possible, metals must not only be present at concentrations above aquatic
life benchmarks but must also be bioavailable (i.e., available for uptake by organisms).  For instance, a
portion of the lead in sediments must not be bound to the organic matter in the sediment, and the lead
levels in the sediment must exceed the aquatic life benchmark in order for toxic effects  to occur. Eskin et
al. (1996) found low bioavailability through most of the mainstem of the bay. However, bioavailable
conditions were found in a northern reach of the bay from Turkey Point to Annapolis.  This reach
includes the most contaminated segment of the bay, between Baltimore and Annapolis (Eskin et al.
1996).
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Chapter n
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                                         Table 11-9
            Cadmium and Lead in Sediments of the Chesapeake Bay Mainstem
Contaminant
Cadmium
Lead
Concentration
Median
(ppm)
0.4
35
Maximum
(ppm)
2.9
86
Aquatic Life
Benchmark
NOEL"
(ppm)
1.0
21
PEL"
Jppm)
7.5
160
Location of Maximum
Concentrations
Baltimore region south to
the Little Choptank River;
mouth of Potomac River
Baltimore region
Trends
Concentrations
are declining
Concentrations
are declining in
some areas
 * No Observed Effect Level. Level above which impacts are considered "possible.
 b Probable Effect Level. Level above which impacts are considered "probable."
 Source: Eskin et al. 1996

       In the Delaware Bay, one study attributed decreases in lead levels in horseshoe crab eggs to a
general lowering of pollutants to the bay. Horseshoe crab eggs provide a bioindicator of pollutant levels
in the Delaware Bay because they are laid beneath the sand at the bay's high tide line and are
continuously inundated with water. Burger (1997) measured levels of lead and cadmium in the eggs and
leg muscles of horseshoe crabs in 1993, 1994, and 1995 in the Delaware Bay and found a decrease in
lead levels in horseshoe crabs from 1993 to 1995. Cadmium levels in the eggs were significantly higher
in 1994 than hi 1993 or 1995 (Table 11-10). The variations in cadmium levels may suggest an episodic
source of cadmium to the bay, which is probable given the high level of upstream industrialization in
Trenton, New Jersey; Wilmington, Delaware; and, Philadelphia, Pennsylvania.  Burger (1997) also
analyzed lead and cadmium levels in female horseshoe crab leg muscle tissues from the Delaware Bay
and found that lead and cadmium levels hi leg muscle tissues were lower than in eggs and were indicative
of few adverse effects.

                                         Table 11-10
              Lead and Cadmium in Horseshoe Crab Eggs from Delaware Bay
Year
1993
1994
1995
Lead (ppb)
558 (±160)
206 (±34)
87 (±8)
Cadmium (ppb)
17 (±5)
310 (±130)
24 (±7)
                 Source: Burger 1997
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                                                                                       Chapter II
                                                                          Environmental Progress
 COMBUSTION EMISSIONS

 Dioxins and Furans

         Polychlorinated dibenzo-p-dioxins
 (PCDDs; dioxins) and polychlorinated
 dibenzofurans (PCDF; furans) are compounds that
 are similar in structure but differ in the number
 and position of chlorine atoms. Much of the
 current research uses toxic equivalent quantities
 (TEQs) to express quantities of dioxins and
 furans. The TEQs aggregate all of the dioxin and
 furan congeners into a single factor that is
 weighted by toxicity of the individual congeners
 based on ratios to 2,3,7,8-tetrachlorodibenzo-p-
 dioxin (2,3,7,8-TCDD) and to 2,3,7,8-
 tetrachlorodibenzofuran(2,3,7,8-TCDF).
 Therefore, dioxin and furan  quantities are
 commonly expressed as dioxin TEQs and furan
 TEQs, respectively.  This is  the convention
 followed in this report to the extent permitted by
 the research results reported in the literature.
                 HIGHLIGHTS
              Dioxins and Furans

> Sources. The largest sources of dioxin and furan
emissions in the U.S. are municipal waste
combustion and medical waste incineration. By
2002, controls applied to these sources will reduce
their dioxin and furan emissions by 95-99 percent
(see Chapter III).

>• Loadings. In the Great Lakes region, sediment
accumulation rates indicate a decline in dioxin and
furan inputs since the 1970s. The relative
atmospheric contribution and sediment accumulation
rates of dioxins and furans entering the Great Lakes
differs both between and within the lakes.  In some
lakes, the atmospheric contribution of dioxins and
furans is 100 percent, whereas in other lakes, the
atmospheric contribution of dioxins and furans is less
than 5 percent.  In general, the pattern of
industrialization around the lakes influences relative
contributions and accumulation rates.

>• Concentrations in Biota.  In general, long-term
monitoring data indicate that dioxin and furan
concentrations in biota in many Great Waters have
declined over time.
        Dioxins and furans are byproducts of
combustion that enter the environment primarily as a result of waste incineration and, to a lesser extent,
various manufacturing processes, but also through natural combustion processes. Different sources emit
different dioxin and furan compounds in certain combinations.  These combinations, or source profiles,
can then be used to identify the source of the emissions. One such study developed a chemical mass
balance model to determine the contribution of different types of sources to sediment levels in the
Housatonic River in Connecticut, Lake Huron, and the Baltic Sea.  The study found that air paniculate
matter, coal-fired power plants, municipal incinerators, and pentachlorophenols (from manufacturing)
were, in general, the largest sources of dioxins and furans  in sediments. The same study reported that
coal-burning was the major source of dioxins and furans prior to 1955 in the U.S. and 1970 in Europe,
with municipal incinerators dominating after that time (Su and Christensen  1997). These results are
similar to recent EPA estimates of national air emissions and sources of dioxin and furan TEQs which
indicate that of the 0.0027 tpy of dioxin and furan TEQ air emissions, municipal waste combustion
accounts for 47 percent and medical waste incineration accounts for 24.6 percent (Table II-l 1).  A large
number of smaller sources also emit dioxins and furans (U.S. EPA 1999a).

        Emissions data for the U.S. and Canada were used with NOAA's hybrid single particle
Lagrangian integrated trajectory (HYSPLIT)/transfer coefficient (TRANSCO) computer program to
analyze dioxin and furan sources and their contributions to atmospheric deposition of dioxins and furans
in the Great Lakes. For any given lake, the simulation results indicated that approximately half of the
atmospheric deposition of dioxins and furans arose from sources in the immediately surrounding States
and provinces, and half arose from the remainder of the U.S. and Canada. Furthermore, the relative
contribution of sources by class were ranked, showing that municipal waste incineration, iron sintering,
cement kilns burning hazardous waste, and medical waste  incineration are responsible for at least 85
percent of the total atmospheric deposition of dioxins and  furans to the Great Lakes. This study also
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Chapter II
Environmental Progress
found that sources of dioxins as far away as central Canada may influence deposition of dioxins to the
Great Lakes (Cohen et al. 1995).

                                          Table 11-11
               National Anthropogenic Dioxin and Furan TEQ Air Emissions
                   (Based on EPA's 1990-1993 National Toxics Inventory)
Source Category
Municipal waste combustion
Medical waste incineration
Secondary aluminum smelting
Utility boilers: coal combustion, all types
Industrial boilers: wood/wood residue combustion
Mobile sources: on-road vehicles
Open burning: wildfires and prescribed burnings
Portland cement, excluding hazardous waste-fired
Residential wood/wood residue combustion
Wood treatment/wood preserving
Others (< 1 percent each) a
Total U.S. Anthropogenic Dioxin and Furan TEQ Air
Emissions
Anthropogenic
Air Emissions
(tons/year)
0.0012
0.0007
0.0002
0.0001
0.00009
0.00009
0.00009
0.00004
0.00004
0.00003
0.00007
0.0027b
Percent Contribution to
Total U.S. Anthropogenic
Air Emissions
47.0
24.6
7.2
4.2
3.4
3.4
3.4
1.5
1.5
1.1
2.6
100b
   1A list of the source categories that contribute less than 1 percent to total U.S. emissions is provided in
   Appendix B.
   bThis value represents anthropogenic dioxin and furan TEQ air emissions in the U.S. only.
   Source: U.S. EPA1999a

        Sediment core studies have also been used to determine the relative atmospheric contribution of
dioxins and furans. One sediment core study indicates that the relative atmospheric contribution of
dioxins and furans differs by lake based on comparisons of pollutant compositions and accumulation
rates among cores to estimates of atmospheric deposition (Table 11-12). In the Great Lakes region,
accumulation rates of dioxins and furans in sediments began to increase in the early 1940s, Maximum
accumulation rates were observed in 1970 ±10 years, and current accumulation rates are 30 to 70 percent
of the maximum levels (Pearson et al. 1997a). Current accumulation rates of dioxins and furans in
sediments indicate inter- and intra-lake variations.  For example, the current dominant source of dioxins
and furans in Lake Superior is believed to be the atmosphere because sediment accumulation rates of
dioxins and furans are similar to those of lakes in which the atmosphere is the only possible source of
dioxins and furans. In southern Lake Michigan near the Chicago urban area, the atmosphere contributes
most of the dioxins in the lake, but 65 to 95 percent of furans entering southern Lake Michigan are
estimated to be from non-atmospheric sources. In northern Lake Michigan, the analysis of sediment
cores indicates that approximately 50 percent of dioxins and greater than 75 percent of furans are from
non-atmospheric sources. From 65 to 95 percent of dioxins and greater than 95 percent of the furans
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                                                                                  Chapter II
                                                                     Environmental Progress
accumulated in Lake Ontario are estimated to be from non-atmospheric sources based on the analysis of
sediment cores (Pearson et al. 1998).

                                         Table 11-12
      Current Rates of Dioxins and Furans Accumulation in Great Lakes Sediments
Location
Lake Superior
Northern Lake
Michigan
Southern Lake
Michigan near
Chicago Urban
Area
Lake Ontario
Number of
Sediment Cores
Analyzed
2
2
1
3
Accumulation Rates in Sediment
(pg/cm2/yr)
Dioxins a
7.4 - 8.0
44- 49
17
120-220
Furans a
0.8-0.9
22 - 25
17
130-230
Percent Contribution from
Atmospheric Sources
Dioxins a
100
33-55
100
5-35
Furans a
100
5-35
5-35
<5
  ' Includes the total of all dioxin homologs. Includes the total of all furan homologs.
  Source: Pearson et al. 1998

       To help explain and understand the inter- and intra-lake variations in loadings and accumulations
of dioxins and furans, the HYSPLIT/TRANSCO computer program was used to estimate the amount of
dioxin and furan emitted from identified sources to air and water that enter the five Great Lakes (Cohen
et al. 1995).  The model was run using 1993 source and emissions data from 1,329 identified sources in
the U.S. and Canada. As shown in Table 11-13, the modeled deposition flux of dioxins and furans
increases from Lake Superior, Lake Huron, Lake Michigan, Lake Erie, to Lake Ontario, following the
pattern of industrialization around the lakes. In addition, modeled waterborne inputs (i.e., direct
discharges) of dioxins and furans to Lake Superior, Lake Michigan, and Lake Huron play a lesser role
than air deposition. For Lake Michigan, these relative source findings are different from those found by
Pearson et al. (1998) who used a sediment core methodology to estimate relative atmospheric
contributions. In Lake Erie and Lake Ontario, the modeled waterborne inputs are uncertain because of
the difficulty in quantifying discharges to and from inter-lake channels (Cohen et al. 1995).

                                         Table 11-13
            Modeled Air Deposition, Depositional Flux, and Waterborne Inputs
                        of Dioxins and Furans to the Great Lakes
Dioxins and Furans
Atmospheric Deposition (g TEQ/yr)
(range)
Depositional Flux (ug/km2/yr)
Waterborne Inputs (g TEQ/yr)
Percent Contribution from
Atmospheric Sources
Superior
5.6
(2-17)
69
1.4
80
Huron
8.6
(3-25)
145
1.4
86
Michigan
13.7
(5-43)
238
1.9
88
Erie
7.3
(2-21)
284
11
40
Ontario
6.4
(2-18)
337
>3.9
-62
Total
42
(13-124)
172
>19.6
-68
Source: Cohen et al. 1995
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        Biota in many Great Waters are contaminated with dioxins and furans (Firestone et al. 1996,
Metcalfe et al. 1997a, 1997b, Wade et al. 1997b). Recent studies of contamination of biota in the Great
Waters implicate non-atmospheric sources of dioxins (Firestone et al. 1996, Wade et al. 1997b) and
furans (Wade et al. 1997b); however, the relative importance of atmospheric sources and non-
atmospheric sources remains unclear.  In many instances, long-term monitoring indicates that
concentrations of dioxins and furans have declined over time. For example, the U.S. Food and Drug
Administration monitored the presence of dioxin in the edible portions of fish and shellfish from major
U.S. waterways from  1979 to 1994, and the analytical results indicate that levels in aquatic species from
most waterways are declining steadily (Firestone et al. 1996). In several locations (e.g., Chesapeake Bay,
Delaware Bay,  Gulf of Mexico, and Galveston Bay), no dioxin was found in fish samples taken between
1987 and  1994.  In addition, Huestis et al. (1997) reported that levels of dioxins and furans in Lake
Ontario trout collected from 1977 to 1993 have declined substantially, although most chemical levels
appear to have reached a steady state or are declining more slowly now.
Polycyclic Organic Matter

        Polycyclic organic matter (POM2),
like dioxins and furans, is a byproduct of
fossil fuel combustion and natural
combustion processes (e.g., forest fires),
and consists of a group of compounds with
similar chemical structures. The POM
compounds are emitted in distinct patterns
from various source types, allowing the
identification of emission sources from
emission "fingerprints" (or patterns) in
contaminated sediments.  Within this class
of POM are the polycyclic aromatic
hydrocarbons (PAHs).  In most cases,
human-made sources of PAHs account for
the majority of PAHs released to the
environment (Simcik et al. 1996). These
compounds are usually the POMs of
concern as many PAHs are known or
suspected human carcinogens. Therefore,
the discussion of POMs focuses on PAHs.

        There is not one standard
convention to measure and express
emissions and quantities of POM.
Multiple conventions have been developed
because of the differences in the health
effects of the variety of POM and PAH compounds. Some of the measures that are used include 16-PAH
(i.e., the 16 PAH compounds that can be measured using EPA test method 610), 7-PAH (i.e., the seven
PAH compounds that are probable carcinogens), or extractable organic matter (EOM) (i.e., the solvent
                                          HIGHLIGHTS
                                     Polycyclic Organic Matter

                       > Sources. Nationally, the largest source of PAHs
                       is consumer products usage, along with many smaller
                       emission sources. Studies in the Great Lakes region also
                       indicate that vehicular emissions, coal-fired power plants,
                       and coke and steel production are large sources of PAH
                       emissions. Note that multiple conventions are used to
                       report POM and PAH quantities because of the differences
                       in health effects of the variety of POM and PAH
                       compounds.

                       > Loadings.  In general, PAH deposition levels follow the
                       pattern of population density and urbanization. In the Great
                       Lakes region, maximum sediment accumulation levels of
                       PAHs occurred between 1950 and 1975, after which
                       accumulation levels declined. Data from recent years in the
                       region, however, do not indicate a clear trend. In the
                       Chesapeake Bay, data  indicate that total loadings for
                       several PAH compounds decreased in recent years, but
                       data collection methodologies were altered over the same
                       time period, making it difficult to assess the true trend.

                       >• Environmental Concentrations.  Concentrations of
                       PAHs in the sediments  of tributaries and  mainstem of the
                       Chesapeake Bay are below the aquatic biota probable
                       effects level (PEL), but are above the no observed effect
                       level (NOEL) for aquatic biota in the northern bay. In the
                       tributaries, PAH sediment concentrations  declined
                       substantially between 1987 and 1991.
       - The abbreviation, POM, is also used by ecologists, limnologists, and oceanographers for Particulate
Organic Matter.
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 extractable portion of organic matter). These conventions, however, are not necessarily followed by
 independent researchers and thus are not always used in this report.

        Based on EPA's 1990-1993 national inventory of air emissions, the dominant 16-PAH emission
 source is consumer products usage (e.g., metal cleaning, solvents, household cleaning products, and
 personal care products), along with many other smaller emission sources (Table 11-14) (U.S. EPA 1999a).

                                          Table 11-14
                       National Anthropogenic 16-PAH Air Emissions
                   (Based on EPA's 1990-1993 National Toxics Inventory)
Source Category
Consumer products usage
Open burning: wildfires and prescribed burnings
Aerospace industry (surface coating)
Petroleum refining: other sources not distinctly listed
Primary aluminum production (from ESD)
Pulp and paper: kraft recovery furnaces
Coke ovens: charging, topside, & door leaks
Coke ovens: pushing, quenching, and battery stacks
MON - continuous processes
Gasoline distribution stage II
Gasoline distribution stage I
Petroleum refining: catalytic cracking units
Open burning: scrap tires
Industrial Organic chemicals manufacturing
Pulp and paper: lime kilns
Others (< 1 percent each) a
Total U.S. Anthropogenic 16-PAH Air Emissions
Anthropogenic
Air Emissions
(tons/year)
5,733
2,540
1,697
783
662
649
538
517
440
374
355
313
294
227
183
1,967
17,271b
Percent Contribution to
Total U.S. Anthropogenic
Air Emissions
33.2
14.7
9.8
4.5
3.8
3.8
3.1
3.0
2.5
2.2
2.1
1.8
1.7
1.3
1.1
11.4
100"
 A list of the source categories that contribute less than 1 percent to total U.S. emissions is provided in Appendix B.
b This value represents anthropogenic 16-PAH air emissions in the U.S. only.
Source: U.S. EPA1999a

       In the Great Lakes and other waterbodies, several researchers analyzed sediment cores to identify
spatial and temporal trends in PAH deposition and sources, as discussed below. Researchers estimated
relative contaminant contributions from specific local human-made sources (e.g., smelters, coke ovens)
along with regional sources (e.g., fuel oil combustion, wood burning).  In general, recent sediment core
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studies show regional deposition from oil and wood burning sources with significant contributions from
local sources in industrialized areas.

       In Lake Michigan sediments, PAHs originate primarily from vehicular emissions; wood, oil, and
natural gas burning for home heating; coal-fired power plants; and, coke and steel production. A study
by Simcik et al. (1996) that focused on the urban complex of Chicago, Illinois and Gary, Indiana
concluded that the dominant source of PAHs to the entire lake from around 1900 to the present is
emissions from coke and steel production.  This conclusion differs from that of Karls and Christensen
(1998) who found a regional historical pattern in central Lake Michigan, with a significant contribution
from wood-burning and an increasing dominance of oil-burning sources (as opposed to coal-burning by
coke and steel production), which is consistent with U.S. fuel consumption data. Karls and Christensen
also found that PAH loadings at Green Bay, the Fox River, and the Kinnickinnic River were strongly
influenced by local industrial activities, primarily coke production at the Milwaukee Solvay Coke
Company which operated from 1900 to the 1970s.  These differing conclusions support the finding that
local urban sources of PAHs are different and often play a larger role in deposition and sediment
accumulation than regional sources.

       Other studies also indicate that urban sources largely influence PAH deposition. For instance,
recent sediment layers in the Milwaukee Harbor area indicate that in urban areas, highway dust can be a
significant source of PAHs from emissions of gasoline engine exhaust tar (Christensen et al. 1997). In a
carbon particle sediment core study, the relative abundance of oil particles in sediments increased in
recent years and is explained by an increase in automobile traffic  (Karls and Christensen 1998). Sharma
et al. (1997) found that source contributions of PAHs to the St. Mary's River (which connects Lake
Superior and Lake Huron) were strongly influenced by traffic density and urban storm water runoff from
impervious street surfaces.

       These recent findings for PAHs follow the pattern that was  illustrated for several other pollutants
of concern:

•      Local point sources and regional sources both play a role in the deposition of pollutants to
       waterbodies;

•      Urban areas play a strong role whether through the proximity of industrialized areas to
       waterbodies or through urban runoff; and,

•      The relative contribution to pollutant loadings by different types of emission sources shifts over
       time depending on industrial activities, pollution controls, and other factors such as trends in fuel
       use.

       Lake Michigan sediment cores show that PAH accumulation began between 1880-1900,
consistent with increased PAH emissions from coal combustion during industrialization.  Maximum PAH
accumulation occurred between 1950-1975 (Simcik et al. 1996).  Karls and Christensen (1998) found
similar results. Maximum accumulation rates were lower in the southern basin near the Chicago urban
area (70 ng/cm2/yr) than in the northern basin (100-150 ng/cm2/yr) because of the south to north transport
of sediment-bound PAHs. One study observed a slight decrease in PAH sediment accumulation rates in
recent years in some cases due to a switch from coal to oil and natural gas and because of industrial
emissions controls (Simcik et al. 1996).  In contrast, recent deposition monitoring data from the IADN
program do not indicate any clear trend in total atmospheric loadings of PAHs, as indicated by data for
benzo[a]pyrene (B[a]P), to the Great Lakes from 1988 to 1996 (Figure II-7). Trends in PAH deposition
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 levels, in general, are difficult to discern because of (1) the degree of uncertainty in loading calculations
 and (2) the fluctuations in ambient air concentrations (U.S. EPA 19981).

                                           Figure 11-7
                IADN Loading Estimates of B(a)P to the Great Lakes (kg/year)
                                        (U.S. EPA 1998i)
             250
             200
             150
             100
Superior
Michigan
                                                Huron
Erie
                                                                          Ontario
       1988
        1992
                                                       1994
                                   1996
        As part of the Lake Michigan Mass Balance Study (LMMBS) and the Atmospheric Exchange
 Over Lakes and Ocean Surfaces (AEOLOS) study, which examine the influence of urban air emissions
 on deposition to the Great Waters, Franz et al. (1998) found that dry deposition of PAHs to Lake
 Michigan contributes approximately 5,000 kg/year.  Wet deposition estimates from previous studies are
 lower at approximately 1,600 kg/year.  Franz et al. (1998) also found that dry deposition of PAHs is
 higher in Chicago than 15 Ion offshore and at rural sites because of (1) the greater degree of
 anthropogenic activity within the Chicago area, and (2) the greater atmospheric burden and subsequent
 deposition of large particles generated within that area. These findings are consistent with the hypothesis
 that larger particles are generated in urban areas and are deposited closer to the sources than smaller
 particles.

        In the Massachusetts Bay, as in other regions, the sum of wet and dry deposition of PAHs is
 greater at monitoring sites in urban areas (i.e., closer to Boston and Logan Airport) than at monitoring
 sites in rural areas (i.e., Truro), with the exception of biphenyl and naphthalenes (Table 11-15). Biphenyl
 and naphthalenes may be more likely to deposit at the rural site because these pollutants are more water
 soluble and, therefore, may be deposited as wet deposition from clouds carrying biphenyl and
 naphthalenes from other geographic areas. Deposition of PAHs in this region is highest in the winter,
 possibly due to increased use of fossil fuels during winter for residential and commercial heating and
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wood burning in stoves and fireplaces, or due to the lower mixing heights in the atmosphere which occur
during winter in North America (Golomb et al. 1997b).

                                         Table 11-15
      Sum of Wet and Dry Deposition of PAHs onto Massachusetts Bay (ug/m2/year)
PAH
Acenaphthene
Acenaphthylene
Anthracene
Benzo[ghi]perylene
Biphenyl
Chrysenes
Dibenzothiphenes
Fluoranthene
Fluorenes
Naphthalenes
Perylene
Phenanthrenes
Pyrenes
Urban
5.0
5.2
9.5
29.2
4.3
98.8
34.8
129.0
50.0
206.6
11.5
215.1
97.8
Rural
1.8
3.3
3.7
4.1
7.7
9.9
13.2
23.9
23.0
240.0
3.2
41.9
16.9
             Source:  Golomb et al. 1997b

        In the Chesapeake Bay, estimates from one study of total inputs and atmospheric inputs of PAHs
 indicate that direct atmospheric deposition to the tidal waters of the Chesapeake Bay range from 30
 percent to 56 percent (Table 11-16). Estimates of the relative atmospheric contribution for
 benzo[a]anmracene and chrysene may be slightly high because estimates were not provided for point
 sources of benzo[a]anthracene and non-tidal watershed inputs for chrysene. Highest loadings occur in
 the West Chesapeake and Potomac regions. Intermediate loadings occur in the James and Patuxent
 regions, and lowest loadings occur in the Rappahannock, York, and eastern shore regions (Eskin et al.
 1996).  Annual net inputs (in terms of atmospheric deposition processes and the largest source of riverine
 inputs) of nine PAH compounds to the Chesapeake Bay are provided in Table 11-17 based on sampling
 and analysis of surface water and air. In general, gas phase absorption (i.e., absorption of pollutants in
 the gas phase in the atmosphere by the water surface) of PAHs is higher than estimates of wet and dry
 deposition loadings; however, wet and dry deposition become more important loading factors for higher
 molecular weight PAHs (Nelson et al. 1998).

        In contrast, the analysis of CBADS monitoring data in the Chesapeake Bay Program's 1999
 Toxics Loading Release and Inventory (TLRI) provides additional and more recent information on total
 inputs and relative atmospheric deposition inputs of PAHs (including benzo[a]pyrene, chrysene,
 phenanthrene, and pyrene) to the tidal and non-tidal portions of the Chesapeake Bay (see Figure II-6 for
 the delineation of the tidal and non-tidal waters in the Chesapeake Bay watershed). Total inputs to the
 tidal waters of the Chesapeake Bay of benzo[a]pyrene, chrysene, phenanthrene, and pyrene are estimated
 to be 29,000 kg/year, 29,000 kg/year, 59,000 kg/year, and 40,000 kg/year, respectively.  Total
 atmospheric deposition (wet, dry, and gas exchange) ranges from < 0.5 percent (35 kg/year) for
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 benzo[a]pyrene to 5 percent (2,900 kg/year) for phenanthrene.  Inputs of PAHs from the non-tidal
 watershed account for less than 3 percent of the total PAH inputs to the Chesapeake Bay (Chesapeake
 Bay Program 1999a).

                                           Table 11-16
                  Estimates of PAH Inputs to the Chesapeake Bay (kg/year)
PAH
Benzo[a]anthracene
Benzo[a]pyrene
Chrysene
Fluoranthene
Naphthalene
Total Inputs to
Chesapeake
Bay
380
430
570
1,300
1,500
Direct Atmospheric
Deposition to Tidal
Waters
130
130
320
640
NE
Direct Atmospheric
Deposition to Tidal Waters
as Percent of Total Inputs
34
30
56
49
NE
      Nb = no estimate
      Source: Eskin et al. 1996
                                          Table 11-17
                Annual PAH Inputs to and Losses from the Chesapeake Bay
PAH
Fluorene
Phenanthrene
Anthracene
2-Methylphenanthrene
1 -Methylphenanthrene
Fluoranthene
Pyrenes
Benz[a]anthracene
Chrysene
Annual Inputs and Losses (kg/year)
Susquehanna
River3
122
450
NA
NA
NA
1130
1030
376
330
Wet
deposition
16
63
6
NA
NA
70
75
9
29
Dry aerosol
deposition11
12
92
6
NA
NA
120
109
34
85
Net gas deposition
(or volatilization)0
379
2875
130
702
280
679
361
(4.6)
29
   i ne ausquenanna Kiver is tne largest source of freshwater to the Chesapeake Bay.
  b Calculated from measured ambient aerosol particle contaminant concentrations and annual average dry aerosol
   deposition velocity of 0.49 cm/s.
  c Values in parentheses represent net volatilization from rather than net deposition to the waterbody
   Source: Nelson etal. 1998

       In a study to quantify the gaseous exchange fluxes across the air-water interface at rural, semi-
urban, urban, and industrialized sites of the southern Chesapeake Bay, researchers found that aerosol
particle-associated PAH concentrations measured in the atmosphere were similar at the four sites and
PAH gas-phase concentrations measured in the atmosphere were as much as 50 times greater at the urban
site than at the rural site. Furthermore, at the rural site (Haven Beach, VA), PAH gas-phase
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concentrations in the atmosphere are decreasing with time. Specifically, in 1991, the PAH gas-phase
concentration was 6,203 pg/m3 whereas in 1994-1995, PAH gas-phase concentrations were only 4,550
pg/m3. This study also analyzed seasonal variations and did not find any seasonal variations in PAH gas-
phase concentrations at this site. At the non-rural sites, an exponential increase in PAH gas-phase
concentrations was observed with temperature increases, indicating that PAHs volatilize from
contaminated surfaces near these sites in warmer weather (Gustafson and Dickhut 1997).

       In a sediment contamination study of the Chesapeake Bay and its tributaries from 1984 to 1991
by Eskin et al. (1996), PAHs were most concentrated in sediments of the northern bay between Turkey
Point and the mouth of the Middle River, just north of Baltimore. Maximum PAH concentrations in
sediments (14,854 ppm) at all locations in the bay were below the aquatic biota PEL for total PAHs of
28,000 ppm. However, maximum concentrations exceeded the NOEL of 2,900 ppm for aquatic biota
over much of the northern bay north of Annapolis. In the Chesapeake Bay tributaries, PAHs were most
abundant in sediments of the western, northwestern, and northeastern tributaries.  The highest
concentrations were located in the Sassafras River. However, concentrations in sediments in tributaries
declined dramatically between 1987 and 1991. Median PAH sediment concentrations in tributaries
rarely exceeded aquatic biota NOELs and never exceeded aquatic biota PELs. Thus, toxic effects from
PAH sediment contamination are possible in the northern part of the mainstem bay, but are not likely in
the tributaries.

NITROGEN AND  COMPOUNDS

       Nitrogen is an ubiquitous element in the natural environment and is essential to all forms of life.
It is a component of protein and genetic material and plays a key role in photosynthesis. Nitrogen cycles
through all terrestrial and aquatic ecosystems and in many systems is a primary factor determining the
nature, diversity, and productivity of the ecosystems. Diatomic nitrogen gas (N2), an inert, largely
biologically inactive gas, comprises almost 78 percent of the earth's atmosphere. Despite the presence
and essential nature of nitrogen throughout the natural environment, excessive levels of certain nitrogen
compounds in the atmosphere, deposited to surface media or introduced to aquatic systems, can be
detrimental to terrestrial and aquatic habitats and potentially to human health.

       Nitrogen compounds are released to the atmosphere from a variety of sources, both natural and
anthropogenic.  Nitrogen compounds can be present in the atmosphere in a variety of inorganic and
organic forms, in gaseous, liquid, or solid (particulate) states.  Table 11-18 identifies the most common
forms of atmospheric nitrogen and summarizes their key sources and properties. As this table indicates,
the most important forms of atmospheric nitrogen from the standpoint of atmospheric deposition and
loadings to surface waters include the following.

        Nitric Oxide and Nitrogen Dioxide (NO and NOV or collectively NOJ. Nitrogen oxide
        compounds are the key forms of anthropogenic nitrogen released to the atmosphere and are
        precursors to the formation of nitrogen compounds that  are ultimately deposited to the Great
        Waters. Most of the nitrogen emitted to the air from anthropogenic sources is in the form of
        NOXi primarily NO.  Once released to the atmosphere, NOX is transformed through a variety of
        complex photochemical reactions to oxidized nitrogen compounds and, ultimately, aerosol nitrate
        and nitric acid. These end products are deposited to the surface and impact surface waters.
        Nitrogen oxide also is a catalyst in the formation of ozone.
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 •       Nitric acid (HNOJ, Aerosol Nitrate
         (NO3), Ammonia and Ammonium
         (NH3 andNHf, or collectively NHJ,
         and Organic Nitrogen Compounds.
         These are the nitrogen compounds that
         are deposited from the atmosphere to
         surface media and impact surface
         waters. Reduced nitrogen compounds
         (NHX) compounds (e.g., ammonia,
         ammonium) also account for a
         significant portion of nitrogen
         emissions from anthropogenic (as well
         as biogenic) sources.

 Discussions of atmospheric nitrogen emissions,
 deposition, and effects in this report focus on
 these compounds.  In particular, the term
 "atmospheric nitrogen" hereafter refers to these
 compounds and excludes N2, the inert, natural
 component of the earth's atmosphere.

 Nitrogen Emissions and
 Atmospheric Transport

        In the natural environment, diatomic
 nitrogen gas (N2) is converted to biologically
 available forms of nitrogen (e.g., NOX,
 ammonium compounds) through nitrogen
 fixation processes such as lightning and
 biological fixation. Nitrogen emissions from
 lightning have been estimated at less than 10
 million metric tons per year.  Releases of fixed
 nitrogen from marine ecosystems are less
 certain and range from less than  30 to greater
 than 300 million metric tons per  year. Nitrogen                        ~~     ~^~~~^~^~~~~
 fixation in terrestrial ecosystems, prior to human influences, ranged from 90 to 140 million metric tons
 per year; however, these emission levels have increased due to human alterations to the nitrogen cycle
 (Vitousek et al.  1997).

        Of the various forms of nitrogen emitted to the atmosphere through anthropogenic activities, only
 NOX emissions have been quantified adequately to allow evaluation of nationwide emissions trends.
 Nationwide emissions of NOX generally reflect trends in population, economic activity, and
 industrialization for most of this  century. Nitrogen oxide emissions steadily increased in the first three
 decades of the century, but declined in the  1930s due to the lower economic activity during the Great
 Depression. With the start of World War II, NOX emissions nationwide began a rapid upward trend that
 continued well into the 1970s. Between 1940 and 1970, total nationwide NOX emissions increased by a
 factor of three, from 6.5 million to 19 million metric tons per year (U.S. EPA 1997f, U.S. EPA 1997h).
                  HIGHLIGHTS
              Nitrogen Compounds

 >- Sources. Sources of anthropogenic nitrogen
 emissions to air include on-road vehicles, fuel
 combustion for electricity generation, farm animal
 wastes, non-road vehicles and engines, fuel
 combustion by industry, fertilizer application, biomass
 burning, and miscellaneous other minor sources.
 Anthropogenic nitrogen oxide (NOX) emissions rose
 rapidly through the late 1970s. Nitrogen oxide
 emissions have leveled off since around 1980, mainly
 due to controls under the CAA.  Nationwide trends in
 emissions of other compounds cannot be determined
 with available data.

 >- Loadings. The rate of anthropogenic nitrogen
 compound deposition from the air to the Great Waters
 rose through the late 1970s, but has leveled off since
 around 1980. Trends in atmospheric deposition
 nitrogen (ADN)  loading to the Great Waters are
 uncertain, but have probably been static for the past
 two decades. ADN loadings to various Great Waters
 along  the east coast account for roughly 10 percent to
 40 percent of total nitrogen loadings.

 >• Human and Ecological Effects. The effects of
 ADN on the  Great Waters is indistinguishable from the
 effects of nitrogen from other sources. Anthropogenic
 nitrogen loads to the Great Waters are currently many
 times  natural rates. Mechanisms for eliminating or
 assimilating  nitrogen are overwhelmed in many
 waterbodies, leading to nitrogen  buildup. Effects of
 excess nitrogen include algal blooms, eutrophication,
 anoxia, loss  of species diversity,  and fundamental
 changes to ecosystem structure. These effects are
observed with increasing frequency and extent in many
of the Great Waters of the east and Gulf coasts. In
sufficient concentrations, some nitrogen compounds
have toxic effects on humans.  However, nitrogen
compounds generally do not cause exceedances of
drinking water standards in the Great Waters.
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Chapter n
Environmental Progress
                                     Table 11-18
                       Common Forms of Atmospheric Nitrogen
Compound
Notation
Sources
State in the
Atmosphere
Effects
Inert Compounds
Diatomic
nitrogen gas
Nitrous oxide
N2
N20
Comprises approximately
78 percent of the earth's
atmosphere
Wide variety of natural
sources, fertilizer
production and use, fossil
fuel combustion, industrial
acid production, microbial
denitrification in soil and
water
Gaseous
Gaseous
Inert; no direct effects.
Converted to other compounds
through certain biological and
physical processes
Not reactive in lower
atmosphere; potent greenhouse
gas, 320 times as effective as
CO2 in trapping heat in the
atmosphere
Oxidized Compounds
Nitric oxide
Nitrogen dioxide
Aerosol nitrate
Nitric acid
NO
NO2
N03
HN03
Natural soil emissions,
lightning, combustion
processes with
temperatures greater than
2200 °C
Combustion processes with
temperatures greater than
2200 °C, atmospheric
oxidation of NO
Photochemical oxidation of
NOX (i.e., NO and NO2) in
the atmosphere;
combustion processes.
Partitioning of HNO3 to the
aerosol phase by ammonia
gas in the atmosphere;
microbial oxidation of
ammonium in soil and water
Photochemical oxidation of
NOX in the atmosphere.
Gaseous
Gaseous
Fine particles,
dissolved in
precipitation
Vapor, liquid
aerosol,
dissolved in
precipitation
Precursor in the formation of
NO2, nitrates, nitric acid, and
ozone in the atmosphere, and to
NO2, nitrate, and nitric acid
deposition
Highly reactive; a variety of
acute and chronic human health
effects; precursor or catalyst in
the formation of nitrates, nitric
acid, and ozone in the
atmosphere; deposits slowly to
surface media; precursor to
nitrate and nitric acid deposition
Possible mutagen; variety of
adverse health effects
associated with fine particles;
deposits to surface media.
Excess NO3 in drinking water
has adverse health effects,
including methylglobinemia in
infants. Potent nutrient
stimulant of plant growth,
contributing to eutrophication in
waterbodies
Deposits quickly to surface; is
the source of most oxidized
nitrogen deposited to the
surface; causes surface water
acidification, property damage;
detrimental to aquatic biota and
ecological systems. Contributes
to NO3 concentrations and
related health effects in drinking
water. Potent nutrient stimulant
of plant growth, contributing to
eutrophication in waterbodies
 Page 11-42
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                                                                                     Chapter II
                                                                       Environmental Progress
Compound
Other oxides of
nitrogen
Notation
PAN,
N205,
others
Sources
Intermediate reservoir
products in atmospheric
chemical reactions forming
HN03 from NOX
State in the
Atmosphere
Gaseous
Effects
Eye irritant; possible mutagen;
precursor or catalysts in
formation of ozone; PAN is an
important oxidant in the
atmosphere and a component of
photochemical smog
Reduced Compounds (NHJ
Ammonia
Ammonium
NH3
NH4+
Volatilization from animal
wastes; natural microbial
decomposition of organic
matter in oceans and soils;
manufacture and
application of fertilizers;
hydrolysis of urea in
fertilized soils; biomass and
fossil fuel combustion
Formed in the atmosphere
from reaction of NH3with
atmospheric acids such as
H2SO4 and SO4, microbial
transformation of organic
nitrogen, microbial fixation
in soil and water
Gaseous,
vapor,
dissolved in
precipitation
Particulate,
dissolved in
precipitation
Highly reactive; reacts to form
NH4+, establishing an NH4+/NH3
equilibrium in the atmosphere.
Deposits to the surface; potent
nutrient stimulant of plant
growth, contributing to
eutrophication in waterbodies
Can be transported long
distances; ultimately deposits to
the surface; with NH3
contributes as much as 20-40
percent of atmospheric nitrogen
deposition to coastal waters.
Potent nutrient stimulant of plant
growth, contributing to
eutrophication in waterbodies.
Organic Compounds
A wide variety
of compounds
of unknown
composition,
believed to
include urea,
pollen and,
amino acids
Various,
mostly
unknown
Primarily released from
biological processes; also
released from
anthropogenic processes
and formed in the
atmosphere from chemical
and photochemical
reactions of NOX,
hydrocarbons, and O3
Various
Comprises10-30 percent of
atmospheric nitrogen wet
deposition to coastal waters;
contributes to eutrophication in
surface waters
       The 1970 CAA introduced significant regulation of NOX emissions. Various programs and rules
under the CAA regulate specific sources of NOX air emissions (a more detailed discussion of programs
affecting NOX emissions is presented in Chapter III).  Nationwide NOX emissions continued to increase
and reached a peak in 1978, but declined slightly in 1979 and 1980 as more and more CAA NOX
programs began to take effect. Since 1980, the effects of increasing economic activity and the effects of
increasingly comprehensive regulation of NOX  have roughly balanced out, and NOX emissions have been
relatively constant.

       Figure II-8 shows the trend in national NOX emission rates from 1985 to 1996. As this figure
indicates, nationwide NOX emissions have fluctuated around 21 to 23 million metric tons per year
throughout this period.  Nationwide NOX emissions in 1996 were 21.2 million metric tons (U.S.  EPA
1997g). Figure II-9 presents 1996 NOX emissions by State (U.S. EPA 1997f).
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Chapter II
Environmental Progress
       Figure 11-10 presents relative NOX emissions from principal anthropogenic sources in 1996 on a
nationwide basis (U.S. EPA 1997rf). The "all other" category includes miscellaneous minor sources such
as chemical and allied product manufacturing, storage, and transport; metals processing; petroleum and
related industrial processing; solvent utilization; other industrial processes; and, waste disposal and
recycling.

       Reduced nitrogen (ammonium) compounds are also released from anthropogenic sources at rates
approaching those for NOX in some areas. Relative contributions of various anthropogenic nitrogen
sources to atmospheric nitrogen and nitrogen deposition vary from region to region depending on the
predominant economic activities of each region. Both North Carolina and the Chesapeake Bay region,
for example, have relatively high concentrations of animal farming operations, a key source of
ammonium compound emissions. For example, Aneja et al. (1998) determined that anthropogenic
emissions of ammonium compounds account for over 40 percent of anthropogenic nitrogen releases to air
in North Carolina (Figure II-l 1). Similarly, Fisher and Oppenheimer (1991) found that ammonia and
ammonium primarily released from crop and animal farming operations contributes 20 to 40 percent of
total atmospheric deposition nitrogen (ADN) to the Chesapeake Bay. However, additional research is
needed to better quantify ammonia and ammonium emissions to the environment.  The EPA is
collaborating with the U.S. Department of Agriculture (USDA) and academia to develop emission factors
for various practices and to better model transport and deposition.

       A recent monitoring study of wet deposition of nitrogen in the Chesapeake Bay used stable
isotope analysis to identify sources. Results of the study indicate some seasonal trends.  For example, in
the spring, a peak in ammonium was observed as a result of agricultural emissions, including fertilizers,
soil, animal excreta from the southwest and west regions of the bay.  An observed peak in nitrate in the
spring indicates greater soil  emission rates during the spring; however, the dominant source of nitrate in
the region is probably fossil fuel combustion primarily from the northwest and west regions of the bay.
No seasonal trend was observed for dissolved organic nitrogen, but it is likely that it originates from
sources similar to nitrate sources (Russell et al. 1998).

       Once emitted to the atmosphere, nitrogen compounds (particularly NOJ can travel great
distances — 600 to 800 kilometers or farther from the point of emission to the point of deposition (Dennis
1997). The airsheds of the Great Waters for nitrogen compounds (defined as the geographic region from
which atmospheric nitrogen deposited to the Great Waters originates) are, therefore, extensive and
collectively encompass much of the U.S. as well as parts of neighboring countries. Using the Regional
Atmospheric Deposition Model (RADM), Dennis (1997) determined that the NOX airshed for the
Chesapeake Bay watershed encompasses roughly 900,000 square kilometers, including all or part of 15
States and two Canadian provinces, extending into Indiana to the west, South Carolina to the south, and
Quebec to the north.  Using  the same methodology, Dennis recently conducted a more refined analysis
and revised the estimate of the Chesapeake Bay airshed upward to  1,081,600 square kilometers (see
Figure IV-2). Thus, nitrogen emitted to the atmosphere several States away can be deposited to the
watersheds of the Great Waters and to the waterbodies themselves.
Page 11-44
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                                                                                Chapter II
                                                                   Environmental Progress
                                        Figure 11-8
                        National NOX Emission Trends, 1985-1996
                                     (U.S. EPA 1997f)
     27-
     26-
     25-
     24-
     23-
     22-
     21-
     20-
     19-
     18
1
         1985   1986   1987    1988   1989   1990   1991   1992   1993   1994   1995   1996
                                       Figure 11-10
       1996 National Anthropogenic NOX Emissions by Principal Source Category
                                     (U.S. EPA 1997f)
                                                          j| On-Road Vehicles
                                                          ^ Fuel Combustion-Other
                                                          ^\ Non-Road Engines and Vehicles
                                                          gj All Other
                                                          3 Fuel Combustion-Industry
                                                          3 Fuel Combustion-Electric Utility
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
                                                                              Page II-45

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                                                                                     Chapter II
                                                                       Environmental Progress
                                          Figure 11-11
            Estimated Nitrogen Emissions to Air by Principal Source Category
                      in North Carolina - Anthropogenic and Biogenic
                                      (Anejaetal. 1998)
                     0.5%  2.5%
Other Point Sources (NH3)

Fertilizer Application (NH3)
Highway Mobile (NO,)

All Point Sources (NOJ
Area and Non-Road Mobile (NOJ
                                                                             gj Biogenic (NOX)
                                                                             | Swine (NH3)
                                                                             fi Cattle (NH3)
                                                                             13 Poultry (NH3)
       3.0%
Nitrogen Deposition in the U.S.

        Nitrogen compounds are deposited to surface media by dry and wet deposition. Rates and trends
of inorganic nitrogen wet deposition to the Great Waters can be evaluated based on data developed by the
National Atmospheric Deposition Program (NADP) National Trends Network (NADP/NTN), which
monitors wet deposition rates for ammonium (NH4+) and nitrate (NO3) at approximately 200 monitoring
stations across the country. The network provides weekly and annual deposition rates for these two
nitrogen compounds (in terms of kg/ha as the ions) and for total inorganic nitrogen (in terms of kg/ha as
N).3

        The NADP/NTN has monitoring sites within the watersheds of most of the Great Waters,
providing measurements of nitrogen wet deposition to at least portions of the watersheds. Data from
monitoring points nearest the Great Waters can be extrapolated to estimate regional nitrogen wet
deposition to the Great Waters and their watersheds.  While this approach involves increasing uncertainty
with increasing distance between monitoring sites and waterbodies, it nevertheless is currently the best
available approach for evaluating the trends in inorganic nitrogen wet deposition to the Great Waters.

        Figure 11-12 presents rates of inorganic nitrogen wet deposition from the atmosphere as measured
at the NADP monitoring sites nationwide for 1997. Data from individual monitoring points have been
extrapolated in this figure to obtain isopleths for inorganic nitrogen wet deposition rates nationwide
(including the Great Waters). These data indicate that inorganic nitrogen wet deposition ranged from
lows of 0.1 kg/ha/yr in Alaska and 0.2 kg/ha/yr in Oregon to a high of 9.6 kg/ha/yr in upstate New York.
       3 Total inorganic N is calculated based on the sum of ammonium and nitrate nitrogen (Personal
Communication with Van C. Bowersox, NADP Coordinator, 12/9/98).
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                                   Page 11-47

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                                                                                       Chapter II
                                                                         Environmental Progress
        The NADP monitoring data suggest that the rates of inorganic nitrogen wet deposition to many
 of the Great Waters watersheds have been relatively constant for the past two decades. Figures 11-13, II-
 14, and 11-15 present the average rates of nitrogen wet deposition within the watersheds of three of the
 Great Waters, from 1980 through 1997.3 Year-to-year patterns vary among watersheds, but all three
 watersheds exhibit a similar trend - relatively constant rates of nitrogen wet deposition over this period.
 Data from other sources suggest that deposition trends vary locally, however. Deposition of NHX has
 increased since 1980 in areas downwind of intensive livestock operations (Paerl 1999), and annual
 atmospheric deposition of NO3, NIL., and total inorganic nitrogen measured at the NADP site nearest to
 Tampa and Sarasota Bays has increased significantly in the past decade. The increase in nitrogen
 atmospheric deposition near Tampa and Sarasota bays is correlated with increases in population in the
 region over the same time period (Dixon et al.  1996).

        As with all dry deposition processes, nitrogen dry deposition is extremely difficult and expensive
 to monitor directly, and no programs currently do this. The lack of a reliable approach for quantifying
 dry deposition remains a significant gap in the understanding of nitrogen deposition processes and
 effects. Dry deposition can be inferred based on the nitrogen content of atmospheric gases and particles
 and computed deposition rates.  Two networks are using this approach: NOAA's Atmospheric Integrated
 Research Monitoring Network (AIRMoN-dry) and the EPA-sponsored Clean Air Status and Trends
 Network (CASTNet).  However, extrapolation of inferred nitrogen dry deposition values to surrounding
 areas is unreliable (Hicks 1998, Dennis 1999) and is still under investigation. In the absence of measured
 nitrogen dry deposition rates, many investigators have attempted to estimate dry deposition based on a
 ratio of dry deposition to wet deposition. A 1:1 ratio is most commonly derived (Hinga et al.  1991,
 Valiela et al. 1997).  However, this approach also introduces considerable uncertainty, and the 1:1 ratio is
 applicable only for oxidized inorganic nitrogen, not ammonium compounds (Dennis 1999, Chimka et al
 1997).

        Organic nitrogen is also deposited from the atmosphere to the ground and surface waters.
 However, measurement of dry organic nitrogen deposition is unreliable and, to  date, only a limited
 number of measurements of organic nitrogen dry deposition rates have been made (Scudlark et al. 1998).
 Measurement of wet organic nitrogen is more reliable, and more and more data on wet deposition are
 becoming available.  Based on a number of measurements of the organic nitrogen content in precipitation
 on the mid-Atlantic coast, Scudlark et al. (1998) found that organic nitrogen averages  at least 20 percent
 of total dissolved nitrogen in precipitation, and can comprise as much as 64 percent of total dissolved
 nitrogen for single precipitation events. Based on measurements in North Carolina, Peierls and Paerl
 (1997) determined that roughly 30 percent of dissolved nitrogen in  precipitation and rainwater deposition
 was organic nitrogen. Based on these results, it appears that organic nitrogen is a significant component
 of atmospheric deposition nitrogen (ADN) loads to surface waters,  although the current understanding of
 the contribution of organic nitrogen to overall ADN is limited.
        3 NADP data were analyzed by selecting the monitoring sites within the watersheds of the Great Waters
and averaging the reported deposition rates for all monitoring sites within each watershed to obtain an average
deposition rate for the watershed.  Data from 9 monitoring sites were averaged for the Chesapeake Bay watershed;
data from 18 monitoring sites were averaged for the Great Lakes watersheds, and data from 4 monitoring sites were
averaged for the Lake Champlain watershed.
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CHAPTER II
ENVIRONMENTAL PROGRESS
                                       Figure 11-13
               Nitrogen Wet Deposition in the Chesapeake Bay Watershed
                                    (NADP/NTN 1998b)
                                                   • Chesapeake Bay NO3
                                                   U Chesapeake Bay Inorganic N
                                                   D Chesapeake Bay NH4
                 1980
                          1983
                                              1989
                                                        1992
                                                                  1995
                                        Figure 11-14
                 Nitrogen Wet Deposition in the Great Lakes Watersheds
                                    (NADP/NTN 1998b)
              201
                                  • Great Lakes NO3
                                  • Great Lakes Inorganic N
                                  D Great Lakes NH4
                 1980
                          1983
                                     1986
                                               1989
                                                         1992
                                                                    1995
                                        Figure 11-15
                Nitrogen Wet Deposition in the Lake Champlain Watershed
                                    (NADP/NTN 1998b)
                                                        • Lake Champlain NO3
                                                        S Lake Champlain Inorganic N
                                                        D Lake Champlain NH4
                 1980
                                    1986
                                              1989
                                                        1992
                                                                   1995
        Note: Total inorganic N expressed as N; NO3 and NH4* expressed as the ions.
 Page n-50
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                                                                                      Chapter II
                                                                         Environmental Progress
 Atmospheric Nitrogen Loadings to the Great Waters

        The total ADN load delivered to each of the Great Waters is a sum of the nitrogen deposited
 directly to the waters surface, plus a portion of the nitrogen deposited to the watershed. Although only a
 fraction of the atmospheric nitrogen deposited to watersheds ultimately reaches downstream Great
 Waters waterbodies, ADN transfer from watersheds is nevertheless the more important pathway for
 introduction of ADN to these waterbodies. This is due to the much larger areal extent of watersheds
 relative to the surface areas of the receiving waterbodies. The portion of ADN transferred from
 watersheds to downstream waterbodies is still relatively uncertain, and although several ongoing projects
 are attempting to quantify this, the rate of ADN transfer from watersheds to downstream waterbodies
 remains one of the greatest sources of uncertainty in estimating nitrogen and ADN loadings to surface
 waters. Transfer rates appear to vary greatly among watersheds and among areas within watersheds. For
 example, estimates of ADN transfer rates from various watershed areas to  Great Bay Estuary, New
 Hampshire and to Waquoit Bay, Massachusetts are presented in Table 11-19. Table 11-20 presents
 estimated overall ADN transfer estimates for the watersheds of various coastal waterbodies (as developed
 by a number of researchers using a variety of techniques).  The ADN transfer rates in Tables 11-19 and II-
 20 were generally estimated based on estimated steady-state flux of nitrogen.

        The ADN loads to surface waters join nitrogen loadings from a variety of other sources. Key
 sources of nitrogen reaching surface waters via routes other than the atmosphere (i.e., point source
 discharges, runoff, ground water) include (1) fertilizer from agricultural operations, recreation areas,
 suburban lawns; (2) manure from animal production facilities; (3) municipal and industrial treatment
 plant sludge and effluent and residential septic tanks; (4) crop residues (especially nitrogen-fixing crops
 such as legumes); and, (5) industrial wastes.

        Table 11-21 presents a number of estimates of the total nitrogen load, the nitrogen load
 attributable to ADN, and the portion of total nitrogen load represented by ADN for a number of Atlantic
 and Gulf coast Great Waters (developed using a variety of techniques). Based on these data, ADN
 contributes roughly 10 to 40 percent of total nitrogen loads reaching the bays and estuaries studied.  If
 these values are assumed to be representative of the remaining Great Waters in the east and Gulf coast
 region, it is clear that ADN contributes very significantly to the total load of nitrogen reaching the Great
 Waters of these regions. It should be noted, however, that ADN accounts for roughly only 1 percent of
 nitrogen loadings in the Mississippi River basin, which has highly diverse sources of anthropogenic
 nitrogen (Goolsby et al. 1998, as cited by Paerl 1999). The ADN is also likely to be a relatively less
 important contributor to nitrogen loadings in Pacific coast Great Waters than is the case in the east and
 Gulf coast areas, due to the prevailing westerly winds over Pacific coastal waters and their watersheds,
 originating from unpolluted ocean areas.
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Chapter II
Environmental Progress
                                     Table 11-19
                 Transfer of Atmospheric Deposition Nitrogen (ADN)
                            from Various Watershed Areas
Great Bay Estuary, New Hampshire3 || Waquoit Bay, Massachusetts"
Type of Area Receiving
ADN
Urban
Active agriculture
Forest
Surface water in the
watershed
Wetlands
Disturbed/open land
Percent ADN
Transferred to
Estuary
38
10
5
90
3
6
Type of Area Receiving
ADN
Roads, runways,
commercial areas
Agricultural land (other
than turf and cranberry)
Natural vegetation
Ponds in the watershed
Cranberry bogs
Turf
Percent ADN
Transferred to Bay
25
10
9
44
10
10
    'Talbot and Mosher 1998
    bValielaetal. 1997
                                     Table II-20
                  Transfer of Atmospheric Deposition Nitrogen (ADN)
                    from Watersheds to Several Bays and Estuaries
Watershed
Albemarle-Pamlico Sounds
Chesapeake Bay
Delaware Bay
Long Island Sound
Narragansett Bay
New York Bight
Wapuoit Bay
Percent of ADN
Transferred to
Bay/Estuary
15
15
9.4
15
7
12
11
Reference
Paerl and Fogel 1994, as cited in Valigura et al.
1997
Linker 1998
Scudlark and Church, 1993, as cited in Valigura
al. 1997
Long Island Sound Study, as cited in Valigura et
1997
et
al.
Hinga et al. 1991, as cited in Valigura et al. 1997
Hinga et al. 1991, as cited in Valigura et al. 1997
Valielaetal. 1997
 Page H-52
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                                                                                      Chapter II
                                                                        Environmental Progress
                                           Table 11-21
               Atmospheric Nitrogen Loads Relative to Total Nitrogen Loads
                                   in Selected Great Waters*
Waterbody
Albemarle-Pamlico Sounds3
Chesapeake Bayb
Delaware Bay0
Long Island Soundd
Narragansett Bay6
New York Bight6
Total Nitrogen Load
(million kg/yr)
23
170
54
60
5
164
Atmospheric Nitrogen
Load (million kg/yr)
9
36
8
12
0.6
62
Percent Load From
the Atmosphere
38
21
15
20
12
38
Based on ADN loads from the watershed only (excluding direct nitrogen deposition to the bay surface):
Waquoit Bay, MAf
.022
.0065
29
Based on atmospheric N deposition directly to the Waterbody (excluding ADN loads from the watershed):
Delaware inland bays9
Flanders Bay, NYh
Guadalupe Estuary, TX1
Massachusetts Bays'
Narragansett Bayk
Newport River Coastal Waters, NCa
Potomac River MD1
Sarasota Bay, FLra
Tamoa Bav. FLn
1.3
.36
4.2-15.9
22-30
9
.27 - .85
35.5
.6
3 8
.28
.027
.31
1.6-6
.4
.095 - .68
1.9
.16
1 1
21
7
2-8
5-27
4
>35
5
26
28
"As cited in Valigura et al. 1997: aPaerl and Fogel 1994, "Linker 1998, cScudiark and Church 1993, dLong Island
Sound Study 1996,6Hinga et al. 1991, Valiela et al. 1996, Delaware Bays NEP, hPeconic Bay NEP, 'Brock et al.
1995, 'Massachusetts Bays NEP 1996, "Nixon et al. 1995, 'Boynton et al. 1995, ™Sarasota Bay NEP 1995 "Tampa
Bay NEP, Zarbock et al. 1994

Effects of Nitrogen Loadings on the Great Waters

        While ADN contributes significantly to the overall adverse effects associated with excessive
nitrogen loadings to the Great Waters, the effects of atmospherically-derived nitrogen on the Great
Waters is very difficult to distinguish from the effects of nitrogen loadings from other sources. The
effects of atmospheric nitrogen deposition to the Great Waters and associated trends can only be
reviewed in terms of the effects of overall nitrogen loadings to these waters and the associated trends.

        Although historical data for total aquatic nitrogen concentrations in the Great Waters are not
available, nitrate concentrations have been monitored in many rivers and drinking water supplies in the
U.S. for decades.  Nitrate (NO3) concentrations in surface water are directly related to anthropogenic
nitrogen loadings to watersheds and surface waters (Vitousek et al. 1997). Aerosol nitrate is the most
mobile form of nitrogen in watersheds and aquatic systems, and other forms of anthropogenic nitrogen,
notably NHX and organic nitrogen, are partly oxidized to NO3 in the environment (Hessen et al. 1997).
Surface water NO3 concentration trends, although only part of the picture, provide some insight on the
trends in anthropogenic nitrogen loadings and their effects on the Great Waters.

       Available data indicate a significant increasing trend in the fluxes of nitrates in major surface
waters in the U.S., including the Great Waters and their tributaries.
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Chapter n
Environmental Progress
•      Nitrate has more than doubled in the Mississippi River since 1965 (Vitousek et al. 1997). Note,
       however, that ADN accounts for roughly only 1 percent of nitrogen loadings in the Mississippi
       River basin (Goolsby et al. 1998, as cited by Paerl 1999).

•      Nitrate fluxes in 10 major rivers feeding coastal waters in the northeastern U.S. have increased
       by factors of three to eight since 1900 (Jaworski et al. 1997). This increase is correlated with a
       three- to five-fold increase in NOX emissions in the watersheds of these same rivers and more
       than a four-fold increase in atmospheric nitrogen deposition rates to northeastern coastal
       watersheds over the same time period (Vitousek et al. 1997).

•      Increases in surface water nitrogen concentrations of 10 to 25 percent have been observed in
       Long Island Sound, portions of the Potomac River, and the Chesapeake Bay, the Neuse River,
       and portions of Biscayne Bay over the past 2 to 15 years (NOAA 1996, NOAA 1997a, as cited in
       U.S. EPA 1997f).

       The long-term upward trend in nitrogen fluxes and nitrogen concentrations in many surface
waters reflects similar upward trends in atmospheric emissions of nitrogen, in fertilizer use, and in
municipal wastewater discharges in the initial seven decades of this century. Some evidence suggests,
however, that nitrogen fluxes attributable to atmospheric deposition may have leveled off in more recent
years in at least some waterbodies.

•      Based on historical watershed data, Jaworski et al. (1997) found that nitrogen fluxes (total and
       attributable to ADN) for a number of northeastern U.S. coastal waters rose rapidly until about
        1970, but have been more or less constant since then.

•      Stoddard et al.  (1998) found that the nitrate concentrations in higher elevation lakes and streams
       in the northeastern U.S. have either remained relatively constant or shown no discernable trend
       since the early  1980s. Atmospheric deposition nitrogen is the principal and, in some cases, the
       only source of anthropogenic nitrogen loadings to these lakes, which feed tributaries of the Great
       Waters.

       Fluxes of ADN and total nitrogen to some of the Great Waters may, therefore, have leveled off in
recent years.  For many of the Great Waters, however, these fluxes remain many times greater than
natural levels that occurred prior to human activity in the watersheds and airsheds (Vitousek et al. 1997).
Human loadings of nitrogen to the land can overwhelm the capacities of watersheds to assimilate
nitrogen, meaning that  greater and greater percentages of the nitrogen deposited to watersheds are
transferred directly to downstream waterbodies. Thus, constant rates of nitrogen deposition to
watersheds can result in increasing nitrogen loadings to downstream waterbodies. Loadings of nitrogen
to waterbodies can similarly overwhelm the capacity of waterbodies to assimilate or eliminate nitrogen,
leading to a significant buildup of nitrogen concentrations and, in some cases, nitrogen saturation and
related ecosystem degradation (Vitousek et al. 1997, Moffat 1998). These factors are believed to
contribute to significant increases in concentrations of nitrogen in some of the Great Waters and rivers
feeding the Great Waters, specifically the Mississippi River and a number of major rivers in the
northeastern U.S. (Vitousek et al. 1997).

        The "natural" or  ecologically ideal concentration of nitrogen in the water column varies
considerably among waterbodies. As one example, the Chesapeake Bay Program (1992, as cited in U.S.
EPA 1998b) has determined that the most desirable concentration of dissolved inorganic nitrogen in the
Chesapeake Bay (i.e., the concentration necessary to promote continued survival of submerged aquatic
vegetation) is <0.15 mg/L.
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        Recent NOAA Estuarine Eutrophication Surveys (NOAA 1996, 1997a, b, c, as summarized in
 U.S. EPA 1998t) indicate elevated nitrogen concentrations in many of the Great Waters coastal estuaries
 on the Atlantic and Gulf coasts. These surveys found the following:

        High aquatic nitrogen concentrations (> 1 mg/L) in two of 18 estuaries on the U.S. north Atlantic
        coast, 14 of 22 mid-Atlantic estuaries, 11 of 21 south Atlantic estuaries, and 18 of 37 Gulf of
        Mexico estuaries; and,

        Moderate to moderately elevated aquatic nitrogen concentrations (0.1 - 0.9 mg/L) in 13 of 18
        north Atlantic estuaries, five of 22 mid-Atlantic estuaries, seven of 21 south Atlantic estuaries,
        and 19 of 37 Gulf of Mexico estuaries.

        Excess  nitrogen loadings in the Great Waters can have a range of effects on the ecological
 structure and processes of these waters and, ultimately, on human use of the waters.  Effects of excess
 nitrogen loadings can be considered in three broad categories (U.S. EPA 1997a).

 1.      Dramatic increases in plant productivity and algal blooms in systems where algal growth was
        previously nitrogen-limited. This can in turn cause fish kills, loss of submerged aquatic
        vegetation due to reduced sunlight penetration, loss of recreational use of waterbodies, and
        ultimately hypoxic  (low oxygen) or anoxic (no  oxygen) conditions as algal blooms die and
        decomposition processes consume the available oxygen - a condition referred to as
        eutrophication.  Hypoxic and anoxic conditions can lead to loss of aquatic biodiversity as species
        requiring higher oxygen concentrations are lost, can affect the biogeochemical cycling of
        nutrients and toxic compounds, and can affect the bioavailability of toxic compounds.  In
        addition to these consequences associated with normal algal blooms, excess nitrogen loadings are
        also linked to harmful or toxic algal blooms, often referred to as red or brown tides, involving
        algae species that are toxic to other aquatic biota or humans, often causing fish kills and human
        illness or mortality  (Paerl et al. 1999, 1998, Paerl 1997a, Pelley 1998, Tibbets 1998, Rabalais et
        al. 1996).

        Changes in the ecological balance brought on by fundamental changes at the base of the food
        web (i.e., the loss of aquatic grasses and other vegetation and the dominance of a relatively few
        algal species) and loss of biological diversity throughout the system as fundamental aquatic
        ecological parameters such as oxygen level, sunlight penetration, diversity and abundance of
        food species, and habitat availability change.

        Direct toxicity of some nitrogen compounds to aquatic organisms. Toxicity of nitrogen
        compounds to aquatic organisms is not well understood, but mounting evidence suggests that
        these compounds can affect the ability of some  species to adapt to other stresses (Linton et al.
        1998).  Dissolved ammonia at concentrations above 0.2 mg/L can be toxic to aquatic organisms
        (Paerl 1997a, as cited by U.S. EPA 1997a).

        Many of these adverse effects have been observed by researchers in the Great Waters. Examples
are provided below.

        McClelland and Valiela (1998) and Short and Burdick (1996) found that increased loads of
        anthropogenic nitrogen to Waquoit Bay, Massachusetts have a significant effect on the pathways
        by which nitrogen enters the food web.  The diets of primary consumers in the bay are influenced
        by the dominant forms of food material available. Eelgrass is an important dietary component of
        primary consumers in areas of the bay receiving lower anthropogenic nitrogen loadings.
2.
3.
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       Laboratory studies by Short and Burdick (1996) indicated that excessive nitrogen loadings
       stimulated growth of algal competitors that shade and stress eelgrass.  These laboratory results
       were borne out in field observations in Waquoit Bay, where domination by algal competitors was
       observed in areas of significant eelgrass decline. McClelland and Valiela (1998) found that
       eelgrass is lost and is largely replaced by algae in areas of the bay receiving higher anthropogenic
       nitrogen loadings. Thus, an important pathway for nitrogen entry to the food web may be
       altered. McClelland and Valiela conclude that this change in the nitrogen pathway probably
       affects the rate and manner in which nitrogen is cycled within the bay ecosystem and may reduce
       the stability of shallow estuarine ecosystems in the bay.  Loss of eelgrass also results in loss of
       habitat for shellfish and other small fish, further affecting the ecological structure and function of
       the bay.

•      Allen and Hershey (1996) demonstrated that the immediate effects of atmospheric deposition of
       nitrogen can vary seasonally for some waterbodies. In a north shore river tributary to Lake
       Superior, availability of nitrogen was found to alternate with availability of phosphorus and other
       factors as the limiting factor controlling algal biomass growth.  Introduction of additional
       nitrogen resulted hi increased algal biomass during early summer and late summer, but not
       during other seasons.  Introduction of additional phosphorus caused increased algal growth in
       spring, but not hi other seasons. Algal growth was not affected by additional nitrogen or
       additional phosphorus during the fall season, suggesting limitation by factors other than nitrogen
       or phosphorus availability. The dissolved inorganic nitrogen to soluble reactive phosphorus
       (DIN/SRP) ratio was not a reliable predictor of nutrient limitation in the studied river.

•      Linton et al. (1998) found that the combination of global warming and increased ammonia
       loadings from atmospheric and other sources could have a greater impact on aquatic species in
       Lake Superior than either factor alone.  These researchers studied rainbow trout reactions to
       elevated aquatic ammonia concentrations in conditions simulating Lake Ontario under a global
       wanning scenario (2 °C above natural water fluctuating water temperature cycle). Their results
       indicate that elevated ammonia concentrations could reduce the ability of rainbow trout to adapt
       to long-term, small temperature increases such as could be caused by global warming.

•      The disappearance of the economically important scallop from Tampa Bay waters is attributed to
       algal blooms and associated changes in ecological conditions in the bay, which in turn is
       attributed to excess nitrogen loadings (U.S. EPA 1997a).

•      Hypoxia attributed to nitrogen-induced eutrophication is now a common and recurring condition
        hi many bays along the Atlantic and Gulf coasts, notably Long Island Sound, New York-New
       Jersey Harbor, Chesapeake Bay, Albemarle-Pamlico Sound, and the Mississippi Delta region
        (U.S. EPA 1997a).

•      Major algal blooms attributed to increases in aquatic nitrogen concentrations have occurred in
        several Atlantic and Gulf coast waters in recent years.  These blooms have been accompanied by
        deleterious visual and odor effects and fish kills (U.S. EPA 1997a).

        The number of U.S. coastal areas experiencing major, recurring harmful or toxic algal blooms,
        linked to increases in aquatic nitrogen availability, have doubled since 1972 and  include areas
        on the Atlantic, Gulf of Mexico, and Pacific coasts (Pelley 1998, Tibbetts 1998).

        The NOAA Estuarine Eutrophication Surveys (NOAA 1996, 1997a, b, c, as summarized in U.S.
EPA 1998t) indicate that the adverse effects of excess nitrogen concentrations are currently evident to
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 greater or lesser degrees in approximately 89 percent of the U.S. coastal estuary Great Waters.  These
 surveys report the following:

 •      Anoxic or hypoxic conditions (oxygen content 0-2 mg/L) in portions of four of 18 north
        Atlantic estuaries, 13 of 22 mid-Atlantic estuaries, 13 of 21 south Atlantic estuaries, and 26 of 37
        Gulf of Mexico estuaries; and,

 •      Biologically stressful levels of oxygen (2 - 5 mg/L) in at least portions of nine of 18 north
        Atlantic estuaries, 21 of 22 mid-Atlantic estuaries, seven of 21 south Atlantic estuaries, and 35 of
        37 Gulf of Mexico estuaries.

 Human Health Effects of Nitrogen in  the  Great  Waters

        Under the Safe Drinking Water Act, EPA set maximum contaminant levels (MCLs) for nitrate
 and nitrite in drinking water to protect human health.  These levels are established at 10 mg/L of nitrate
 and 1 mg/L of nitrite. The primary adverse human health  effect associated with exposure to nitrate or
 nitrite is methemoglobinemia, a dangerous condition in which nitrite in the blood stream prevents oxygen
 transport, potentially leading to brain damage or death.  This condition is rare in adults, but is a
 significant danger for infants because microbes present in  the stomachs of infants can convert large
 amounts of nitrate to nitrite.  The National Research Council concluded, in 1995, that results from
 epidemiological studies are inadequate to support an association between nitrate or nitrite exposure from
 drinking water in the U.S. and increased cancer rates in humans.  However, an epidemiological study led
 by a researcher from the National Research Council, published in 1996, of rural populations using
 community water supplies in Nebraska concluded that long-term exposure to elevated nitrate levels in
 drinking water may contribute to the risk for non-Hodgkin's Lymphoma. Research is continuing in this
 area (U.S. EPA 1997h, Ward et al. 1996).

        Data indicate that most of the Great Lakes nearshore waters can be used as a source of drinking
 water with normal treatment, meeting the nitrate and nitrite levels (U.S. EPA 1998n). Similarly, Lake
 Champlain was not associated with any violations of standards in place for drinking  water supplies due to
 Great Waters pollutants of concern from 1986 to 1995 (Lake Champlain Basin Program 1999).  Further
 reductions in pollutant concentrations may reduce the cost of drinking water treatment in some areas.

        Excess nutrients in coastal waters have also been implicated in the increased incidence of
 harmful or toxic algal blooms in the coastal waters of nearly every U.S. coastal State. These blooms
 have been linked to health effects among exposed human populations ranging from shortness of breath to
 dizziness, diarrhea, disorientation, permanent memory loss, and occasion death (Pelley 1998, Tibbetts
 1998). To the extent that ADN contributes to elevated nitrogen content in coastal waters, ADN also
 contributes to human health risks associated with harmful and toxic algal blooms.  No evidence exists to
 date suggesting negative human health effects attributable  directly to atmospherically-derived nitrogen in
 the Great Waters.
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BANNED AND RESTRICTED USE SUBSTANCES
Polychlorinated Biphenyh
(PCBs)

       Manufacture of PCBs in the U.S. was
voluntarily stopped in the late 1970s, and the
use of PCBs was restricted under the Toxic
Substances Control Act (TSCA) in 1979.
Therefore, sources of PCBs in the U.S. are
limited. However, PCBs are still present in
older commercial and industrial equipment
(e.g., electrical transformers and capacitors)
and are released from non-point and non-
regulated sources including Superfund sites.
In addition, despite reductions in use, PCBs
are released during some combustion
processes, such as the incomplete burning of
PCB-containing wastes during incineration.
New research is also indicating that PCBs are
actually being formed during certain
combustion processes, similar to the way in
which dioxins and furans are  formed (Lemieux
etal. 1999).

       The number and magnitude of sources
of PCBs have decreased 20-fold in the last 20
years, and sources of PCBs generally are
limited to atmospheric deposition and
localized point source discharges (Froese et al.
1997). Some studies detected PCBs  in
smallmouth bass from Fumee Lake, a remote lake in Michigan (Henry et al. 1998), and in the blubber of
Beluga whales from Alaska's north coast (Wade et al. 1997a), indicating long range transport and
atmospheric deposition as a major source in these areas. Many recent studies in the Great Waters,
however, implicate non-atmospheric sources of PCBs (e.g., Brazner and DeVita 1998, Metcalfe et al.
1997a). The relative importance of atmospheric inputs and non-atmospheric sources remains unclear.
Nevertheless, the largest stationary source of PCB air emissions on a national basis, as indicated by
EPA's 1990-1993 NTI, is hazardous waste incineration at dedicated hazardous waste incinerators, along
with several other smaller sources (Table 11-22) (U.S. EPA  1999a). The EPA is pursuing additional
research to determine the extent of PCB releases during incomplete combustion in these and other
facilities as well as the effects on emissions and loadings of PCBs.

        In Lake Superior, specifically, approximately 52 kg/year of PCBs are from point source inputs,
15 kg/year are from runoff (including pollutants in rainfall plus pollutants that are transported from land
areas), and 85-156 kg/year are from wet and dry deposition (Hoff et al. 1996).  Similarly, water samples
collected during an investigation of the source of PCBs in the Detroit River (which feeds Lake Erie)
indicate that the dominant sources of PCBs in this location are surface runoff from urban areas during
rainfall and resuspension of in-place deposits of PCBs in the sediments of the river and bays due to high
flow events in the rivers and due to severe wind conditions  in the lakes (Froese et al. 1997).
                                           HIGHLIGHTS
                                     Polychlorinated Biphenyls

                         > Sources. In general, the number and magnitude of
                         PCB sources have decreased 20-fold in the past 20
                         years. PCB sources generally are limited to atmospheric
                         deposition and localized stationary sources. The largest
                         national-level stationary air emission source of PCBs  is
                         hazardous waste incineration, along with several smaller
                         sources.  Sources to surface waters include atmospheric
                         deposition, urban runoff, resuspension of contaminated
                         sediments, and recycling through volatilization followed
                         by deposition.

                         > Loadings. In the Great Lakes, studies show that
                         deposition of PCBs has decreased and that PCBs in
                         surface waters may be in equilibrium with the
                         atmosphere (i.e., no net loadings). Deposition rates are
                         higher near the Chicago urban area when compared to
                         offshore and rural locations.  In the Chesapeake Bay, a
                         net loss of PCBs from the water surface has been
                         observed.

                         > Environmental Concentrations and Exposure.
                         PCB contamination levels in biota from the Great Lakes
                         have declined; however, certain human subpopulations
                         continue to be exposed to PCBs through fish
                         consumption.  In the Chesapeake Bay, maximum PCB
                         sediment concentrations are below the PEL and NOEL
                         for aquatic biota, with the exception of one location on
                         the James River.
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                                          Table 11-22
                         National Anthropogenic PCB Air Emissions
                   (Based on EPA's 1990-1993 National Toxics Inventory)
Source Category
Hazardous waste incineration
Sewage sludge incineration
Fabricated metal products, nee
Industrial boilers: natural gas combustion
Portland cement manufacture: all fuels
Scrap and waste materials
Scrap tire combustion
Refuse systems
Fabricated rubber products, nee
Others (< 1 percent)3
Total U.S. Anthropogenic PCB Air Emissions
Anthropogenic
Air Emissions
(tons/year)
0.03
0.005
0.005
0.004
0.004
0.001
0.001
0.0006
0.0005
0.0008
0.052b
Percent Contribution to
Total U.S. Anthropogenic
Air Emissions
56.0
10.3
10.1
7.7
7.3
2.7
2.1
1.2
1.0
1.7
100b
        Appendix B.
        bThis value represents anthropogenic PCB air emissions in the U.S. only.
        Source: U.S. EPA1999a

        Research based on deposition monitoring under the Atmospheric Exchange Over Lakes and
 Ocean Surfaces (AEOLOS) project found that the "urban plume" of Chicago increases the deposition of
 PCBs to Lake Michigan and is a major source of atmospheric PCBs to coastal Lake Michigan. Total
 ambient air PCB concentrations on the lakeshore near Chicago are two to three times higher than
 background levels and the values collected under IADN, which monitors remote locations on the Great
 Lakes (Offenberg and Baker 1997).  Franz et al. (1998) found similar results using dry deposition
 monitoring data from AEOLOS and the Lake Michigan Mass Balance Study where fluxes of particulate
 PCBs were higher in Chicago than less than  15 km offshore and at rural sites.  The higher urban fluxes
 are due to increased anthropogenic activity and the greater atmospheric burden of large particles that are
 generated in the urban area and deposited closer to their sources. Franz  et al. (1998) estimated dry
 deposition of PCBs to Lake Michigan to be approximately 1,100 kg/year, which is at least an order of
 magnitude greater than some previously reported values. Other studies report inputs of PCBs through
 air/water exchange at approximately 880 kg/year and wet deposition at 50 - 250 kg/year (Franz et al.
 1998). In contrast, Offenberg and Baker (1997) found that the amount of yearly wet deposition plays a
 major role in determining the annual deposition of PCBs to Lake Michigan, and IADN monitoring results
 indicate that gas absorption is a dominant deposition process for delivering PCBs to lake surfaces
 (U.S./Canada IADN Scientific Steering Committee 1998). The observed differences from these studies
 illustrate the importance of considering local meteorology and the location of monitoring stations (rural
 versus urban) when interpreting deposition data.

        In addition to depositing PCBs released to the atmosphere from emission sources, atmospheric
 deposition processes play a strong role in PCB recycling in Lakes Superior, Michigan, and Huron, but
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less of a role in Lakes Erie and Ontario. Volatilization of PCBs from the water, however, is the dominant
mechanism for exchange of PCBs between the lakes and the atmosphere.  According to IADN
monitoring data from 1988 to 1996, wet and dry deposition of PCBs to each of the Great Lakes decreased
(Hoff et al. 1996) (Table 11-23). In the Detroit River, which is a heavily industrialized and urbanized area
and is a primary transport route of PCBs to Lake Erie and Lake Ontario, the mass of PCBs transported
through the Trenton Channel to the western basin of Lake Erie in 1995 was estimated at 600 kg/yr,
constituting a potential decrease from 1986 estimates of approximately 1,500 kg/year. (Note, however,
that different sampling methodologies were employed in the different years and may be responsible for a
portion of the change (Froese et al. 1997)).  Other monitoring studies show a net loss of PCBs to the
atmosphere, particularly from Lake Superior and Lake Michigan (Offenberg and Baker 1997, U.S. EPA
1998m). For example, PCBs are being purged from Lake Superior at 21 percent per year of its annual
burden (Hoff et al. 1996).  Another monitoring data analysis indicates that gas transfer of PCBs out of the
lakes is counteracted by net deposition, meaning PCBs are in equilibrium with the water surface and the
atmosphere (Hillery et al. 1997).

                                         Table  11-23
       IADN Loading Estimates of PCBs (wet and  dry) for the Great Lakes (kg/year)
Year
1988
1992
1994
1996
Superior
550
160
85
50
Michigan
400
110
69
42
Huron
400
110
180
N/A
Erie
180
53
37
34
Ontario
140
42
64
N/A
           Source: U.S. EPA 19981

         Studies using surface water and air sampling indicate that Chesapeake Bay waters have higher
relative concentrations than the overlying atmosphere, and volatilization is the dominant loss process for
PCBs from the bay. Polychlorinated biphenyls are volatilizing to the atmosphere at an average rate of 35
ug/m2/yr, with a range of 31 to 112 ug/m2/yr. Annual loss of PCBs from the bay from net volatilization
(403 kg/yr) is 10 tunes greater than inputs from wet and dry deposition of 37 kg/yr and is more than two
times greater than the loadings from the Susquehanna River of 165 kg/yr (Nelson et al. 1998). The
Chesapeake Bay Program's 1999 Toxics Loading and Release Inventory (TLRI) provides information on
the total inputs and relative atmospheric inputs of PCBs to the tidal and non-tidal waters of the
Chesapeake Bay based on monitoring data. Total PCB inputs to the Chesapeake Bay, without point
source estimates, are similar for both inputs from the non-tidal watershed (254 kg/year) and inputs from
wet and dry atmospheric deposition to the tidal waters (245 kg/year) (Chesapeake Bay Program 1999a).

        The comparison of current contamination levels to historical values provides evidence that
concentrations of PCBs in biota have declined in the Great Lakes. For example, Dykstra et al. (1998)
measured PCB concentrations in nestling blood (1989-1994) and addled eggs (1986-1993) of bald eagles
in Lake Superior and inland Wisconsin sites. A comparison to published and unpublished historical data
of PCBs in addled bald eagle eggs on Lake Superior indicates that PCB levels declined significantly
between 1969 and 1993; however, PCBs may still be at levels high enough to affect reproductive success.
Similarly, Ion et al. (1997) measured the concentration of PCBs in yellow perch from the St. Lawrence
River between 1975 and 1991-1992. Comparison of average PCB concentrations detected to historical
levels in St. Lawrence River fish indicates that levels have decreased by a factor of 30 since  1975.  The
concentration of PCBs in all fish sampled by Ion et al. (1997) were below the International Joint
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 Commission guideline of 100 ng/g in whole fish, which is protective of aquatic life and consumers of
 fish.

        A study by Eby et al. (1997) shed doubt on findings reported in the Second Great Waters Report
 to Congress that concluded that PCB concentrations in Great Lakes have leveled off or even increased
 slightly in the last 10 years (U.S. EPA 1997b). In those earlier studies, scientists hypothesized that the
 trend in PCB contamination could be due to changes in the composition of the food web.  Eby et al.
 (1997) demonstrate, however, that sampling methodology may have influenced the apparent PCB
 concentration trends rather than changes in fish diet. As part of a long-term PCB monitoring survey, the
 USGS collects and analyzes bloaters (Coregonus hoyi) from the same site in Lake Michigan every year.
 Because fish size is used to predict fish age, similar size fish are collected each year.  However, since the
 early 1980s, bloater populations experienced a decline in growth rate due to a shift in diet, which placed
 older, more contaminated bloaters in the size range sampled. This resulted in an apparent trend of steady
 state or increasing PCB levels. In contrast, Eby et al. (1997) modeled an increase in the amount of the
 most contaminated prey in the bloater diet and found that this shift in diet had little effect on PCB
 contamination levels in bloaters.

        A recent study by Haffner et al. (1997) found that total PCB concentrations in herring gull eggs
 decreased significantly between 1981 and 1992 in Lake Ontario and Lake Erie, although the decrease in
 lake Erie was not of the same magnitude. The PCB concentrations detected during this study are not
 expected to affect reproduction in herring gull populations. In addition, Haffner et al. (1997) found that
 total PCB concentrations in double-crested cormorant eggs did not decrease in Lake  Ontario but
 decreased slightly in Lake Erie between 1981  and 1992. The PCB concentrations detected in this study
 may be high enough to cause toxicological stress on the cormorant population (e.g., egg mortality,
 infertility, deformity).

        Although some studies indicate that PCB levels in fish have decreased or reached a steady state
 in recent years, consumption of contaminated  fish from the Great Lakes remains a concern.  Several
 recent studies examined the relationship between increased health risks in certain subpopulations and the
 consumption offish from the Great Lakes contaminated with PCBs, concluding that certain
 subpopulations continue to be exposed to PCBs through fish consumption despite declines in
 contamination levels and despite continued fish consumption advisories. Study results include the
 following.

        Pellettieri et al. (1996) determined that the estimated PCB intake for sport fisherman in the
        Chicago area exceeded the level recommended by the Great Lakes Advisory Task Force of no
        more than one meal offish per week (assuming the average meal offish is composed of 227 g of
        uncooked fish and that the intake of PCBs is reduced by half due to skinning, trimming, and
        cooking).

 •       A study of Ojibwa tribal members from the Great Lakes region indicated that PCB
        concentrations in Ojibwa populations were low with a maximum value of 9.6 ppb in blood
        serum; however, a significant association was found between serum PCB concentration and age
        (Gerstenberger et  al. 1997). This is important because PCBs are persistent and bioaccumulate in
        the food chain.

        According to a 1997 survey (Tilden et al.  1997) of Great Lakes States' residents, the most widely
        accepted fish consumption advisory recommendation was cleaning and cooking methods. A
        study of six cooking methods determined that choice of cooking method greatly impacted the
        loss of PCBs during the cooking process, with smoking and microwave baking as the most
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        effective methods.  Smoking reduced PCB levels by 65 percent, and microwave baking reduced
        PCB levels by 60 percent (Salama et al. 1998).

        In a sediment contamination study of the Chesapeake Bay and its tributaries from 1984 to 1991
by Eskin et al. (1996) under the Chesapeake Bay Program, PCBs were detected at low levels in sediments
throughout the bay and its tributaries, indicating that aquatic life impacts (based on the aquatic biota
NOEL and PEL) from PCBs in the bay are not widespread. The highest concentrations were detected in
sediments in the northern bay near the Baltimore area and on the James River. Maximum PCB
concentrations were below aquatic biota NOEL and PEL concentrations in sediments at all locations,
with the exception of one location on the James River.

        Despite  observed declines in some organisms, a study of PCB levels (as serum concentrations) in
male and female juvenile American  alligators  in Lake Apopka, Florida indicated that 23 of 28 PCB
congeners were present in juvenile alligators.  The mean total PCB concentration in the serum was 1.54 ±
0.12 (SE) ng/mL.  Alligators in Lake Apopka have been reported to have a number reproductive and
endocrine system abnormalities which may be due to embryonic exposure to these and other compounds
(Guillette et al. 1999).
Pesticides

        Table 1-1 presents the uses and sources
of Great Waters pesticides and indicates that
many of these pesticides are banned or use
restricted; however, many of these pesticides
may still be used in other countries. Therefore,
long-range transport of emissions from other
countries may contribute to current levels in
Great Waters along with other current sources,
such as use of existing stocks of pesticides, and
releases from contaminated sites (e.g.,
Superfund sites) and from soils upon which
pesticides were applied in the past. Because
most of these pesticides are persistent  and
bioaccumulative, pesticides that were used or
unintentionally released previously can cycle
between environmental compartments (e.g., air,
water, soil, sediment,  biota). Therefore, some of
these pesticides can be re-released to the
atmosphere, transported short or long distances,
and redeposited to surface waters.

        Given these possible sources of banned and restricted use pesticides, efforts to reduce releases
focus primarily on promoting (1) international agreements to reduce or eliminate the manufacture and use
of these pesticides, and (2) pesticide collection programs (i.e., Clean Sweeps as described on page III-
56). Additional future reductions may result from the clean up of existing stockpiles and contaminated
sites. Research continues at EPA and  other institutions on soil remediation methods that will reduce
emissions of these pollutants from contaminated sites.  In addition, efforts to limit the exposure of human
and ecological populations to these pesticides include EPA and other agency monitoring programs and
continued outreach activities to make the public aware of contaminated fish and waterbodies. Some
                                            HIGHLIGHTS
                                              Pesticides

                            >- Sources.  Because most of the Great Waters
                            pesticides of concern are banned or restricted use
                            substances, the major sources include long range
                            transport from other countries, use of existing
                            pesticide stocks, and releases from contaminated
                            sites and soils.

                            >• Loadings. Since many of these pesticides are
                            persistent and bioaccumulative, they are cycling
                            between environmental compartments. In general,
                            deposition of these substances remained constant or
                            declined in recent years.

                            >• Environmental Concentrations.  DDT and its
                            metabolites have, in general,  declined to levels below
                            which adverse environmental effects of concern are
                            expected.  In  Chesapeake Bay sediments,  chlordane
                            and dieldrin concentrations were between the level
                            expected to show widespread effects and the level
                            expected to show limited effects.
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recent studies of these pesticides focus on the role of atmospheric transport, both historic and current, in
the contamination of waterbodies and biota of the Great Waters.

        Atmospheric transport and deposition of these pesticides remains a principal source in the Great
Waters, as shown by studies of both regional and global transport.  For most pesticides, however, the
relative contribution of atmospheric deposition versus other sources (e.g., runoff from contaminated
soils, groundwater contamination) to total loadings is not yet known. It is expected that with the
development of mass balance models and better sources and emissions estimates, it will be possible to
determine relative contributions of different sources of pesticides and other pollutants to the Great
Waters waterbodies. Furthermore, the contamination of biota in remote waterbodies that receive no point
source inputs emphasizes the role of atmospheric transport and deposition of pesticides. For example,
DDT/DDE, toxaphene, chlordane, dieldrin, and hexachlorobenzene were detected in smallmouth bass
from Fumee Lake, which is in the Upper Peninsula of Michigan. The remote location of Fumee Lake
suggests atmospheric loading is the source of pesticide contamination. Concentrations of these pesticides
(except toxaphene which is associated with elevated levels in Lake Superior because of point source
inputs) were similar to those found in fish from Lake Superior, where atmospheric inputs are thought to
be the primary source of contaminants. All pesticide concentrations were less than those reported in
Lake Michigan, which typically receives contaminants by direct input from point sources as well as
atmospheric deposition (Henry et al.  1998). The detection of toxaphene, DDT/DDE, and chlordane in
the blubber of Beluga whales from Alaska's north coast (Wade et al. 1997a) demonstrates the global
scale of atmospheric transport. Toxaphene, chlordane, lindane, a-HCH, hexachlorobenzene, dieldrin,
and DDE also were detected in a variety of organisms at multiple trophic levels in Lake Superior
(Kucklick and Baker 1998).

        Banning and restricting uses of these pesticides under the Federal Insecticide, Fungicide, and
Rodenticide Act (FIFRA) in the past 25 years have proven to be the most effective methods of removing
these compounds from the  environment, as would be expected.  Because these substances are no longer
intentionally released in the U.S. and the goal was to remove them from the environment, a group of
researchers investigated how long these pesticides would persist in the atmosphere above the Great
Lakes. Cortes et al.  (1998) calculated atmospheric half-lives (i.e., the amount of time required for the
concentration in the  air to decrease by 50 percent) and used measured atmospheric concentrations to
estimate minimum virtual elimination dates (i.e., when the contaminant levels are below the detection
limits of the measurement equipment) in the Great Lakes regional atmosphere for DDT, DDE, dieldrin,
chlordane, lindane (y-HCH), and hexachlorobenzene (HCB) (Figure 11-16). Based on these dates, DDT
and DDE will be the first compounds to be reduced to concentrations below current detection limits in
the Great Lakes atmosphere, followed by dieldrin and chlordane between 2010 and 2030, y-HCH by
2030, and HCB by 2060. These estimates assume current rates of long-range transport of these pollutants
into the region. Because of their persistence, it should be noted that elimination of these pollutants in the
atmosphere does not mean that concentrations would be eliminated in deposited media by these dates.
However,  these estimates indicate that reduction strategies in the Great Lakes, along with the original
bans or restrictions on the use of these substances, are having the intended effect.

        DDT/DDD/DDE.  In general, several studies indicate declines in atmospheric deposition of DDT
and its metabolites as well as declines in concentrations in different environmental media. According to
deposition monitoring data collected under IADN, wet and dry deposition of DDT to Lakes Superior,
Michigan, and Erie in 1996 was less than values from 1994, 1992, and 1988 (Table 11-24) (U.S. EPA
19981).  The IADN data from 1993-1994 indicate that the net flux of total DDT is into Lake Superior and
Lake Erie, possibly due to the high levels of wet deposition during 1993-1994. In Lake Huron, there is a
net loss  of total DDT to the atmosphere, and total DDT is in equilibrium between the surface water and
the atmosphere in Lake Ontario.  These data indicate a reversal from net volatilization of total DDT from
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                                        Figure 11-16
  Expected Year that Great Waters Pesticides will be Below Current Detection Limits in
                               the Great Lakes Atmosphere
                                    (Cortes etal. 1998)
           CO
2100  --


2070  --


2040


2010
                           O  Eagle Harbor
                           A.  Sleeping Bear Dunes
                           ^  Sturgeon Point
                           CH  Point Petre
                                                                      P
                                                           P    9
                                                           ^  %   A


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Haven, Michigan. South Haven is located in an area which is primarily devoted to fruit and vegetable
production where the historic application of DDT could have been extensive. However, another potential
source of DDT and its metabolites could be the current use of dicofol (l,l-&zs(4'-chlorophenyl)2,2,2-
trichloroethanol). It has been postulated that agricultural practices and air-soil diffusion affect DDT
volatilization rates from soil. Therefore, a study by the Michigan Department of Environmental Quality
is under way to determine impacts of tillage practices on ambient DDT levels in southwest Michigan and
to assess any possible long-range transport effects (Michigan Department of Environmental Quality
1998).

       Brazner and DeVita (1998) detected DDE in yellow perch and spottail shiners from 23 sites in
Green Bay, Lake Michigan. Because the overall distribution of DDE tissue concentrations was fairly
uniform within the bay, DDE contamination probably originates primarily from non-point sources,
including atmospheric deposition. The few sites that exhibited unusually high DDE residues in fish may
have point sources of DDE in nearby rivers.

        l,l'-(dichloroethenylidene)bis(4-chlorobenzene), or DDE, has been detected in a variety of
organisms at multiple trophic levels in Lake Superior (Kucklick and Baker 1998).  For example, Dykstra
et al. (1998) measured DDE concentrations in nestling blood (1989-1994) and addled eggs (1986-1993)
of bald eagles in Lake Superior and inland Wisconsin sites. A comparison to published and unpublished
historical data indicated that DDE levels declined significantly between 1969 and  1993, with current
levels below those known to result in reproductive impairment.

       In a study of juvenile American alligators in Lake Apopka, Florida, p,p'-DDE was detected in
female serum at 17.98 ± 5.3 (SEM) ng/mL and in male serum at 7.35 ± 2.4 (SEM) ng/mL. Serum
concentrations were significantly higher in females than males. Both male and female alligators in this
area have been associated with abnormal reproductive and endocrine functions (Guillette et al. 1999).

       In a sediment contamination study of the Chesapeake Bay and its tributaries from 1984 to 1991
by Eskin et al. (1996) under the Chesapeake Bay Program, concentrations of DDT and its metabolites
tended to decline from the head to the mouth of the mainstem bay. Highest concentrations (0.0016 ppm
DDT and 0.0023 ppm DDE) were detected in sediments in the upper half of the bay and near the mouths
of the York and Potomac Rivers. Elsewhere in the lower half of the bay, concentrations were generally
below detection limits.  All DDT sediment concentrations were below the aquatic biota  PEL of 0.270
ppm and the aquatic biota NOEL of 0.0045 ppm.  DDE sediment concentrations were below the aquatic
biota PEL of 0.130 ppm at all locations, but maximum concentrations exceeded the DDE NOEL of
0.0017 ppm for aquatic  biota in some locations in the upper bay. In the tributaries, concentrations were
generally below the PELs for aquatic biota.

       Dieldrin. Recent monitoring data from IADN indicate that dieldrin is being transferred out of
the Great Lakes with volatilization from Lake Superior, Lake Erie, and Lake Ontario at 5.9, 6.7, and 6.6
tunes the loadings in 1994 (Hoff et al.  1996). In general, concentrations of dieldrin in precipitation
decreased from 1986 to 1994, but concentrations were three to four times higher at the Lake Erie site
than at the other sites due to higher usage rates in the surrounding agricultural areas. Higher wet
deposition levels were also observed over Lake Michigan due to the greater degree of urbanization
surrounding that lake (U.S. EPA 19981). In Chesapeake Bay sediments between 1984 and 1991, dieldrin
was detected at one site at levels between the aquatic biota PEL and NOEL (Eskin et al. 1996).

       Chlordane.  Chlordane, which was restricted in 1973 to use as a termiticide and was banned in
1988, was used primarily as a pesticide for corn crops (Aigner et al. 1998). Gas phase concentrations of
chlordane in the air over Lake Superior do not currently exhibit a decreasing trend, as has been seen with
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several other banned pesticides. In Chesapeake Bay sediments between 1984 and 1991, maximum
chlordane concentrations were detected at levels between the aquatic biota PEL and NOEL (Eskin et al.
1996).

       Toxaphene. In general, historical toxaphene concentration profiles in sediment cores across the
Great Lakes indicate that the onset of contamination was between 1940 and 1950.  Maximum levels
occurred in the early 1970s to early 1980s, and accumulation rates in Lake Superior and Lake Michigan
largely declined from historical peaks, as shown by comparing maximum historical rates to present rates
(Table 11-25). In addition, Lake Ontario and Lake Superior may have received toxaphene from non-
atmospheric sources in the past (Pearson et al. 1997b).  A back trajectory analysis using IADN
monitoring data indicates that the Great Lakes receive toxaphene via atmospheric deposition from
sources outside of the Great Lakes basin (U.S./Canada IADN Scientific Steering Committee  1998).
Pearson et al. (1997b) investigated the history of toxaphene concentrations and accumulation in dated
sediment cores from Lakes Superior, Ontario, and Michigan and two control lakes near Lake Superior
that receive toxaphene  only via atmospheric deposition. Concentrations at the surface of the cores,
which represent current contamination levels, were similar among all samples with the exception of two
samples from northern Lake Michigan. The similar toxaphene concentrations among the Great Lakes
cores and control lakes suggest atmospheric input is the dominant source of toxaphene to the Great
Lakes. The higher concentrations in the surface of the two northern Lake Michigan cores indicates that
this area may be receiving current inputs (as great as 30-50 percent) from non-atmospheric sources.

                                         Table 11-25
  Current and Maximum Rates of Toxaphene Accumulation in Great Lakes Sediments a
Location
Lake Superior
Northern Lake Michigan
Southern Lake Michigan
near Chicago Urban Area
Lake Ontario
Number of Sediment
Cores Analyzed
3
3
1
3
Accumulation Rates in Sediment
(ng/cm2/yr)
Present
0.097-0.14
0.52-1.01
0.24
0.39 - 0.60
Maximum Historical
0.25
1.07
0.32
1.4
      • All accumulations are focus-corrected.
      Source: Pearson et al. 1997b

       Hexachlorocyclohexanes. The a-HCH and y-HCH isomers are Great Waters pollutants of
concern, whereas (3-HCH (i.e., another of the eight HCH isomers) is not. Both a-HCH and y-HCH can
be transformed into [3-HCH, which is a more toxic and bioaccumulative HCH isomer. Monitoring data
indicate that air concentrations of HCH are decreasing, but the atmosphere continues to be a large source
of HCHs to the Great Lakes. Since the 1980s, a-HCH and lindane (y-HCH) precipitation concentrations
declined; however, between 1991 and 1994,  lindane concentrations increased at Lakes Superior and
Ontario, possibly simply due to data variability. Although dry deposition inputs of HCH are relatively
small (e.g., ranging from 0.2 to 1.5 kg/yr in all but Lake Ontario), the 1994 estimates of dry deposition
are three to 10 times higher than 1992 estimates.  Wet deposition, which is generally uniform across the
lakes, ranges from 46 to 170 kg/yr and is between 0.25 and 1.2 times 1992 estimates, indicating a general
downward trend in wet deposition. A gradient of a-HCH exists, with higher loadings in the lower lakes
than in Lakes Superior and Michigan. Lindane has the highest wet deposition inputs over Lake Huron,
possibly due to a source in upper Michigan (U.S. EPA 19981).
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       The net gas flux of HCH ranges from -140 to +1200 kg/yr (where positive values indicate
volatilization out of the lake) based on monitoring studies.  Both Lake Michigan and Lake Ontario are
saturated with a-HCH (Hoff et al. 1996).  For example, the mass of a-HCH lost through air-water gas
exchange in Lake Ontario is similar to major input and loss factors such as wet deposition and advection
(i.e., transport of the pollutant out of the lake) (Ridal et al. 1997).  The IADN monitoring data also
indicate that total HCHs are in equilibrium with the surface water and the atmosphere in the Great Lakes
(Hillery et al. 1997).

       Hexachlorobenzene. In general, levels of atmospheric deposition of HCB has remained
constant over the past few years. Cohen et al. (1995) used the HYSPLIT/TRANSCO computer program
to determine the amount of HCB emitted from sources to air and water media that is deposited in the five
Great Lakes. The model was run using 1993 source and emissions data from 1,329 identified sources in
the U.S. and Canada.  Table 11-26 provides modeled air deposition estimates, average depositional flux,
and water effluent inputs for the five Great Lakes. The results indicate the following.

•      The depositional flux of HCB to the lakes increases from Lake Superior, Lake Michigan, Lake
       Huron, Lake Erie, to Lake Ontario, following the trend in industrialization around the lakes.

•      Hexachlorobenzene inputs from air deposition are greater than water discharge inputs for Lake
       Superior, Lake Michigan, and Lake Huron.  In Lake Ontario and Lake Erie, the opposite is true;
       however, the estimates for air deposition and waterborne inputs are uncertain for HCB because
       sources outside the U.S. and Canada were not considered in the model and because estimates
       represent the amount of HCB that would be deposited if the lakes were uncontaminated with
       HCB (Cohen et al. 1995).

                                        Table 11-26
            Modeled Air Deposition, Depositional Flux, and Waterborne Inputs
                                of HCB to the Great Lakes
HCB
Total Deposition (kg/yr)
(range)
Depositional Flux (g/km2/yr)
Waterborne Inputs (kg/yr)
Superior
11
(4-49)
0.13
0.1
Michigan
15
(5-73)
0.26
0.8
Huron
16
(6-74)
0.27
0.6
Erie
15
(6-65)
0.58
<72
Ontario
23
(9-101)
1.19
35
Total
79
(30-362)
0.32
<108.5
Source: Cohen etal. 1995

       In general, based on IADN monitoring data, wet and dry deposition of hexachlorobenzene (HCB)
to the Great Lakes did not change from 1992 to 1994. In Lake Ontario, however, wet deposition of HCB
increased six times in 1994 over the 1992 estimate. Hexachlorobenzene is in near equilibrium with the
atmosphere and surface water, but is slightly loading Lake Superior and Lake Michigan and slightly
volatilizing from Lake Erie and Lake Ontario (Hoff et al. 1996).

CROSS-POLLUTANT TRENDS

       The EPA and other groups have initiated programs and projects to collect and compile
information to assess current sources, emissions, loadings, exposure, and effects of pollutants in the
Great Waters. Because many of these programs and projects address multiple pollutants of concern and
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present cross-pollutant results, it is more appropriate to present the pollutant-specific information
together with the program background rather than to split the information between pollutant categories.
Therefore, background information on these various programs or projects along with information on their
results is presented below by program or project. Note that most of these programs and projects are
designed to assess contamination levels in certain media or specific waterbodies.  While each program or
project discussed below addresses a Great Waters waterbody and pollutants of concern, these programs
generally do not directly assess atmospheric deposition. Instead, they address general pollution from
many sources, one of which may be the atmosphere. Other programs and initiatives that portray how
EPA and other agencies are working together to address the remaining issues related to atmospheric
deposition of pollutants to the Great Waters are discussed in Chapter III.
FISH CONSUMPTION
ADVISORIES

       Fish consumption advisories are means
of limiting human exposure when fish taken from
a particular waterbody contain levels of
pollutants that exceed recommended intake
levels. National and regional trends in fish
advisories can be estimated using EPA's database
which contains information such as date of
advisory, waterbody name and location, pollutant;
fish or other wildlife species and range, advisory
type, advisory status (e.g., active), and a contact
name and telephone number (U.S. EPA 1998k).
Note that different sampling methodologies and
different approaches among States and years
makes comparisons among States and years  difficult
widely from State to State.
                                        Types of Fish Advisories

                             States, including the four U.S. Territories and tribal
                             governments, issue advisories for waterbodies in an
                             effort to reduce health risks associated with exposure
                             to pollutants in certain freshwater fish and shellfish
                             species:

                             + Advisories to limit consumption — advisories to
                               either the general population or subpopulations
                               potentially at greater risk (e.g., children, pregnant
                              or nursing women) to restrict their consumption
                              of specific species of fish and other wildlife.

                             + Commercial fishing bans — advisories that prohibit
                               the commercial harvest and sale offish, shellfish,
                               and/or wildlife species from a designated water
                               body (U.S. EPA 1998k).
                             In addition, the amount of monitoring can vary
        In 1997, the number of waterbodies under advisory represented 16.5 percent of the Nation's
total lake acreage and 8.2 percent of the Nation's river miles.  In addition, 100 percent of the Great Lakes
surface waters and their connecting waters, and a large portion of the Nation's coastal waters, are under
advisory for one or more Great Waters pollutants of concern.  According to the Listing of Fish and
Wildlife Advisories in December 1997, 39 of 56 Great Waters were associated with fish advisories for
pollutants of concern (see Appendix C for details on fish advisories in the Great Waters). The number of
advisories in effect for U.S. waterbodies in 1997 increased 5 percent over the number reported in 1996
and 80 percent over the number reported in 1993 (U.S. EPA 1998k). This increase does not necessarily
reflect actual increases of these pollutants in the environment.  Rather, the increase is attributed to an
increase in the number of assessments of contamination levels in fish and wildlife tissues as well as the
use of more rigorous EPA risk assessment procedures by some States to set advisories.

        Although advisories in the U.S. have been issued for a total of 46 pollutants, five Great Waters
pollutants - mercury, PCBs, chlordane, dioxins, and DDT - comprised 95 percent of the advisories in
1997 (U.S. EPA 1998k). The number of advisories in the U.S. increased for three of these major
pollutants and decreased for one, specifically:
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•      Mercury advisories increased 6 percent (1,677 to 1,782) from 1996 to 1997 and 98 percent from
       1993 to 1997 (899 to 1,782).  This increase is primarily because of new mercury advisories in 11
       States, particularly in Minnesota, Ohio, and Louisiana.

•      Advisories for DDT and dioxin rose slightly from 1996 to 1997. Advisories for DDT rose 3
       percent (32 to 33), and dioxin advisories rose 8 percent (60 to 65), after a decline in the number
       of dioxin advisories in 1996.  Dioxin advisories were rescinded in some States, in part, because
       many pulp and paper mills changed their processes.  However, in Michigan, according to the
       1999 Michigan Fish Advisory from the Michigan Department of Community Health, dioxin fish
       advisories were expanded to include Lake Huron, Lake Michigan, and Lake Superior.

•      The number of PCB advisories rose 84 percent from 1993 to 1997. In the last year of this period,
       however, advisories decreased 5 percent (617 to 588), due primarily to rescinding and
       readjusting some previously issued advisories. Despite this recent decline, 30 new advisories
       were issued in 1997 -- mostly by Ohio, Maine, Alabama, Connecticut, Minnesota, Nebraska, and
       New York - making it difficult to discern trends from these advisories alone.

WATER QUALITY ASSESSMENTS

       Surface waters and ground waters throughout the U.S. are monitored regularly to ensure that they
are meeting the water quality standards appropriate to the intended uses. Pollutant concentration levels
are measured to ensure that freshwater sources, including the Great Lakes and Lake Champlain, that are
intended to be used for drinking water do not exceed the maximum contaminant level (MCL) guidelines
for drinking water sources.  In other surface waters, including all Great Waters, monitoring is conducted
to ensure that ambient water quality criteria and other relevant guidelines are not exceeded and that the
waterbodies meet the designated uses (e.g., fishing, swimming, boating).  The current status of the Great
Waters in terms of water quality criteria is described below.

Drinking  Water

       Of the Great Waters, only the Great Lakes and Lake Champlain are fresh waters that can be used
as drinking water sources. Data indicate that both of these water systems provide safe drinking water,
particularly as related to the  Great Waters pollutants of concern. Based on data from 1994 and 1995
collected in support of section 305(b) of the Clean Water Act (CWA) by States, tribes, and other
jurisdictions, most of the Great Lakes nearshore waters can be used as a source of drinking water with
normal treatment (U.S. EPA 1998n). Similarly, the Lake Champlain Basin Program reported that from
1986 to 1995, only nine violations of EPA drinking water standards were reported- all of which were for
coliform contamination in Vermont (Lake Champlain Basin Program 1999).

Other Water Uses

       Data on water quality conditions of the Nation's waters, including the Great Lakes in particular,
are collected and reported by States, tribes, and other jurisdictions to EPA every 2 years as required
under section 305(b) of the CWA. These assessments are based on water quality data that are compared
to water quality standards, such as designated beneficial uses, numeric and narrative criteria for
supporting each use, and an antidegradation statement to protect existing uses and to protect waterbodies
from deteriorating in quality. Data from 1994 and 1995 indicate that approximately 40 percent of the
Nation's surveyed rivers, lakes, and estuaries are too polluted to support basic uses, such as fishing and
swimming. Nutrients and metals are the most widespread pollutants  impacting lakes and rivers with
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agriculture as the most common sources of pollutants; however, atmospheric deposition was also
identified as a source of pollutants.  In estuaries, nutrients are the most widespread pollutants with
industrial point sources, urban runoff, and storm sewers as the most common sources of pollutants (U.S.
EPA 1998n).

       Most of the Great Lakes, in contrast, are safe for swimming and other recreational activities.
However, approximately 97 percent of the surveyed shoreline area shows unfavorable conditions for
supporting aquatic life and is impacted by toxic organic chemicals that appear in fish tissue samples at
much higher concentrations than in water samples. These impacts are partially due to persistent toxic
pollutant burdens, such as PCBs, in the food web. Several of the Great Lakes States identified air
pollution, discontinued discharges from industrial facilities that are no longer in use, urban runoff and
storm sewers, contaminated sediments, land disposal of wastes, and unspecified non-point sources as
pollutant sources contributing to water quality problems (U.S. EPA 1998n).

NOAA'S NATIONAL  STATUS AND TRENDS PROGRAM

       Since 1984, NOAA's National Status and
Trends (NS&T) Program has conducted annual
monitoring of chemical contamination and
biological responses to contamination to
document current conditions and long-term trends
in the environmental quality of U.S. near shore
waters and sediments. The Mussel Watch Project
is a major component of this monitoring program.
Initiated in 1986, the Mussel Watch Project is
designed to provide long-term trends and large-
scale monitoring of pollutant distributions, with
an emphasis on temporal rather than spatial
trends. The project tracks trends in pollutant
concentrations in mollusks at 287 coastal and
estuarine sites on the Atlantic, Pacific, and Gulf
coasts (including Great Waters). Eighty-three of
these sites were recently added, including several
sites from the Great Lakes region. Mussels and
oysters are useful for monitoring changes in
pollutant levels because they are sedentary
organisms and concentrations in their tissues
generally reflect changes in the concentrations in the surrounding water.  Trends were examined in the
Mussel Watch Project for the following Great Waters pollutants of concern: DDT, chlordane, dieldrin,
PCBs, PAHs, cadmium, lead, and mercury (O'Connor 1999).
                                          Florida NS&T Sites

                             A recent monitoring study suggests general
                             decreasing trends in contaminant levels in South
                             Florida (Cantillo et al. 1997), based on
                             concentrations of PAH, PCB, DDT, lindane,
                             hexachlorobenzene, chlordane, lead, mercury, and
                             cadmium in bivalves from seven South Florida sites
                             monitored by the NS&T Program during the period
                             1986 to 1994.  Contaminant levels in South Florida
                             were generally lower than nationwide.  Nevertheless,
                             a recent sediment quality assessment indicates that
                             resident benthic communities may be adversely
                             impacted by contaminants at a number of locations in
                             Tampa Bay (Carr et al. 1996).  For instance, up to 73
                             percent of the sediment pore water samples were
                             toxic to sediment biota in at least one of the toxicity
                             tests. In addition, sediment concentrations of several
                             metals and PAHs were correlated with sediment
                             toxicity, and concentrations of lead, PAHs, PCBs,
                             and DDT equaled or exceeded sediment quality
                             guidelines in several locations.
        Also as part of the Mussel Watch and Benthic Surveillance Projects, NOAA conducts sediment
toxicity assessment studies to determine the extent and severity of sediment toxicity in U.S. coastal
regions.  Sediment toxicity studies are conducted based on the following considerations: (1) a high level
of contamination in oysters or mussels sampled hi the NS&T Program; (2) the likelihood of adverse
biological effects of contamination based on State and local data; and (3) possible collaboration with
other Federal, State, and local agencies.  Since 1991 when NOAA began conducting these studies, 23
coastal bays and estuaries covering approximately 4,000 km2 have been the subject of studies (see text
box). Study sites range in size from 0.3 km2 to 1,350 km2. Sediment toxicity surveys include three
different toxicity tests which measure different biological endpoints leading to different results: (1) the
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 amphipod survival test using whole sediment; (2) the sea urchin fertilization test using sediment
 porewater; and (3) the Microtox test which measures decreased light production by a luminescent marine
 bacterium, Vibrio flscheri, using an organic extract of the sediment. The concentration of approximately
 80 chemical contaminants, including mercury, lead, cadmium, PAHs, chlorinated dioxins and
 dibenzofurans, DDT and its metabolites, dieldrin, chlordane, lindane, HCH, and HCB, are measured in
 sampled sediments.  Results of these studies are discussed below (NOAA 1999).

 National Trends

        Data collected between 1986 and 1996 from the Mussel Watch Project indicate that
 concentrations of most of the Great Waters pollutants of concerns in mussel and oyster tissues are
 decreasing at some sites. Specifically, decreasing trends of DDT, chlordane, dieldrin, PCBs, and
 cadmium were evident. Concentrations of cadmium declined despite the fact that other trace metals,
 including mercury and lead, exhibited no overall trend during this period. Data for PAHs also indicated
 no overall trend.  Lindane and hexachlorobenzene were so infrequently detected that no trend
 determinations could be made. Another study found a decreasing trend for cadmium and lead, and no
 overall trend for PAHs (Lauenstein and Daskalakis  1999, O'Connor 1999, NOAA 1998).

        The NOAA analyzed spatial trends in sediment contamination based on data collected for the
 Benthic Surveillance Project and the Mussel Watch Project (NOAA 1998), and found that both trace
 metal and organic contamination are associated with urban areas. Sites with "high" levels of
 contamination were located in urbanized areas of the Northeast, San Diego, Los Angeles, and Seattle.4
 The cut-off levels that indicated "high" concentrations for DDT, PCBs, chlordane, dieldrin, PAHs,
 mercury, cadmium, and lead are 140 ppb, 430 ppb, 34, ppb, 9.1 ppb, 1100 ppb, 0.23 ppm, 6.2 ppm, and
 4.8 ppm (mussels) and 0.84 ppm (oysters), respectively. "High" concentrations were rare in the
 southeast and along the Gulf of Mexico.  Most sites with "high" contaminant concentrations can be
 linked to anthropogenic sources.  Tissue concentration data can be misleading, however, because in some
 areas natural background levels and characteristics of chemicals can result in higher tissue
 concentrations. For example, high concentrations of cadmium and other trace metals in zebra mussels of
 the Great Lakes may be due  to greater bioavailability of those metals in fresh water (NOAA 1998).

        The sediment toxicity surveys, on a national level, indicate that 7 percent of the sediment in all of
 the study area was toxic based on the amphipod survival test; 39 percent was toxic based on the sea
 urchin fertilization test; and 66 percent was toxic based on the Microtox luminescence test.  In general,
 larger estuaries and bays (areas greater than or equal to 250 km2 or 100 mi2) had a lower average spatial
 extent of sediment toxicity (i.e., 6 percent)  as compared to smaller estuaries and bays (i.e., 10 percent).
 However, sediment toxicity varies considerably among study areas in terms of spatial extent and severity
 of toxicity. Furthermore, based on amphipod survival tests, NOAA found that the spatial extent of
 toxicity was about 35 percent in small urbanized estuaries in the Northeast and southern California and
 was only 3 percent in southeastern estuaries, which border coastlines, farms, forests, wetlands, and fewer
 industrialized areas (NOAA  1999).
       4 Areas with "high" concentrations were identified based on concentration distributions. "High"
concentrations were defined as those with logarithmic values greater than the mean logarithmic value for all
concentrations plus one standard deviation. Therefore, about 15 percent of all concentrations were "high."
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Trends in Great Waters

       Pollutant trends based on mussel and oyster tissue data collected for the Mussel Watch Project
from 1986 to 1996 at several Great Waters sites are shown in Table 11-27 (NOAA 1998).  Similar trends
were also reported in the Second Report to Congress (U.S. EPA 1997b). Decreasing trends are
statistically significant (confidence level of 95 percent); however, quantitative information regarding the
changes in pollutant levels was not provided. Therefore, the magnitudes of the increases or decreases
cannot be compared between sites.

                                         Table 11-27
         Trends of Pollutant Concentrations in Mussel Watch Project (1986-1996)
Waterbodies
(number of sites
examined)
Chesapeake Bay
(6 sites)
Delaware Bay
(6 sites)
Long Island Sound
(9 sites)
Narragansett Bay
(3 sites)
Tampa Bay
(6 sites)
Galveston Bay
(6 sites)
Contaminant Trend (number of sites affected) a
Mercury
~(6)
~(6)
~(9)
~(3)
~(6)
~(6)
Lead
-(5)
*(1)
-(6)
-(8)
4(1)
~(2)
4(1)
**(5)
T(1)
-(6)
Cadmium
"(5)
*d)
-(5)
4(1)
4(5)
~(4)
~(3)
-(6)
*-(6)
PCB
4(4)
-»(2)
-(5)
4(1)
4(5)
~(4)
-(3)
-(6)
-(6)
DDT
"(3)
4(3)
-(6)
-(5)
4(4)
-(3)
<-»(4)
4(2)
~(6)
PAH
-(6)
-(6)
~(9)
-(3)
-(6)
-(6)
Chlordane
4(5)
-(1)
~(4)
4(2)
4(6)
-(3)
~(3)
-(3)
4(3)
~(4)
*(2)
Dieldrin
-(3)
4(3)
-(5)
4(1)
~(9)
"(3)
-(6)
"(4)
*(2)
• Sites were sampled in at least 6 of 10 years; trend indicated by arrow (i.e., 4 = decreasing trend; I = increasing
trend; <-* = no trend). Number of sites showing trend within each waterbody is indicated in parentheses.
Source: NOAA 1998

        In Tampa Bay, specifically, NS&T chemical contamination data for sediments, bivalves, and
fish through 1991 indicate that there is not a bay-wide pattern of increasing or decreasing concentrations
over recent years. However,  increases and decreases were observed in some sample locations. Local
geographic contamination trends indicate that sediment toxicity is highest in regions of northern
Hillsborough Bay and moderate in regions of western Old Tampa Bay, along the western shore of Middle
Tampa Bay, and in lower Boca Ciega Bay. The least toxic or nontoxic samples were taken from portions
of Old Tampa Bay, and Middle and Lower Tampa Bay.  Relatively high concentrations of petroleum
hydrocarbons, chlorinated pesticides, other chlorinated hydrocarbons, ammonia, and trace metals were
detected in the most toxic samples (Long and Greening 1999).

        In the Chesapeake Bay, NS&T Program data from 186 sites from 1986 through 1995 generally
indicate no trend in contamination levels in mollusks for each chemical analyzed. However, when trends
were detected, decreases greatly outnumbered increases. Specifically, contamination levels decreased for
chlordane, DDT, and dieldrin (Cantillo et al. 1998).

        Consistent with trends on a national level, most of the Great Waters  sites do not exhibit a
statistically significant trend or change in pollutant levels in mollusk tissues during  the 10-year period.
Trends, when present, were mainly decreasing since 1986 (i.e., for cadmium, PCBs, DDT, PAHs,
Page 11-72
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                                                                                  Chapter II
                                                                     Environmental Progress
chlordane, and dieldrin).  According to O'Connor (1999) and NOAA (1998), decreases in levels of these
chemicals are probably the result of bans on the use of chlorinated hydrocarbons (e.g., chlordane, DDT,
PCBs) and the reduced use of certain chemicals.

NATIONAL SEDIMENT QUALITY  SURVEY

       The National Sediment Quality Survey (NSQS) describes the accumulation of chemical
contaminants in the Nation's rivers, lakes, estuaries, and coastal waters. The NSQS is the first of three
volumes of the first biennial Report to Congress on  the Incidence and Severity of Sediment
Contamination in the United States (U.S. EPA 1997i). The NSQS includes a screening-level assessment
comparing human and ecological health benchmarks (e.g., draft sediment quality criteria, EPA cancer
and noncancer human health risk levels) to concentrations of contaminants in sediment or, for human
health only, to actual or estimated fish tissue concentrations.  Results indicate the following.

•      About 5 percent (i.e., 96) of the Nation's watersheds include APCs (Figure 11-17, Appendix D
       includes the names of the numbered sites). The watersheds of the Great Lakes, Chesapeake Bay,
       and at least 17 NEP and NERRS sites are associated with APCs. An additional 39 percent of
       watersheds include at least one sampling station where contamination levels suggest probable
       adverse effects. Among that 39 percent are  the watersheds of the Great Lakes, Chesapeake Bay,
       Lake Champlain, and some coastal waters.  Only about 6 percent of watersheds did not indicate
       potential adverse effects on aquatic life or human health.  Although there were no contaminant
       data for 35 percent of the watersheds,  the data used were from monitoring programs targeted to
       areas with known or suspected contamination.

•      Probable aquatic life impacts were observed 41 percent more frequently than probable human
       health impacts. Specifically, of the 21,096 sites  sampled, 3,287 had probable aquatic life impacts
       and 2,327 had probable human health impacts.

•      The contaminants detected most frequently at levels indicating probable adverse effects include
       PCBs, mercury, pesticides, and PAHs. Polychlorinated biphenyls were the sole or among the
       responsible indicators at 58 percent of the most contaminated (i.e., probable effects) sampling
       stations. Non-mercury metals were solely responsible for about 6 percent of the most
       contaminated sampling stations and 28 percent of the moderately contaminated (i.e., possible
       effects) sampling stations.

CHESAPEAKE BAY PROGRAM

       As part of the Chesapeake Bay Program and in support of the goals and commitments of the
Chesapeake Bay Agreement, information has been collected to assess the progress that has been made in
reaching those goals.

•      A recent analysis of 10 years of monitoring  data indicates that the water quality of major rivers
       and freshwater portions of the bay has improved, probably due to reduced runoff from
       agricultural lands, the phosphate detergent ban, and point source reductions in phosphorous and
       nitrogen releases (e.g., at wastewater treatment facilities) (Chesapeake Bay Program 1998d).

•      The amount and extent of submerged aquatic vegetation (SAV) is a good indicator of water
       quality in the Chesapeake Bay. Although the areal coverage of bay grasses, or SAV, increased
       by 9 percent to 69,238 acres in 1997, in 1998 the acreage had decreased by 8 percent to 63,496
Deposition of Air Pollutants to the Great Waters - 3  Report to Congress 2000
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               (A
               •o
               Q)


               I
               O
               <*-«


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               o

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                                                                                   Chapter II
                                                                      Environmental Progress
        acres. The reasons for the 1998 decrease are unclear, but higher-than-average flow conditions in
        1998 are a likely factor.  Even so, the total acreage of SAV in 1998 still represents a 70 percent
        increase over the 1984 low point and 56 percent of the goal to restore 114,000 acres of SAV by
        2005 (Chesapeake Bay Program 1999b).

 •       National Toxics Release Inventory (TRI) data from 1988 to 1997 indicate a 67 percent reduction
        in chemical releases and transfers from industrial facilities to the bay. Releases of eight of the
        Chesapeake Bay Program Toxics of Concern (several of which are Great Waters program
        pollutants of concern), however, increased sharply in 1995, mostly due to the activities of a few
        facilities that were responsible for almost half of the releases (Chesapeake Bay Program 1998c).

 •       From 1985 to 1997, total nitrogen concentrations decreased in the Susquehanna River, which
        provides over 50 percent of the fresh water to the bay.  Nitrogen concentrations decreased in six
        of the major rivers to the bay (i.e., Susquehanna, Patuxent, Rappahannock, Mattaponi, James,
        Appomattox) and remained unchanged in two other rivers (i.e., Potomac, Pamunkey (a tributary
        to the York)). In contrast, total nitrogen concentrations increased in the upper central portion of
        the bay (i.e., the region around the Patapsco and Chester rivers) (Chesapeake Bay Program
        1998b).

 LAKE CHAMPLAIN SEDIMENT TOXICS ASSESSMENT PROGRAM

        Phase II of the Lake Champlain Sediment Toxics Assessment Program investigated the three
 most contaminated areas of the lake: Cumberland Bay, Burlington Harbor, and Malletts Bay (Mclntosh
 et al. 1997). Sediments of Cumberland Bay at Plattsburgh, New York are contaminated with PCBs from
 local historical sources and a possible source entering from the Saranac River. Water column
 concentrations in Cumberland Bay generally range from 0.3 to 2.1 ng/L, approximately an order of
 magnitude higher than in the main portion of the lake which has concentrations similar to present day
 levels in the Great Lakes.  Water column concentrations of PCBs decreased dramatically with distance
 from the PCB "hot spot" near Wilcox Dock.  Maximum concentrations near Wilcox Dock are up to 41
 ng/L or 100 times greater than levels in the main body of the lake (Mclntosh et al. 1997). The New York
 State Department of Environmental Protection recently completed a cleanup plan for Cumberland Bay,
 which will remove the most contaminated sediment near Wilcox Dock.

        Surface sediment analyses at Burlington Harbor reveal that cadmium, copper, chromium, lead,
 and zinc display no clear spatial distribution, suggesting non-point sources (e.g., storm water,
 atmospheric deposition) for these metals. Bioavailability of metals appears to vary seasonally. Organic
 contaminants in Burlington Harbor (including PCBs, PAHs, and selected pesticides) generally exceeded
 the low estimate of sediment contamination levels  at which adverse effects are predicted to occur among
 sensitive species or sensitive life stages. The PAHs and DDE exceeded the estimate of the sediment
 concentration levels at which toxic effects are predicted to occur among most species. Toxicity tests and
 benthic community analyses in Burlington Harbor  showed chronic toxicity for a limited number of
 species, but the harbor does not appear to exhibit widespread hazardous conditions for aquatic life. In
 outer Mallets  Bay, sediments frequently exceeded severe effects levels for some metals; however,
 mercury, lead, and cadmium were not the responsible contaminants (Mclntosh et al. 1997).
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SAN FRANCISCO ESTUARY REGIONAL MONITORING PROGRAM
FOR TRACE SUBSTANCES

       The San Francisco Estuary Regional Monitoring Program for Trace Substances began in 1993,
and results are available from monitoring through 1996.  This program collects data on water, sediment,
and tissue contamination levels for a variety of pollutants, including some Great Waters pollutants of
concern. Analyses of water column concentrations indicate that PCBs, PAHs, certain chlorinated
pesticides, and mercury exceed water quality criteria (Table 11-28).  In sediments, mercury, total DDTs,
and dieldrin frequently exceed levels at which adverse ecological effects are possible.  An analysis of
contaminant bioaccumulation by bivalves indicates that PCBs and PAHs are above the maximum tissue
residue levels (MTRLs, relatively recently developed, science-based guidelines). Polychlorinated
biphenyls, dioxin, mercury, dieldrin, DDT, and chlordane concentrations in fish tissue exceed EPA
screening values for human consumption. Lead levels are usually below water and sediment quality
guidelines and have not shown evidence of bioaccumulation or biological effects. In comparing data
over several years, concentrations of mercury, lead, and chlordane are decreasing in tissues. Overall, the
condition of the San Francisco estuary seems to be improving over time. Additional trends analyses will
be conducted as additional data are collected (San Francisco Estuary Institute 1997).

                                        Table 11-28
                 Percentages of 1996 Samples that Exceeded Guidelines
                              in the San Francisco Estuary
Pollutant
Cadmium
Mercury
Lead
PCBs
PAHs
Chlordane
Dieldrin
p.p'-DDE
Water (Dissolved)
0
0
0
NA
NA
NA
NA
NA
Water (Total)
0
19
6
93
0
12
8
16
Sediment
0
81
6
6
38
31
68
71
Bivalve Tissue
-
0
-
100
100
89
78
15
— = no consistent guidelines
Source: San Francisco Estuary Institute 1997
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                                       CHAPTER III
                 MAJOR PROGRAMS AND ACTIVITIES
   National Programs and Activities	  HI-3
   ••Multimedia Activities	IH-4
   ••HAP Controls	HI-11
   ••Stationary Source Controls Addressing NO x	Ill-17
   ••Mobile Source Program Activities	111-29
   ••Ozone and PM NAAQS	111-30
   ••Other National Programs  	111-30

   Regional and Waterbody-specific Programs  ... 111-34
   ••Great Lakes Program	111-35
   ••Lake Champlain Basin Program	111-37
   ••Chesapeake Bay Program	111-38
   ••Gulf of Mexico Program  	111-41
   ••National Estuary Program 	111-42
   •-NOAA Activities 	111-48
   ••Ozone Transport Commission 	111-49
State, Local, and Tribal Activities	111-51
••State and Local Activities	 111-51
••Tribal Activities	 IH-60

Industry Activities  	IH-63
••Chlor-alkali Industry Mercury Reduction Goal  111-63
••Voluntary Mercury Agreement with Northwest
  Indiana Steel Mills  	 111-64
"American Hospital Association MOU 	 111-64
••Electric Power Research Institute Studies .... 111-65

Work With Other Countries 	ffl-66
••Canada-U.S. Binational Toxics Strategy 	 111-66
••International Joint Commission	 111-69
•-LRTAP Protocol on Heavy Metals and POPs . 111-70
-UNEP Global POPs Initiative 	 111-71
••NAFTA Commission on Environmental
  Cooperation  	 111-71
••U.S.-Canada Air Quality Agreement 	 111-72
        This chapter summarizes major programs and activities undertaken or completed since the
Second Great Waters Report to Congress. All of these programs and activities are helping to address
issues relevant to the Great Waters program.  The focus of this chapter primarily is on regulatory and
policy initiatives as opposed to new science or research, which is covered in Chapter IV. Although some
of the programs and activities described are being performed in conjunction with the EPA's Great Waters
program, most are not. Many of the activities are led by partners outside the EPA, and have been
included because they contribute to emission reductions and loadings of Great Waters pollutants of
concern.
Deposition of Air Pollutants to the Great Waters - 3  Report to Congress 2000
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Chapter in
Major Programs and Activities
                                       CHAPTER 3 HIGHLIGHTS
     There are more than 60 programs in progress, described in this chapter, that directly or indirectly address issues
     of concern to the Great Waters.

     Programs described in this chapter reduce the use of Great Waters pollutants of concern, reduce emissions of
     pollutants, restore (e.g., by sediment remediation) the Great Waters where they have been impacted, mitigate
     (e.g., by reducing consumption of contaminated fish) human health or ecological effects of Great Waters
     pollution, and provide a better scientific understanding of the sources, processes, and effects of and solutions to
     atmospheric deposition.

     Essentially all of EPA's Program Offices and most Regional Offices are involved in national, regional, or
     waterbody-specific activities addressing Great Waters issues.

     The EPA activities affecting Great Waters issues are performed under EPA's traditional media- and statute-
     specific programs (e.g., CAA programs) and under Agency-wide and inter-program multimedia initiatives (e.g.,
     the Persistent Bioaccumulative Toxics Initiative (PBTI),  Clean Water Action Plan).

     In addition to EPA, numerous other parties (including other Federal agencies; municipal, State, tribal and
     international governing  bodies; the private sector; and, academic researchers) are leading programs which
     address Great Waters issues and pollutants of concern.

     The majority of the programs and activities described in this chapter involve collaborative partnerships, and
     many use community-based approaches to address local environmental priorities that are also Great Waters
     issues.
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                                                                                      Chapter III
                                                                   Major Programs and Activities
 III.A
NATIONAL PROGRAMS AND ACTIVITIES
        A number of EPA's national programs and activities contribute to understanding and reducing
pollutant impacts on the Great Waters. As discussed in Section IB, most of the Great Waters pollutants
of concern are also the focus of other national programs and activities. These programs and activities
protect and enhance the quality of surface waters throughout the U.S., including the Great Waters.
Recent accomplishments of these other programs and activities are summarized below, organized by
whether they are considered multimedia activities, HAP-specific controls, mobile source program
activities, or other national programs.
     Persistent
 Bioaccumulative
        Toxics
      Initiative
        TMDL
      Program


        Waste
   Minimization
      National
         Plan
                                        Stationary Source Controls (MACT, NOX Programs)
                     Acid Rain Program
                                                                             Integrated Urban
                                                                            Air Toxics Strategy
                       Clean Water
                       Action Plan
" Contaminated Sediment
 Management Strategy •
                                Great Waters
                                  Aquatic
                                Ecosystems
                         -  I.

                          •""" '
                                                Sediment
     Fish
 Contamination
   Program
 Sediment Quality
Report to Congress
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Chapter in
Major Programs and Activities
MULTIMEDIA ACTIVITIES


Persistent Bioaccumulative Toxics Initiative

        The Persistent Bioaccumulative Toxics Initiative (PBTI) which was developed in an EPA-wide
effort chaired by the Office of Prevention,
Pesticides and Toxic Substances (OPPTS),
supports Great Waters program goals by helping
to reduce environmental releases of certain Great
Waters pollutants of concern. The goal of the
PBT Initiative is to further reduce risks to human
health and the environment from existing and
future exposure to persistent, bioaccumulative,
and toxic (PBT) pollutants. The initiative seeks to
accomplish this goal through increased
coordination among EPA national and regional
programs with the significant involvement of
international, State,  local, and tribal organizations,
the regulated community, environmental groups,
and private citizens. This effort fortifies existing
EPA commitments related to priority PBTs, such
as the 1997 Canada-U.S. Binational Toxics Strategy (BNS), the North American Agreement on
Environmental Cooperation, and EPA's Clean Water Action Plan (see below for more information on
these activities).

        The PBT Initiative initially will focus on the 12 priority pollutants identified under the
Binational Toxics Strategy (BNS) (see sidebar below). The.initiative includes the following steps:
                                   Guiding Principles for PBT Initiative

                               Address problems on multimedia basis through
                               integrated use of all EPA tools
                               Coordinate with and build on relevant
                               international efforts
                               Coordinate with relevant Federal programs and
                               agencies
                               Stress cost-effectiveness
                               Involve stakeholders
                               Emphasize innovative technology and pollution
                               prevention
                               Protect vulnerable subpopulations
                               Base decisions on sound science
                               Use measurable objectives and assess
                               performance
                                                  Binational Toxics Strategy - Level I Substances
                                                 Aldrin/dieldrin"
                                                 Benzo(a)pyrene"
                                                 Chlordane'
                                                 DDT (ODD/DDE)*
                                                 Hexachlorobenzene"
                                                 Alkyl lead'
                                                 Mirex
                                                      Mercury and
                                                      compounds"
                                                      Octachlorostyrene
                                                      PCBs*
                                                      Dioxins and furans*
                                                      Toxaphene"
                                                        "Great Waters pollutants of concern
1.      Develop and implement national action
       plans for priority PBT pollutants.  Near-
       term activities include pollution
       prevention projects, enforcement and
       compliance assistance, development or
       revision of water quality criteria,
       research and analysis of emission and
       discharge controls and other topics, and
       collaboration with other international
       efforts beyond the BNS. The draft
       Mercury Action Plan has been developed
       and includes regulatory and
       nonregulatory initiatives.

2.      Screen and select more priority PBT pollutants for action.  The EPA will apply selection criteria
       for additional pollutants in consultation with a technical panel.

3.      Prevent introduction of new PBTs.  The EPA is acting to prevent new PBT chemicals from
       entering commerce by (1) proposing criteria for new PBT chemicals, (2) developing a rule to
       prevent re-introduction of phased out PBTs, (3) developing incentives to reward development of
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                                                                                       Chapter in
                                                                   Major Programs and Activities
        PBT alternatives, and (4) documenting how PBT-related screening criteria are being taken into
        account for approval of new pesticides and re-registration of existing pesticides.

4.      Measure progress. The EPA is in the process of defining measurable objectives to assess
        progress. These could include trend detection in environmental health, direct measurements of
        human exposure through biomarkers, tracking of chemical releases to the environment, and
        program activity measures such as enforcement actions.

        The EPA solicited public comments on a draft PBT Initiative published in late 1998. For further
information on the status of the initiative, see the web page at www.epa.gov/pbt/strtegy.htm.

Total Maximum Daily Loads

        Under the Federal Clean Water Act of 1972 (CWA), EPA is required to develop effluent
guidelines for specific categories and classes of point sources. The guidelines are used to set discharge
limits for specific facilities that discharge pollutants to surface waters or to municipal sewage treatment
systems (63 FR 22644, April 27, 1998). However,
many U.S. waterbodies do not meet applicable
water quality standards, which include standards
for many Great Waters pollutants of concern,
despite the implementation of the CWA (see
sidebar), in part because of non-point source
pollution, including atmospheric deposition. Total
maximum daily loads established under section
                                                         National Water Quality Inventory

                                                 "The final National Water Quality Inventory Report to
                                                 Congress for 1996 indicates that of the 72 percent of
                                                 estuary waters assessed, 38 percent are not fully
                                                 supporting uses/standards and 4 percent are
                                                 threatened." (U.S. EPA 1998o).
303(d)(l) of the CWA, provide a framework for
addressing pollution from both point and non-point sources. A TMDL is developed for a waterbody if
water quality standards within the waterbody are not being met using technology-based or other effluent
controls. A TMDL establishes the maximum allowable pollutant loading for a waterbody (including
allocations for point source loads and non-point source loads, and a margin of safety) that will result in
the waterbody meeting established water quality standards.  Specifically, TMDLs assess non-point
source loads, such as atmospheric deposition, in addition to point source inputs.  In some cases, TMDLs
                                                   attempt to identify the source of atmospheric
                                                   deposition in order to implement appropriate
                                                   measures to decrease the pollutant inputs to a
                                                   watershed. In terms of atmospheric deposition,
                                                   EPA is developing science and tools to assess the
                                                   contribution of atmospheric sources to water
                                                   pollution and to assist in decreasing total
                                                   pollutant loadings to waterbodies.
    Mercury TMDL Air Deposition Pilot Project

In order to assist States in preparing TMDLs for
waterbodies affected by atmospheric pollutants, the
EPA Office of Water (OW) and Office of Air Quality
Planning and Standards (OAQPS) have initiated the
Mercury TMDL Air Deposition Pilot Project.  This
project, a collaborative effort between OAQPS, OW,
the Office of Research and Development, EPA
regional offices and State agencies, will investigate
tools and approaches for developing TMDLs in cases
involving atmospheric pollutants. The project will
design, develop, and identify uncertainties and data
needs for pilot mercury TMDLs for two waterbodies
receiving mercury contributions from the air. In the
process, the compatibility of air and water quality
modeling systems, as well as the linkages between
the CWA and CAA will be evaluated.  Two pilot
TMDL waters have been selected for study (Devil's
Lake, Wisconsin, and the Everglades Conservation
Area 3a, Florida). Modeling work is under way.
                                                           As required by the CWA, States are
                                                   directed to identify and directs States to identify
                                                   and establish a priority ranking for waters that do
                                                   not meet applicable water quality standards after
                                                   application of technology-based and other
                                                   controls, taking the severity of the pollution and
                                                   the designated uses of the waterbody into
                                                   consideration. The EPA's implementing
                                                   regulations require States to submit these lists
                                                   every 2 years. Once the list of priority waters is
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Chapter HI
Major Programs and Activities
approved by EPA, the State establishes TMDLs for each waterbody on the list to restore water quality.
The TMDL specifies the amount of pollution or other stressor that needs to be reduced to meet water
quality standards, allocates pollution control or management responsibilities among sources in a
watershed, and provides a scientific and policy basis for taking actions needed to restore a waterbody
(U.S. EPA 1998o). A TMDL may also identify the need for point source or non-point source controls.
The EPA recently began development of a TMDL pilot project addressing atmospheric  deposition of
mercury (see sidebar).

       A variety of tools have been created to assist States in the process of developing TMDLs. Many
of the tools were created in response to challenges encountered in allocating non-point source inputs of
nitrogen compounds to specific land uses.  Additional tools have been developed to assist in decreasing
loadings to waterbodies. See, for example, the discussion of the Albemarle-Pamlico Estuary (NC) under
the National Estuary Program in Section III.B.

       Also, to assist in the implementation of TMDLs in States, EPA published a report,  TMDL
Development of Cost Estimates: Case Studies of 14 TMDLs (U.S. EPA 1996b).  The selected TMDL case
studies are from a variety of geographic locations, address the most common pollutants, range from
small- to large-scale projects, and represent a range of complexity levels.  The report also identifies
funding sources and discusses benefits of TMDLs (U.S. EPA 1998v).

Pulp and Paper Cluster Rule

       In April 1998, EPA promulgated the pulp and paper cluster rule - a joint CAA and CWA rule -
which is designed to protect human health and the environment by reducing releases of toxic pollutants
from the pulp and paper industry to air and water. This rule is the first integrated regulation to control
the release of pollutants to more than one media from one industry. Implementation of the rule will
further reduce paper industry air emissions and surface water discharges of certain Great Waters
pollutants of concern (e.g., dioxins and furans).

       By issuing joint standards, industry can consider all regulatory requirements at  one time;
therefore, reducing the regulatory burden and allowing mills to select the best combination of pollution
prevention and control technologies that will provide the greatest protection to human health and the
environment.  The cluster rule requires new and existing pulp and paper mills (1) to capture and treat
toxic air pollutant emissions that occur during cooking, washing, and bleaching stages of the pulp
manufacturing process and (2) to meet new effluent limits for toxic pollutants in the wastewater
discharged during the bleaching process and in the final discharge from mills in the bleached papergrade
kraft and soda subcategory and in the bleach papergrade sulfite subcategory.  The rule limits releases of
toxic air pollutants from processes that are used at 155 of the 565 U.S. pulp and paper mills (i.e., the rule
applies to paper and paperboard mills, also referred to as kraft, soda, sulfite, and semi-chemical mills)
along with water discharges of toxics and other pollutants from the 96 of those 155 mills that bleach pulp
to make paper. The new water limits are based on substituting chlorine dioxide for chlorine in the
bleaching process (63 FR 18504, April 15, 1998).

       The new air and water standards under the pulp and paper cluster rule will provide significant
environmental benefits, including:

•      Seventy-three rivers  and streams will become cleaner because of toxic release reductions;

•      Emissions of over 160,000 tons of toxic air pollutants will be eliminated;
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                                                                                     Chapter IU
                                                                  Major Programs and Activities
 •       Dioxin and furan discharges to water will be reduced by 96 percent; and,

 •       Ultimately, all dioxin fish consumption advisories associated with the 96 mills affected by this
        action will be eliminated (63 FR 18504, April 15, 1998).

        The pulp and paper cluster rule also includes an innovative voluntary incentives program (i.e.,
 the Voluntary Advanced Technology Incentives Program). Under this program, mills are voluntarily
 subject to more stringent standards in return for rewards, such as increased compliance time, reduced
 monitoring requirements and inspections, greater permit certainty, reduced penalties, and public
 recognition (63 FR  18504, April 15, 1998).  For example, mills participating in the program are allowed
 6 years instead of 3  years to comply with air standards and 6 to 16 years to comply with water discharge
 permit limits, depending on the performance level of the new technology or process change. This
 program also encourages mills to consider all technology options prior to making large investment
 decisions, such as purchasing new emissions control devices or implementing major process changes
 (U.S. EPA 1997d).  In the long term, this innovative program could result in additional reductions in air
 toxics releases and water pollutant discharges.

 Mercury Research  Strategy

        The EPA, in an intra-agency effort led by EPA's Office of Research and Development, is
 developing a Mercury Research Strategy, which is expected to be completed in 2000. The EPA plans for
 the strategy to describe:

 •       The key scientific questions of greatest concern to EPA for mercury risk assessment and  risk
        management that EPA plans to investigate over the coming 5 years; and,

 •       A research program which would provide information, methods, models, and data to address
        these key scientific questions.

 The research strategy is intended to guide EPA's development of research plans and decisions about
 future research priorities and budgets. It may also provide useful information to others in guiding then-
 research. However, the strategy is not intended to convey information on specific projects, nor will it
 provide a detailed schedule of outputs or
 products.
Clean Water Action Plan

        Completed in February 1998, the Clean
Water Action Plan is an interagency, multimedia
strategy to address remaining obstacles to the
original goal of the Clean Water Act - "fishable
and swimmable" water for all Americans (U.S.
EPA 1998a). The action plan was requested by
Vice President Al Gore on October 1997 to mark
the 25th anniversary of the Clean Water Act. It
forms the core of President Clinton's Clean Water
Initiative, which was proposed in the 1998 State
of the Union Address. Together, the Clean Water
           Clean Water Action Plan:
Key Actions to Assess and Reduce Air Deposition
                 of Nitrogen

"EPA and NOAA will work with other Federal, State,
tribal, and local government agencies and others to
better quantify the risks associated with atmospheric
deposition of nitrogen compounds and other
pollutants to waterbodies."

"EPA will work through the TMDL program to
evaluate the linkage of air emissions to the water
quality impacts to help determine appropriate
reduction actions. EPA will work with States, tribes,
and Federal land management agencies to employ
both Clean Water Act and Clean Air Act authorities to
reduce air deposition of nitrogen compounds and
other pollutants that adversely affect water quality."
(U.S. EPA1998a)
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Chapter III
Major Programs and Activities
Action Plan and Initiative outline specific actions to strengthen and expand efforts to restore and protect
water resources.

       The plan identifies non-point sources (including atmospheric deposition) as the most important
remaining threat to water quality.  Because EPA's existing water programs do not focus on control of
non-point sources, the action plan emphasizes innovative approaches such as partnerships with local
stakeholders and watershed-level projects. Atmospheric deposition is among the leading non-point
sources addressed by the action plan. In particular, agencies pledged to work together to better assess the
risks associated with atmospheric deposition of nitrogen compounds (see sidebar) and other pollutants to
waterbodies and to integrate air deposition into TMDL evaluations.  In addition, EPA will include air
deposition in a multiagency coastal research strategy and coordinated coastal monitoring plan, expected
to be issued in 2000.

       Another action in the President's Clean Water Action Plan is to conduct a national survey of
levels of persistent bioaccumulative toxic (PBT)  chemical levels in fish and shellfish throughout the
country.  Specifically, EPA and NOAA are conducting a study to estimate the national distribution of the
mean levels of selected PBT chemical residues in fish and shellfish tissue in U.S. waters.  The study will
provide information for the Agency's PBT Initiative, which seeks to identify potential areas of concern
for human and/or ecological health.  The study offish tissue may reveal where PBT chemicals not
previously considered a problem are present in the environment at levels of concern. For the national
fish study, fish will be obtained from lakes and reservoirs which have been selected according to a
probability design. The shellfish survey will be based on the data obtained by NOAA's ongoing Mussel
Watch Project. Both studies will be coordinated with State and tribal efforts to maximize geographic
coverage.

Sediment Quality Report  to Congress

       Once deposited to surface waters from the air or other sources (e.g., industrial and municipal
point discharges, urban and agricultural runoff), most of the Great Waters pollutants of concern tend to
accumulate in sediments where they may reach concentrations harmful to aquatic life and the food web.
In recognition of environmental and economic problems associated with contaminated sediment,
Congress included in the Water Resources Development Act (WRDA) of 1992 a requirement for EPA, in
cooperation with NOAA and the U.S. Army Corps of Engineers, to conduct a comprehensive national
survey of data regarding the quality of aquatic sediments in the U.S.

       In September 1997, EPA's Office of Science and Technology within the Office of Water
published the first biennial Sediment Quality Report to  Congress, entitled the Incidence and Severity of
Sediment Contamination in the Surface Waters of the United States. The report consisted of three
volumes:

       Volume 1:  The National Sediment Quality Survey (U.S. EPA 19971);
       Volume 2:  Data Summaries for Areas of Probable Concern (U.S. EPA 1997J); and,
       Volume 3:  The National Sediment Contaminant Point Source Inventory (U.S. EPA 1997k).

       The National Sediment Quality Survey (NSQS) (U.S.  EPA 1997i)  describes the accumulation of
chemical contaminants in river, lake, ocean, and estuary bottoms and includes a screening assessment of
the potential for associated adverse  effects on human and environmental health. Key findings of the
NSQS are discussed in Chapter II.
 Page IH-8
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                                                                                  Chapter III
                                                                Major Programs and Activities
       In developing the NSQS, EPA compiled all available computerized data on the quantity,
chemical and physical composition, and geographic location of pollutants in sediment.  The database is
referred to as the National Sediment Inventory (NSI) and is the largest set of sediment chemistry and
related biological data ever compiled by EPA. The NSI will be updated on a regular basis in order to
assess trends in both sediment quality and the effectiveness of existing regulatory programs at the
Federal, State, and local levels. The NSI is discussed further in Chapter IV.

       The EPA's mandate to investigate sediment contamination in the Nation's water included a
directive to identify potential pollutant sources. Volume 3 of the Sediment Quality Report to Congress
(U.S. EPA 1997k) evaluated point sources (i.e., direct discharges to waterbodies).  In future biennial
Reports to Congress, EPA will assess loadings from non-point sources, including harvested croplands,
urban areas, atmospheric deposition, and abandoned and inactive mine sites (U.S. EPA 1997i). To
prepare the non-point source inventory for the second Sediment Quality Report to Congress, EPA is
currently compiling data from the Bureau of the Census, the U.S. Department of Agriculture, the U.S.
Department of the Interior's U.S. Geological Survey and Bureau of Mines, and others.

Contaminated Sediment Management Strategy

       The EPA is using data compiled for the Sediment Quality Report to Congress and other resources
for a multiprogram, multimedia effort to coordinate and streamline contaminated sediment management
decisions within the Agency. In April 1998, EPA's Office of Water completed the Contaminated
Sediment Management Strategy (U.S. EPA 1998d), which outlines the following specific actions:

1.      Control sources of sediment contamination and prevent the volume of contaminated sediment
       from increasing;

2.      Reduce the volume of existing contaminated sediment;

3.      Ensure that sediment dredging and dredged material disposal are managed in an environmentally
       sound manner; and,

4.      Develop scientifically sound sediment management tools for use in pollution prevention, source
       control, remediation, and dredged material management.

       The Contaminated Sediment Management Strategy identifies atmospheric deposition as an
important source of sediment contamination. Specifically, the strategy directs EPA's Office of Air and
Radiation to use the National Sediment Inventory (NSI) to evaluate the contribution of atmospheric
deposition to sediment quality problems. This new tool will enable EPA to better assess trends in
sediment pollution, including pollution from atmospheric deposition, and focus cleanup and pollution
control activities. In addition, the strategy identifies the Agency's Great Waters program as a significant
component of its coordinated effort to address contaminated sediment problems.

       The Contaminated Sediment Management Strategy includes a research component designed to
identify relationships between sediment contaminants and the viability and sustainability of benthic
ecosystems. Ultimately, the research will help to formulate source control and pollution prevention
strategies. In addition, the strategy outlines coordinated, multiprogram efforts of research and policy
development to ensure that uniform exposure and effects assessment procedures for contaminated
sediments are used throughout the Agency. For example, EPA proposed, and is currently developing,
standard sediment toxicity test methods and chemical-specific sediment quality guidelines.  The strategy
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Chapter III
Major Programs and Activities
proposes several specific uses of the assessment procedures and sediment quality guidelines, and the
Agency has begun to develop an Equilibrium Partitioning Sediment Guidelines User's Guide.

Waste Minimization National Plan

       The Waste Minimization National Plan (WMNP), which EPA's Office of Solid Waste developed
in 1994, is a voluntary, long-term effort to reduce the quantity and toxicity of hazardous waste through
source reduction and recycling, including wastes bearing Great Waters pollutants of concern such as
mercury and dioxin. The plan calls for a 50 percent reduction in the presence of the most persistent,
bioaccumulative, and toxic (PBT) chemicals in hazardous waste by 2005 compared to a baseline year of
1991. This goal was also adopted as a Government Performance and Results Act (GPRA) measurement
goal.

       To assist in implementing the WMNP, the Office of Solid Waste and the Office of Pollution
Prevention and Toxic Substances have developed a draft Windows-based software tool to prioritize PBT
chemicals for waste minimization efforts.  The Waste Minimization Prioritization Tool (WMPT)
provides a screening-level assessment of potential chronic risks that chemicals, including most Great
Waters pollutants of concern, pose to human health and the environment, based on their persistence,
bioaccumulative potential, and human and ecological toxicity.  More information about the WMPT can
be found on EPA's waste minimization home page at www.epa.gov/wastemin.

       The WMPT served as a starting point in developing the draft Resource Conservation and
Recovery Act PBT Chemicals List (63 FR 60332, November 9, 1998). Other factors, such as quantity,
prevalence, environmental presence, and degree of concern to the RCRA program, were used in the
selection of chemicals for the draft list. The final list of chemicals is expected to be published in the
Federal Register in 2000. This final list will serve to focus national waste minimization efforts and track
progress toward the 2005 reduction goal.

Air Characteristic  Study

       The Air Characteristic Study currently being conducted by EPA's Office of Solid Waste
addresses the question of whether some industrial wastes should be classified as hazardous because of
risks posed by their air emissions. The overall goal of this study is to estimate the maximum waste
constituent concentrations that could be present in certain waste management units and still be protective
of human health.

       The study is estimating potential risk to humans for 105 chemical constituents, of which 88 are
HAPs under the CAA and several are Great Waters pollutants of concern (e.g.,  lead compounds,
mercury, benzo[a]pyrene, dioxin, and others). Draft results of the risk analysis indicate that volatile toxic
chemicals managed hi non-storage tanks, such as aerated wastewater treatment tanks, pose the highest
risk, with the waste concentrations for these aerated tanks differing from other units by an order of
magnitude or more.  Storage tanks, land application units, landfills, and waste piles followed aerated
tanks in ranking of risk.  The findings of this study, due to be completed in 2000, will assist EPA in
exploring the need for regulatory changes under RCRA for these waste management units and in
investigating possible options for risk reduction.
Page IH-10
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                                                                                    Chapter III
                                                                 Major Programs and Activities
 HAZARDOUS AIR POLLUTANT  (HAP) CONTROLS

        Under the CAA, EPA is required to regulate sources of 188 listed HAPs.  All but two of the
 pollutants identified as Great Waters pollutants of concern are listed as HAPs. (The two Great Waters
 pollutants that are not HAPs are nitrogen and dieldrin.)  On July 16,  1992, EPA published a list of 174
 industry groups (known as source categories) that emit one or more of these air toxics. For listed
 categories of "major" sources (those with the potential to emit 10 tons/year or more of a listed pollutant
 or 25 tons/year or more of a combination of pollutants), the CAA requires EPA to develop standards
 under section 112(d) that require the application of air pollution reduction measures known as MACT.
 This performance-based approach requires EPA to set standards based on consideration of those controls
 in use at the best controlled facilities within an industry.

        The CAA provided a 10-year schedule in which to promulgate these technology-based standards
 with certain standards being promulgated in the first 2 years, 25 percent in the first 4 years, an additional
 25 percent no later than the 7th year, and the remaining 50 percent no later than the 10th year. The EPA
 has been productive in fulfilling these statutory requirements and, working in partnership with States, has
 built the necessary infrastructure for implementing the air toxics regulations.  For the 45 source
 categories in the 2- and 4-year groups, EPA estimates that the regulations will reduce air toxics emissions
 by approximately one million tons per year. For the 42 source categories in the 7-year group, EPA has
 either proposed or promulgated regulations that are estimated to reduce air toxics emissions by roughly
 500,000 tons per year. A list of all source categories, the MACT implementation schedule, and
 references to proposed and final rules is included in Appendix C of the Residual Risk Report to Congress
 (U.S. EPA 1999d).

        Some regulations are already in place under section 112(d) with sources currently in compliance.
 The source categories affected by these rules are listed in Table III-l  below along with the emission
 reductions of the affected pollutants of concern, where available.

                                          Table 111-1
                    Source Categories With Effective Compliance Dates
                       and Anticipated Reductions of HAP Emissions
Source Category
Coke oven batteries: Charging, leaks,
and bypass/bleeder stacks
Secondary Lead Smelting
Compliance
Date
01/01/98
12/23/97
Pollutant
Coke oven
emissions3
All HAPsb
Lead Compounds
Nationwide
Pre-MACT
Emissions
(tpy)
1600
1900
120
Nationwide
Expected
Percent
Reductions
94
65
40
 L.OKB oven emissions include HUM.
  HAP emissions for this category include lead compounds, dioxins/furans, mercury, and POM among other
pollutants.  Of these, lead compounds is the only pollutant of concern for which pollutant-specific estimates are
available.

        Section 112(c)(6) of the CAA directs EPA to focus attention on seven specific toxic pollutants -
all of which are Great Waters pollutants of concern: alkylated lead compounds, hexachlorobenzene,
POM, mercury, PCBs, dioxins, and furans. The Agency is to ensure that sources accounting for at least
90 percent of the emissions of each of these pollutants are subject to standards under section 112(d)
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter III
Major Programs and Activities
(described above).  Section 112(c)(6) of the CAA requires EPA to identify the source categories that emit
90 percent of the aggregate emissions for each of the seven specific pollutants and add any source
categories not previously identified to the list discussed above.

       Under section 112(c)(6), a review of the available data indicated that nearly all source categories
emitting the seven pollutant groups had akeady been listed for regulation under the CAA or were subject
to comparable regulation under other CAA authorities.  However, two additional source categories were
added to the source category list in a final Federal Register notice on April 3, 1998. These two
categories are open burning of scrap tires and gasoline distribution (Stage I Aviation), which includes
evaporative losses associated with the distribution and storage of aviation gas containing lead. A
comment and response document is available along with the 1990 emissions inventory for the seven
pollutants at www.epa.gov/ttn/uatw/l 12c6/l 12c6fac.html.

       A different section of the CAA (section 129) is devoted to control of certain air toxics, as well as
other pollutants, from solid waste combustion units. The pollutants of concern to the Great Waters
covered are lead, cadmium, mercury, dioxins and rarans, and NOX This regulatory program is discussed
later in this section.

       Under sections 112 and 129, several rules have either been proposed or finalized, but the
compliance date has not yet been reached.  A summary of these actions and their anticipated emission
reductions are listed below in Table III-2. In addition, under the joint authority of section 112 and the
Resource Conservation and Recovery Act (RCRA), EPA's Office of Solid Waste finalized on July 30,
1999 (signed by the Administrator) new emission standards for existing and new cement kilns,
incinerators, and lightweight aggregate kilns that burn hazardous wastes.  These combustors burn about
80 percent of the hazardous waste combusted annually within the U.S.  When fully implemented in 2002,
the MACT standard for these sources is expected to achieve significant reductions in emissions of
several Great Waters pollutants of concern, including dioxin/furans, mercury, lead and cadmium. These
standards will also satisfy our obligation under RCRA to ensure that hazardous waste combustion is
conducted in a manner adequately protective of human health and the environment.

       The remaining 50 percent of MACT regulations are expected to be issued within the next 2 years
(by 2002).  Based on our current knowledge of the remaining industries slated for regulation under
section 112(d),  those that emit pollutants of concern to the Great Waters include chlorine manufacturing
(chlor-alkali plants), coke ovens (pushing,  quenching and battery stacks), industrial boilers, institutional
and commercial boilers, iron and steel, and refractory manufacturing.  There are more MACT rules for
solid waste combustion under section 129 noted later hi this section.

        In addition to the standards development requirements of the CAA, there are a number of other
HAP program requirements that will help reduce emissions of the Great Waters pollutants of concern.
These are briefly described below. Additional information regarding the air toxic program can be  found
on the Internet at EPA's unified air toxics web site at www.epa.gov/ttn/uatw.

Mercury Study Report to Congress

        The Mercury Study Report to Congress, issued by EPA in December 1997 (U.S. EPA1997e), is a
comprehensive document detailing the U.S. mercury emissions inventory, fate and transport of mercury
in the environment, human health effects, an ecological risk assessment, a human and wildlife risk
characterization, and an assessment of control technologies and their costs.  The report also outlines
research needs. Pertinent results and conclusions from this report are described in the mercury and
compounds section of Chapter 2.
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                                                                             Chapter III
                                                            Major Programs and Activities
                                       Table III-2
                Proposed and Final Rules Affecting Pollutants of Concern
Source Category
Municipal waste combustion
(large combustors, > 250 tons
per day)
Medical waste incineration
Pulp and paper cluster0
Primary aluminum production
Secondary aluminum production
Primary copper production
Pesticide active ingredient
production6
Portland cement manufacturing -
nonhazardous waste -fired
Mineral wool production
Hazardous Waste combustion
(existing and new cement kilns,
incinerators, and lightweight
aggregate kilns that burn
hazardous waste)
Status
Final rule and guidelines
Final rule and guidelines
Final rule
Final rule
Final rule
Proposed rule
Final rule
Final rule
Final rule
Final rule
Pollutants
Dioxins/Furans3
Mercury1
Lead
Cadmium
NOX
Dioxins/Furans3
Mercury
Lead
Cadmium
NOX
HAPs
POM
HAP metalsd
Dioxins/Furansa
Cadmium
Lead
Mercury
HAPs8
Dioxins/Furans3
Mercury
HAP metals'
HAP metals9
Dioxins/Furans3
Mercury
Lead and
Cadmium
Other HAP
Metalsh
Nationwide
Pre-MACT
Emissions
(tpy)
0.0025
54
64
4.2
54,000
0.0002
16
12
1.3
1,300
240,000
2,000
64.4
0.0009
0
140
0
4,255
0.0005
4
t
1.1
.000044
6.5
88.5
9.8
Nationwide
Expected
Percent
Reductions
98
78
75
67
36
95-97 b
93-95 b
80-87 b
75-84 b
0-30 b
58
50
62.5
86.6
0
13
0
65
36
0
f
91
70
55
88
75
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter m
Major Programs and Activities
                                     Table 111-2 (continued)
                 Proposed and Final Rules Affecting Pollutants of Concern
'Dioxin/Furan emissions are reported on a 2,3,7,8-TEQ basis.
b Ranges reflect different assumptions on the number of incinerator closures.
0 Values represent air emissions affected by the cluster rule only. Values for individual HAPs were not provided in
the final rule.
d The HAP metals for secondary aluminum production are mercury, lead, and cadmium, as well as eight other HAP
metals.
c This rule covers 11 of the source categories listed for regulation.  Values for individual HAPs are not available.
Included are emissions of HCB and chlordane, although they are not the most prevalent HAPs in this category.
'The rule includes a particulate matter limit, which serves as a surrogate for all non-volatile and semi-volatile HAPs,
including metals. These metals are estimated to be no more than  1 percent of the total particulate matter HAPs.
The rule is estimated to achieve about 20 percent reduction in particulate matter emissions.
9The HAP metals for mineral wool production are cadmium and lead, as well as seven other HAP metals.
h The other HAP metals for hazardous waste combustion include antimony, cobalt, manganese, nickel, and
selenium.
' Emission reductions for municipal waste combustion are often cited from a 1990 baseline, other than the pre-MACT
baseline presented here.  For example, the rule and guidelines will reduce mercury emissions by greater than 90
percent from 1990 levels when fully implemented.

        The Mercury Study Report to Congress is not a regulatory effort; currently it is being broadly
used in support of Great Waters activities, the PBT Initiative, the Binational Toxics Strategy, the mercury
research strategy, and other EPA efforts to understand and control this pollutant.

Utility Air Toxics Study and Regulatory Determination

        In February 1998, EPA issued a study of the public  health impacts of emissions of air toxics from
utilities that burn fossil fuel (U.S. EPA 1998p). About 67 air toxics were found to be emitted from
utilities, including mercury and dioxins. The report includes (1) a description of the utility industry; (2)
an analysis of air toxics emissions data from coal-, oil-, and gas-fired utility plants; (3) an assessment of
risks to public health from exposure to air toxics emissions through inhalation; (4) an assessment of
potential risks to public health from exposure to four specific air toxics (i.e., radionuclides, mercury,
arsenic, and dioxins) through other indirect means of exposure (e.g., food ingestion, dermal absorption);
(5) a general assessment of the fate and transport of mercury through environmental media; and, (6) a
discussion of alternative control strategies.

        The report indicates that, although uncertainties in the analysis exist,  on balance, mercury from
coal-fired utilities is the HAP of greatest potential public health concern. The report identifies three
other air toxics for which there are some potential concerns  and uncertainties that may need further
study:  dioxins, arsenic, and nickel.

        The CAA also requires EPA to make  a determination, after considering the results of the utility
study,  as to whether emission controls for air toxics are appropriate and necessary for utility boilers. The
EPA has delayed this determination until it collects additional information, and EPA's Office of Air and
Radiation is currently collecting the following mercury emissions data from electric utility steam
generating units:

•       Current information on the type of coal they use and on their method of particulate matter (PM)
        and sulfur dioxide (SO2) control at all "traditional" coal-fired electric utility steam generating
        units;

•       Current information on the fuel they use and on their method of PM and SO2 control at all
        independent power producers that could be identified as possibly burning coal;
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                                                                                    Chapter III
                                                                 Major Programs and Activities
 •      1 year of mercury-in-coal analyses at all coal-fired units meeting the section 112(a)(8) definition
        of "electric utility steam generating unit"; and

 •      One series of speciated mercury emissions testing at a randomly selected subset of coal-fired
        units.

 The regulatory determination is scheduled to be provided by December 15, 2000 (U.S. EPA 1998p).

 Residual Risk Report to Congress

        Under section 112(f) of the CAA, EPA is required to develop and implement a program for
 assessing risks remaining (i.e., the residual risk) after facilities have implemented MACT standards, and
 to promulgate rales, if necessary, to protect the public health with an "ample margin of safety" or to
 prevent adverse environmental effects.  Additional risk-based regulations, if needed, are to be
 promulgated within 8 years after EPA promulgates an air toxics standard for a given source category.
 The first such risk-based regulations, if necessary, are due in 2002. If promulgated, residual risk
 standards could further reduce emissions of Great Waters pollutants of concern.

        In March 1999, EPA issued the Residual Risk Report to Congress. This report reviews EPA
 human and ecological risk assessment methods, identifies data sources and data collection needs for
 conducting risk assessments, proposes methods on how to close data gaps, discusses how results of
 residual risk assessments will be used in the residual risk program, and includes an appendix of all
 MACT source categories, the MACT implementation schedule, and references to proposed and final
 rales.  In addition, the report discusses the strategy or "framework" EPA will use in conducting residual
 risk assessments.

        The risk assessment framework under the residual risk program was developed using knowledge
 gained from past risk assessments and information from other regulatory agencies and guidance from
 reports. This strategy calls for an iterative, tiered assessment of the risks to humans and  ecological
 receptors through inhalation and, where appropriate, non-inhalation exposures to air toxics. The residual
 risk assessment framework will allow the Agency to be flexible in its decisions while ensuring that
 public health and the environment are protected. The EPA's objectives also include integration of all
 portions of the Federal air toxics program, continuing the partnership with State/local programs in the
 sharing of data and expertise, and including groups who may be affected by residual risk decisions (e.g.,
 industry, public interest groups) as part of the process.

 Integrated  Urban Air Toxics Strategy and Report  to Congress

       As part of its overall efforts to reduce air toxics, EPA published the integrated urban air toxics
 strategy in the Federal Register on July 19, 1999 (64 FR 38706). The strategy presents a framework for
 addressing air toxics in urban areas as required by section 112(k) of the CAA. The goals of the strategy
 are to reduce by 75 percent the risk of cancer and substantially reduce non-cancer risks associated with
 air toxics while ensuring that disproportionate risks are addressed.  Specifically, the strategy does the
 following:

       Outlines EPA's approach for assessing health risks. The EPA will evaluate risks considering the
       multiple sources of air toxics  in our cities, whether they come from major industrial sources,
       smaller sources (like drycleaners or gas stations), or cars and tracks.  This includes risks from
       consuming fish from waters contaminated by urban air toxic deposition.
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Chapter HI
Major Programs and Activities
•      Builds on the substantial emission reductions already achieved from cars, trucks, fuels, and
       industries such as chemical plants and oil refineries. The strategy outlines actions to reduce
       emissions of air toxics and to improve EPA's understanding of the health risks posed by air
       toxics in urban areas.

•      Identifies a list of the 33 air toxics that pose the greatest threat to public health in urban areas,
       considering multipathway exposure, such as fish consumption, in the identification process.
       These 33 air toxics are a subset of the 188 air toxics and include the Great Waters pollutants of
       concern mercury, cadmium, lead, dioxins and furans, POM, PCBs, and HCB.

•      Identifies the 30 of these 33 urban air toxics with the greatest contribution from smaller
       commercial and industrial operations or so-called "area " sources.  The CAA requires EPA to
       ensure that 90 percent of the aggregate emissions of each of the 30 identified HAPs are subject to
       regulation through EPA's established air toxics program. In order to address this requirement,
       EPA identified 29 area source categories that are significant contributors to the emissions,
       including sources of mercury, cadmium, lead, POM, dioxins and furans. Currently, EPA has
       regulations under development or completed for 16 of these area source categories and intends to
       develop regulations for the remaining 13 area source categories over the next 5 years.  The EPA
       intends to list additional area sources by 2003 as better inventory data become available.

       The strategy also addresses the Agency's efforts to date to  assess the public health risk from air
toxics from mobile sources and highlights EPA's expectation for additional regulations targeting toxics
emissions from motor vehicles and fuels. In the strategy, EPA describes plans to consider diesel
emissions in the upcoming mobile source air toxics regulation and  to issue a rule (the proposed "Tier II
rule"; see page 111-29) which will reduce levels of diesel emissions significantly in both urban and rural
areas.

Rules for Solid Waste Combustion, Including Large Municipal
Waste Combustors and Hospital/Medicdl/Infectious Waste
Incinerators (CAA Section 129)

         Section 129 of the CAA directs EPA to control solid waste combustion and set emission limits
for dioxins and furans, cadmium, lead, mercury, and NOX (all pollutants  of concern to the Great Waters),
as well as particulate matter, opacity, sulfur dioxide, carbon monoxide, and hydrogen chloride. For
existing solid waste combustion units, section 129 requires EPA to develop emission guidelines. These
guidelines do not directly regulate the units. Rather, they establish requirements for State plans, which
are the vehicle by which States implement the guidelines. For new units, section 129 requires EPA to
develop technology-based performance standards following section 111  of the CAA.  Section 129
further subjects solid waste combustion units to the section 112(f) residual risk program, which was
discussed earlier in this section.

       Final rules are now in place for large municipal waste combustors (MWC) and for
hospital/medical/infectious waste incinerators (HMIWI, or often called medical waste incinerators).
There are also rules under development for small municipal waste  combustors, commercial/industrial
waste incineration, and other solid waste incineration.  The commercial/industrial waste incineration rule
is planned to be finalized by November 15, 2000; the small municipal waste combustor rule is planned to
be finalized by 2001.
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                                                                                  Chapter III
                                                                Major Programs and Activities
       Large MWC are those units with a capacity of at least 250 tons of waste per day.  The EPA
initially promulgated standards for new units and guidelines for existing units on December 19, 1995 and
revised them on August 25, 1997. The 24 States with large MWCs were required to submit emission
guidelines implementation plans to EPA by December 19, 1997. The State plans include source and
emission inventories, testing and monitoring, as well as generic or site-specific compliance schedules.
The MWC Federal Plan adopted in November 1998 applies to large MWCs until State plans are
approved. The Federal Plan ensures that large MWCs are on track to complete pollution control
equipment retrofit schedules to meet the final compliance date of December 19, 2000. The emission
guidelines affect 70 large MWCs and will reduce toxic air pollutant emissions by 112,000 tons per year.
Table III-2 provides the nationwide emission estimates and expected percent reductions for pollutants of
concern to the Great Waters. The control equipment expected to be used at a typical existing plant
reduce dioxin emissions by 99 percent, mercury emissions by over 90 percent, NOX emissions by 40
percent, and will sharply reduce other air pollutants like lead and cadmium, as shown in Table III-3.

                                         Table 111-3
              Emission  Reductions Expected from Control Equipment Used
                          to Retrofit A Typical Existing MWC Plant
Pollutant
Dioxin/furan (ng/dscm) total mass
Particulate matter (mg/dscm)
Cadmium (mg/dscm)
Lead (mg/dscm)
Mercury (mg/dscm)
Sulfur dioxide (ppmv)
Hydrochloric acid (ppmv)
NOX (ppmv)
Typical
Uncontrolled Level
1,000
3,700
1.2
25
0.65
160
500
225
Typical
Controlled Level
3
4
0.001
0.01
0.02
5
10
130
Percent Reduction
99+
99+
99+
99+
90+
90+
95+
40+
   Source: U.S. EPA 1998h

       For HMIWI, the emission guidelines and performance standards were published in the Federal
Register in September 1997. The guidelines will apply to about 2,400 existing HMIWI; full compliance
with them is no later than September 2002. In addition, EPA developed a new source performance
standard (NSPS) that applies to new HMIWI that commence construction after June 20, 1996 or that
commence modification after the effective date of the NSPS (i.e., 6 months after promulgation). In the
first 5 years after promulgation, the NSPS are expected to apply to about 10 to 70 new HMIWI. The
pollutants addressed, regulatory baseline emissions, and expected reductions of the emission guidelines
and the NSPS are presented in Tables III-4 and III-5, respectively.

STATIONARY SOURCE CONTROLS  ADDRESSING NOX

       The CAA provisions specifically addressing NOX have had the greatest effect on controlling
stationary source nitrogen compound emissions. Primarily because of these provisions, nationwide NOX
emissions are projected to decrease gradually for the next few years, ultimately leveling off at around 19
million metric tons per year around 2005, representing a decrease from the 1996 level of around 21.2
million metric tons/year (U.S. EPA 19981). Nitrogen oxide emissions are projected to remain at about
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page 111-17

-------
Chapter HI
Major Programs and Activities
that level through 2010. Figure III-l indicates projected trends in NOX emissions through 2010. The
EPA plans to update these projections in 2000 using newer models for mobile and stationary sources.
Among other benefits, these reductions will reduce rates of atmospheric nitrogen deposition affecting the
Great Waters.

        This section summarizes recent developments in key CAA programs that have recently or will in
the near future reduce NOX emissions from stationary sources.  It lists and briefly describes, in Table III-
6, CAA regulatory controls that will result in NOX emission reductions. It also presents the sources
affected, compliance dates, and the emission reductions that each regulation is expected to achieve.
Finally, the section discusses the effect on NOX emissions of possible new 8-hour ozone and PM25
standards, as well as the regional haze rule.

                                           Table  111-4
                    Emission Reductions Expected from Existing HM1WI
Pollutant
Participate matter (Mg/yr)
Carbon monoxide (Mg/yr)
Total Dioxin/Furanb (g/yr)
Dioxin/Furan TEQb (g/yr)
Hydrochloric acid (Mg/yr)
Sulfur dioxide (Mg/yr)
NO, (Mg/yr)
Lead (Mg/yr)
Cadmium (Mg/yr)
Mercury (Mg/yr)
Baseline
Emissions
940
460
7,200
148
5,700
250
1,200
11
1.2
14.5
Nationwide Emission
Reduction
820-870
340-380
6,900-7,000
141-143
5,600
0-74
0-350
8.6-9.4
0.91-1.0
13.5-13.8
Nationwide Emission
Reduction (percent)3
88-92
75-82
96-97
95- 97
98
0-30
0-30
80-87
75-84
93-95
* These reductions represent reductions from the regulatory baseline.  Percent reductions have been calculated
based on the actual (unrounded) values for baseline emissions and nationwide emissions reduction.
b Total dioxin/furan reflects total tetra- through octa-chlorinated dibenzo-p-dioxins and dibenzofurans, as measured
by EPA Reference Method 23.  TEQ reflects the toxic equivalent quantity of 2,3,7,8-tetrachlorinated dibenzo-p-dioxin
using international toxic equivalency factors.
Source: U.S. EPA 1998g
Page 111-18
Deposition of Air Pollutants to the Great Waters - 3  Report to Congress 2000

-------
                                                                                      Chapter III

                                                                   Major Programs and Activities
                                           Table 111-5

   Emission Reductions Expected at New HMIWI after 5 Years of NSPS Implementation
Pollutant
Particulate matter (Mg/yr)
Carbon monoxide (Mg/yr)
Total Dioxin/Furanb (g/yr)
Dioxin/Furan TEQb (g/yr)
Hydrochloric acid (Mg/yr)
Sulfur dioxide (Mg/yr)
NO, (Mg/yr)
Lead (Mg/yr)
Cadmium (Mg/yr)
Mercury (Mg/yr)
Baseline Emissions
28
14
47
1.1
64
28
130
0.39
0.051
0.21
Nationwide Emission
Reduction
23-25
0-7.0
35-41
0.80-0.93
61-62
0-15
0-69
0.33-0.36
0.042-0.046
0.10-0.16
Nationwide Emission
Reduction (percent)3
85-92
0-52
75-87
74-87
95-98
0-52
0-52
85-92
83-91
45-74
  These reductions represent reductions from the regulatory baseline. Percent reductions have been calculated

based on the actual (unrounded) values for baseline emissions and nationwide emissions reduction.

b Total dioxin/furan reflects total tetra- through octa-chlorinated dibenzo-p-dioxins and dibenzofurans, as measured

by EPA Reference Method 23. TEQ reflects the toxic equivalent quantity of 2,3,7,8-tetrachlorinated dibenzo-p-dioxin

using international toxic equivalency factors.

Source: U.S. EPA 1998J
                                           Figure III-1

                     Projected National NOX Emission Trends, 1996-2010

                                        (U.S. EPA 19981)
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Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
            Page 111-19

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                                                                                    Chapter III
                                                                 Major Programs and Activities
 Acid Rain Program NOX Reduction

        Title IV of the CAA requires reductions in NOX emissions from the electric power generating
 industry.  The acid rain NOX requirements incorporate a two-phased strategy to reduce NOX emissions
 from boilers. In the first phase, which became effective January 1, 1996, certain Group 1 boilers (i.e.,
 dry-bottom wall-fired boilers and tangentially-fired boilers) were required to comply with specific NOX
 emissions limitations.10 All additional Group 1 boilers must comply in the second phase, which became
 effective on January 1, 2000. Also included in the second phase are NOX emissions limits for all Group 2
 boilers (i.e., wet-bottom wall-fired boilers, cyclones, boilers using cell-burner technology, and vertically-
 fired boilers).11

        In April 1995, EPA promulgated the rale establishing NOX emission limits for Group 1 boilers.
 These regulations also allowed Phase II Group 1 units to use an "Early Election" Compliance Option.
 Under this regulatory provision, Phase II Group 1 NOX affected units can demonstrate compliance with
 the higher Phase I limits for their boiler type from 1997 through 2007 and not  meet the more stringent
 Phase II limits until 2008. If the utility fails to meet this annual limit for the boiler during any year, the
 unit is subject to the more stringent Phase II limit for Group 1 boilers beginning in 2000 or the year
 following the exceedance, whichever is later.  As a result of these rales, NOX reductions were projected
 to be approximately 400,000 tons per year in 1996 through 1999 (Phase I) and 2,060,000 metric tons per
 year in 2000 and subsequent years (Phase II).

 NOX SIP Call, Section  126  Petitions, and Federal  Implementation
 Plans

        Many States have found it difficult to attain the ozone national ambient air quality standard
 (NAAQS) because of widespread regional transport (i.e., from sources in other States) of ozone and its
 precursors, NOX and volatile organic compounds (VOCs). In 1995, the Ozone Transport Assessment
 Group (OTAG) was formed to address the regional transport problem in the eastern half of the U.S. (i.e.,
 the 37 easternmost States). The OTAG process was a  collaborative effort among 37 affected States, the
 District of Columbia, EPA, and interested members of the public, including  environmental groups and
 industry representatives. The OTAG concluded that further regional reductions in NOX emissions are
 needed to reduce the transport of ozone and its precursors. Furthermore, OTAG recommended in July
 1997 that major sources of NOX emissions (i.e., utility  and other stationary sources) be controlled under
 State NOX budgets and that an emissions trading program be developed.

        In response to  the OTAG recommendations, EPA issued the NOX State implementation plan
 (SIP) call  on October 27, 1998 (63 FR 57356). The SIP call limits  summer season NOX emissions for 22
 States and the District  of Columbia that are significant contributors to ozone in downwind areas. The
 EPA directed the 23 jurisdictions to amend their SIPs to ensure that the NOX budgets are met. The EPA
 set these budgets by assessing the reductions that could be obtained through cost-effective controls on
 electricity generating units and large industrial boilers. However, in order to meet the SIP requirements,
10 The affected dry-bottom wall-fired boilers must meet a limitation of 0.50 Ibs of NOX per mmBtu averaged over
the year, and tangentially-fired boilers must achieve a limitation of 0.45 Ibs of NOX per mmBtu averaged over the
year.

11 The limits are 0.68 Ib/mmBtu for cell burners, 0.86 Ib/mmBtu for cyclones greater than 155 MWe, 0.84 Ib/mmBtu
for wet-bottom boilers greater than 65 MWe, and 0.80 Ib/mmBtu for vertically-fired boilers.

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Chapter HI
Major Programs and Activities
States can adopt NOX trading programs. These programs will be similar to the successful SO2 trading
program under EPA's Acid Rain program. The NOX SIP call is expected to reduce atmospheric nitrogen
emissions by up to 1.05 million tons per ozone season, which should reduce loadings into the Great
Waters in the eastern U.S. [NOTE: In March 2000, in response to arguments made before the court, the
Circuit Court of Appeals for the District of Columbia removed Wisconsin and portions of Georgia and
Missouri from the list of States subject to the call. The emission reduction estimate will be slightly less
with these removals.]

       At the same time that EPA promulgated the NOX SIP call rule, EPA also proposed that NOX
Federal implementation plans (FIPs) may be needed if any State fails to respond to the final NOX SIP call.
In addition, a number of northeastern States petitioned EPA, as allowed by section 126 of the CAA, to
address air pollution transported from upwind States and requested that EPA make a finding  that NOX
emissions from certain major stationary sources significantly contribute to ozone nonattainment
problems. Such a finding would require EPA to establish Federal emissions limits for these sources.  On
April 30, 1999, EPA took final action on the petitions and identified upwind sources that significantly
contribute to ozone nonattainment problems. In December 1999, EPA revised the April 126  petition rule
in light of the rulings by the DC Circuit Court of Appeals related to the NOX SIP call and the 8 hour
ozone standard. The FIPs and the section 126 petition action would directly impose regulatory
requirements on these emissions sources, including a capped, market-based trading program  for certain
stationary sources.

New Source Performance Standards

       New source performance standards (NSPS) require emission reductions in both attainment and
nonattainment areas.  Section 111 of the CAA requires EPA to identify "source categories" emitting
criteria air pollutants (e.g., ozone) or precursors of criteria pollutants (e.g., NOX and VOCs) and to
establish emissions limits for new, modified, and reconstructed sources of emissions.12 Emissions limits
must be based on the "best demonstrated technology," and must apply to all new sources in the country
after the effective date of the rule. To date, EPA has promulgated approximately 100 NSPS, of which
approximately ten directly control NOX emissions.

        In September 1998, under court order, EPA finalized an NSPS for fossil fuel-fired utility and
industrial boilers. Specifically, the final standards revised the NOX emission limits for electric utility,
industrial, commercial, and institutional steam generating units for which construction, modification, or
reconstruction commenced after July 9,1997. These final revised NOX emission limits will reduce the
projected growth in NOX emissions from new sources by approximately 42 percent (41,500 metric
tons/year) from levels allowed under current standards.

New Source Review and RACT

        Under the CAA, States must apply similar requirements to major stationary sources  of NOX
emissions as are applied to major stationary sources of VOCs because these two pollutants are precursors
to ozone. These new NOX provisions require (1) existing major stationary sources to apply reasonably
available control technology (RACT) in certain ozone nonattainment areas and ozone transport  regions,
(2) new or modified major stationary sources to offset increased emissions and to install controls
representing the lowest achievable emission rate (LAER) in areas that do not attain the ozone NAAQS
 12 Few sources emit ozone; rather it is formed in the atmosphere through the reaction of VOCs and NOX.  To attain
 the ozone standard, States typically require VOC and NOX controls.

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                                                                                  Chapter III
                                                                Major Programs and Activities
 (i.e., ozone nonattainment areas) and ozone transport regions, and (3) new or modified major stationary
 sources to install the best available control technology (BACT) in ozone and NO2 attainment areas.

 MOBILE SOURCE PROGRAM ACTIVITIES

        Collectively, mobile sources are major contributors of nitrogen compounds to the atmosphere.
 The EPA's Office of Mobile Sources (QMS) is responsible for regulatory oversight of air pollution
 emitted from mobile sources, primarily automobiles, but also including marine, aircraft, locomotive, and
 small engines such as lawn and garden equipment. The regulatory strategies often focus on both vehicle
 emissions and fuel composition.

        Historically, OMS has led the effort to eliminate lead from gasoline and require more stringent
 tailpipe emissions and fuel changes that benefit air quality. Recent accomplishments by OMS that affect
 Great Waters pollutants of concern are focused primarily on nitrogen compounds. These include the
 following.

        Between 1994 and 1996, OMS phased in Tier I tailpipe emission standards affecting light-duty
        vehicles and trucks.  The EPA expects the standards to reduce NOX emissions by 850,000 metric
        tons per year by 2010.  The Tier II tailpipe emission standards, which will further limit
        emissions, were proposed on May 13, 1999 and, if finalized, will reduce NOX emissions by an
        additional 2.8 million tons by 2030 (see below and the Federal Register at 64 FR 26004, May 13
        1999).

 •       The national low emission vehicle, or NLEV, standard begins with model year 1999 vehicles in
        the Northeast Ozone Transport Region and throughout the Nation in 2001. Compliant vehicles
        will meet California emission standards and will reduce NOX emissions by 181,000 metric tons
        per year by 2007.

 •       Recent regulations for heavy-duty highway diesel engines will result in one million metric tons
        per year reductions in NOX emissions by 2020.  Heavy-duty non-road diesel standards covering
        construction, agricultural, and industrial engines will be phased in between model years 1999 and
        2006 and will result in reductions of 1.1 million metric tons per year of NOX by 2010.

 •       New regulations covering small spark-ignition engines will reduce NOX emissions by 9,000
        metric tons per year in 2020.

 •       New requirements for locomotive engines, both new and rebuilt, will come into effect in 2000
        and result in NOX reductions of 449,000 metric tons per year by 2010.

 Tier II Emission Standards for Vehicles and Gasoline Sulfur
 Standards for Refineries

        In December, 1999 (65 FR 6698), EPA issued new, more protective standards for tailpipe
 emissions from all passenger vehicles (including sport utility vehicles (SUVs), minivans, and pick-up
 trucks) and new standards to reduce sulfur levels in gasoline to ensure the effectiveness of low emission-
 control technologies in vehicles. These new standards were in response to EPA's July 1998 Tier II
 Report to Congress which concluded that more stringent vehicle standards are needed to meet the ozone
 and particulate matter air quality standards, and that technology would be available to meet such
 standards cost-effectively.  The EPA designed the new standards in close consultation with the auto and
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Page 111-29

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Chapter HI
Major Programs and Activities
oil industries, emissions control manufacturers, the States, and public health, consumer, and
environmental groups (U.S. EPA 1999c).

       Under the Tier II standards, SUVs, minivans, and pickup trucks are required to meet the same
protective standards as passenger cars, regardless of the type of fuel used.  The standards also reduce the
amount of sulfur in gasoline, which will ensure the effectiveness of low emission-control technologies in
vehicles and reduce harmful air pollution. When fully implemented in 2030, the new tailpipe and
gasoline standards are expected to reduce NOX emissions from vehicles by 2.8 million tons, emissions of
particulate matter (i.e., soot) by 35,000 tons, and SO2 emissions from vehicles by 334,000 tons. The
significant environmental benefits of this program are expected to come at an average cost increase of
less than $100 per car and less than $200 per light-duty truck. Consumers would pay less than 2 cents
per gallon more for gasoline, or about $100 more over the life of an average vehicle (U.S. EPA 1999c).
Additional information is available at http://www.epa.gov/otaq/tr2home.htm.

OZONE AND PM NAAQS AND THE REGIONAL HAZE RULE

       Since the Second Great  Waters Report to Congress, EPA made revisions to the particulate matter
(PM) and ozone NAAQS. In addition, in April 1999, EPA issued the final regional haze rule to address
visibility impairment in national parks and wilderness areas (also known as Class I areas) caused by
numerous sources located over broad regions.  Some  of these Class I areas are associated with Great
Waters waterbodies, such as Isle Royal National Park in Lake Superior and Swan Quarter National
Wildlife Refuge in the Albemarle-Pamlico Estuary. Implementation of the NAAQS in conjunction with
the regional haze program is anticipated to improve visibility across the country as well as reduce NOX
emissions and consequently nitrogen deposition to coastal waters, particularly in the eastern U.S.  The
EPA will have a better understanding of the NOX emission reductions resulting from these programs
when emissions and monitoring data are collected from the States, nonattainment areas are designated,
and the States submit implementation plans (U.S. EPA 1998f).

       However, on May 14, 1999, in response to a  suit by the American Trucking Associations, Inc., a
panel of the Circuit Court of Appeals for the District  of Columbia issued a decision vacating the revised
PM10 standard and stopping implementation of the new ozone standard. The U.S. Department of Justice
has appealed this decision. The court did not, however, prevent EPA from designating nonattainment
areas for the new ozone standard, and therefore EPA  is considering doing so in 2000.  For the new PM2 5
standards, which the court ruled should stay in place, EPA currently plans to designate attainment and
nonattainment areas as soon as air quality data are collected and analyzed, which is anticipated to be in
2004 or 2005.

OTHER NATIONAL PROGRAMS

Fish Contamination  Program

       The EPA's Fish Contamination Program (FCP) provides technical assistance  to States, tribes,
and  others on matters related to  persistent bioaccumulative toxics in fish and wildlife  and associated
potential health risks to consumers. Since 1992, the FCP has worked with State and tribal agencies to
establish nationally-consistent methods and protocols for assessing contaminants in fish and wildlife for
the purpose of developing and managing consumption advisories. Additional activities of the FCP
include publishing guidance documents, maintaining national databases (e.g., offish consumption
advisories), sponsoring conferences and training workshops, providing grants for advisory development
 Page m-30
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                                    Chapter III
                                                                 Major Programs and Activities
 and special studies, developing outreach materials, and assisting States and tribes in the issuance of
 consumption advisories.

        Since 1993, the FCP has published an annual report on trends in the number offish and wildlife
 consumption advisories. The National Listing of Fish and Wildlife Advisories (NLFWA) identifies all
 State-, tribal-, and Federally-issued fish consumption advisories in the U.S. Recently, it has been
 expanded to include Canadian provinces and territories. According to the 1998 NLFWA, the number of
 consumption advisories in the U.S. rose by 125 in 1997 to a total of 2,299, a 5 percent increase from
 1996. The number of waterbodies under advisory in 1997 represented 16.5 percent of the Nation's total
 lake acres and 8.2 percent of the Nation's total river miles.  The total number of advisories in the U.S.
 increased for three major pollutants - mercury, dioxin, and DDT. The increase in advisories issued by
 the States generally reflects an increase in the number of assessments of the levels of chemical
 contaminants in fish and wildlife tissues, rather than an increase in contaminant levels (U S EPA
 1998m).

 Environmental Justice Initiatives

        Research indicates that people of different racial and ethnic backgrounds and income levels often
 do not eat the same kinds and amounts of food (U.S. EPA 1995). For example, Native Americans and
 the urban poor are at a greater risk for adverse health effects due to high rates of consumption of
 potentially contaminated fish. Fetuses and young children are at risk because they are more vulnerable to
 the effects of the pollutants of concern. Thus, these subpopulations may be disproportionately affected
 by deposition of air pollutants to the Great Waters.

        The EPA recognizes the relationship between health risks, environmental pollutants, and diet as a
 potential environmental justice issue. Since 1992, EPA's Office of Environmental Justice has served as
 the point of contact for environmental justice outreach and educational activities, has provided technical
 and financial assistance, and has disseminated environmental justice information. In conjunction with
 regional and headquarters offices, this office has initiated many programs to address the environmental
 concerns among minority, low-income, and Native American and Alaska Native communities (U.S. EPA
 1995). Likewise, EPA created the American Indian Environmental Office in 1994 for the purpose of
 coordinating the EPA-wide effort to strengthen public health and environmental protection on Native
 American lands (U.S. EPA 1998u). An example of EPA's efforts is the passage of a resolution by the
 National Environmental Justice Advisory Council of EPA's Office of Environmental Justice in
 December 1998 that was developed by the Indigenous People Subcommittee pertaining to the effects of
 mercury contamination on American Indian populations. This resolution requires EPA's Office of
 Pollution Prevention and Toxic Substances to share the 1998 Mercury Action Plan with tribes, to provide
 educational and health information to tribes, to adopt a Mercury Action Plan and regulatory authority to
 eliminate anthropogenic mercury emissions by 2010,  to establish baseline emission standards, and to
 adopt enhanced reporting requirements for mercury emission sources.

       Recent studies continue to examine the relationship between increased health risks in certain
 subpopulations and the consumption offish from the Great Lakes. Study results show that some
 subpopulations are not as aware offish advisories as other populations, and that human health effects
 from consumption offish from contaminated areas vary. Chapter II describes additional relevant
 research relating to exposure and effects of Great Waters Pollutants of concern and sensitive or highly-
 exposed subpopulations.
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Chapter in
Maior Programs and Activities
Children's Health Initiatives
       Children face environmental health threats from many of the Great Waters pollutants of concern.
In addition, child exposures to pollutants tend to occur through multiple exposure routes, including
inhalation, ingestion, dermal contact, and prenatal (transplacental) exposure.  For example:
       Prenatal and childhood exposure to
       contaminants, such as lead, PCBs, and
       mercury, via multiple exposure pathways may
       inhibit a child's intellectual development and
       ultimately may result in behavioral problems.

       Exposure to endocrine disrupting chemicals,
       such as organochlorine pesticides and PCBs,
       may cause birth defects and alterations of
       normal childhood growth and development
       (Browner 1998, U.S. EPA 1998w).
 Children Experience Increased Risk From
     Environmental Hazards Because:

Their systems are still developing making them
more susceptible to environmental threats.

They eat more food, drink more fluids, and
breathe more air per pound of body weight
making them more exposed to environmental
hazards.

Their behavior,  such as crawling on the
ground, and lack of ability to protect themselves
exposes them to hazards that adults can easily
avoid.
        In an effort to protect children from
environmental health threats, EPA published its
National Agenda to Protect Children's Health from Environmental Threats in April 1996. This agenda
calls for the consideration of children's risks in all appropriate agency actions and a greater emphasis on
research to support children's risk assessment activities (U.S. EPA 1996a). In addition, EPA established
its Office of Children's Health Protection (OCHP) in May 1997 to ensure the implementation of the
President's 1997 Executive Order to Protect Children from Environmental Health and Safety Threats.
The OCHP's mission is to make the protection of children's health a fundamental goal of public health
and environmental protection in the U.S. The office supports and facilitates EPA efforts to protect
children from environmental threats (U.S. EPA 1998t).

        The President's Executive Order requires all Federal agencies to address  health and safety risks
to children, coordinate research priorities on children's health, and ensure that their standards take into
account special risks to children. The EPA documents its current actions in regard to children's health in
The EPA Children's Environmental Health Yearbook (U.S. EPA 1998q). The yearbook includes sections
on asthma and respiratory effects, childhood cancer, developmental  and neurological toxicity, health
effects of pesticides, and potential risks from contaminated surface and ground water.  To coordinate
research efforts, EPA and the National Institute of Environmental Health Services developed a grant
program to support the establishment of Centers for Children's Environmental Health and Disease
Prevention Research. The purpose of these centers is to foster the advancement of children's health
through enhancing the public's understanding of basic disease mechanisms and promoting community-
based prevention activities related to children's respiratory disorders, childhood learning, and growth and
development (U.S. EPA 1998t).

        The EPA, in coordination with other Federal agencies, has begun several efforts to address these
specific threats. Most notably, EPA has conducted an Agencywide Risk Assessment Forum colloquium
on children's risk and has begun to review and revise several of its risk assessment guidance documents
to identify areas where children's health protection is or should be considered. Mercury, lead, dioxin,
HCB, and PAHs are among the chemicals included in this risk characterization (Browner 1998). As part
of this effort, EPA requested that the Federal Children's Health Protection Advisory Committee
(CHPAC) recommend existing standards that may merit reevaluation in order to further protect
children's environmental health. One recommendation was to reevaluate the chlor-alkali NESHAP
 Page 111-32          Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                                   Chapter III
                                                                Major Programs and Activities
 (mercury). In response, EPA has begun a process to revise this standard, including a risk assessment of
 mercury emissions from chlor-alkali plants (64 FR 5277, February 3, 1999). Also, EPA, the Department
 of Health and Human Services, and other Federal agencies have begun to develop a comprehensive cross-
 government strategic plan to address the  causes of children's asthma and the scope of the problem
 (Browner 1998).
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Page 111-33

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Chapter III
Major Programs and Activities
III.B
REGIONAL AND WATERBODY-SPECIFIC PROGRAMS
       All of the Great Waters are affected by the policies and activities of multiple communities and
governments on their shores. The Great Lakes, for example, are affected by the environmental
management decisions of two nations, one Canadian Province, eight States, a number of tribes, and
countless municipalities. Intergovernmental or multistakeholder institutions (e.g., the Lake Michigan
Forum) have been established for many of the Great Waters to coordinate resource management decision
making and resolve conflicts. In addition, EPA and NOAA, as directed by Congress, administer several
programs to address particular regional and waterbody-specific environmental challenges. These
programs lead or support many efforts to evaluate or control the impacts of pollution, including pollution
via atmospheric deposition, on the Great Waters ecosystems.

       The EPA has found that regional environmental challenges, such as those facing the Great
Waters, are often best solved through collaboration with local stakeholders and with a holistic approach
that addresses human social and economic needs as they relate to environmental quality. The EPA has
used these approaches in a number of place-based (i.e., geographically-based) programs, including the
National Estuary Program; Great Lakes, Chesapeake Bay, and Clean Lakes Programs; and, the Regional
Geographic Initiative. These approaches are further developed in EPA's Community-Based
Environmental Protection (CBEP) program. The EPA's Strategic Plan (EPA 1997c) recognized CBEP as
the Agency's main tenet for "reinventing" its approach to environmental protection by considering
environmental problems across organizational and political boundaries and in a multimedia fashion.  The
Agency is now using the CBEP approach in several of the regional and waterbody-specific programs and
activities described in this section.
Page UI-34
     Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                                   Chapter III
                                                                 Major Programs and Activities
GREAT LAKES PROGRAM
       Administered by EPA's Great Lakes National Program Office (GLNPO), the Great Lakes
Program consists of programs and activities initiated by EPA, States, tribes, and their partners that are
designed to address challenges facing the Great Lakes ecosystem. Several of these activities involve
atmospheric deposition and Great Waters pollutants of concern.

       The GLNPO has provided funds for monitoring of toxics in conjunction with the Episodic
Events/Great Lakes Experiment (EEGLE) Study research effort. The EEGLE Study is being funded by
the National Science Foundation and NOAA to study nutrient transport hi a plume that occurs in Lake
Michigan annually. This effort enables the study of air-water exchange of toxics in this plume. This
information will be used in support of the Lake Michigan Mass Balance Study (LMMBS) by providing
insight into the air/water exchange of PCBs and PAHs.  The project will also provide information
necessary to determine the spatial and temporal variation of loadings across large lakes.  This project is a
pilot for future air/water toxics sampling projects, such as planned additional over-water measurements
for the Integrated Atmospheric Deposition Network (IADN) program.

       In addition to these activities, the Great Lakes Program is continuing to utilize remedial action
plans (RAPs) for areas of concern (AOCs) and lakewide management plans (LaMPs) to target ecological
problems on a geographic basis, in accordance with the 1978 Great Lakes Water Quality Agreement
(GLWQA) between Canada and the U.S. The LaMPs and RAPs are tools for reducing the input of
pollutants to the Great Lakes and restoring the environmental quality of the  Great Lakes basin.

       The LaMPs and RAPs target ecological problems on a geographic basis and provide a
community-based approach to identifying and solving environmental problems. Both tools were
originated in response to the GLWQA goals of restoring and maintaining the chemical, physical, and
biological integrity of aquatic ecosystems.  The RAPs were first established in 1985 to provide more
uniform guidance  on how to restore uses in AOCs. Rivers, connecting channels, harbors, and
embayments of the Great Lakes are designated as AOCs if there is an impairment of beneficial use or the
area's ability to support aquatic life. Unlike RAPs, the development and implementation of LaMPs for
each of the five Great Lakes was a specific objective of the GLWQA. The LaMPs are frequently
integrated with RAPs and other efforts that are best suited to  address issues  of local concern.
       The Great Lakes Water Quality Board of the
International Joint Commission (IJC) established 42
AOCs in the Great Lakes basin (Figure III-2): 26 within
the jurisdiction of the U.S., 12 within Canadian
jurisdiction, and 5 shared by both countries. The RAPs
are being developed for each of these AOCs to address
impairments to any one of the  14 beneficial uses (e.g.,
restrictions on fish and wildlife consumption, dredging
activities, or drinking water consumption) associated with
these areas. The RAPs are prepared and implemented by
the eight Great Lakes States and the Province of Ontario,    	
with help from Federal agencies and organizations, local
governments, industry, environmental groups, and
individuals. Although there has been significant progress in developing and implementing most RAPs
(including the delisting of the Collingwood Harbor AOC in Canada), considerable challenges remain.
  IJC Identified Seven AOCs That Have
   Developed Particularly Successful
       Remediation Strategies

•i Black River (Ohio)
/ Grand Calmumet River/Indiana Harbor
  Ship Canal
/ Hamilton Harbor (Ontario)
/ Ashtabula River (Ohio)
/ Bay of Quinte (Ontario)
/ Manistique River (Michigan)
/ Muskegon and White Lakes (Michigan)
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
                           Page 111-35

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                                                                                   Chapter in
                                                                 Major Programs and Activities
One of the major problems facing the AOCs today is toxic contamination of sediments, contributing to
beneficial use impairments.
                                     Superior
                                     Michigan

                                     Huron
                                     Erie
                                     Ontario
Current Status of LaMPs in the Great Lakes

      Binational Program to Restore and Protect the
      Lake Superior Basin announced (1991)
      Stage 1 LaMP submitted to IJC (1995)
      Stage 2 LaMP released (1999)
      Stage 3 LaMP in development

      LaMP published in Federal Register (1994)

      LaMP not established

      LaMP Management Committee formed (1994)

      Lake Ontario Toxics Management Plan (1989)
      LaMP Workplan signed (1993)
      Stage 1 LaMP released (1998)
       Both the U.S. and Canadian
governments are charged with
developing LaMPs for each of the
Great Lakes, with the exception of
Lake Michigan. Because Lake
Michigan lies entirely within the
boundaries of the U.S., the Lake
Michigan LaMP was developed
solely by the U.S. government.  The
LaMPs are in various stages of
development for each of the Great
Lakes (see sidebar).  Not all of the
LaMPs have been completed;
however, commitments have been
made  by key stakeholders in the
respective basins to pursue toxics
reductions and actions are being
taken  to achieve these goals. Each LaMP addresses a different list of critical pollutants, commonly
including mercury, PCBs, hexachlorobenzene, dioxins, furans, chlordane, DDT and metabolites, and
dieldrin, all of which are Great Waters pollutants of concern.

       The Lake Superior LaMP is unique in that it is being developed in stages. The Stage 1 LaMP
was submitted to the IJC hi 1995.  The Stage 2 LaMP, which addresses critical pollutants, is available on
EPA's web site at www.epa.gov/grtlakes/lakesuperior/stage21anip.html. The Stage 3 LaMP, which is
currently in development and is  available as a review draft on EPA's web site at
www.epa.gov/grtlakes/lakesuperior/stage3/review.html, addresses selection of remedial measures and
management strategies to achieve critical pollutant load reduction targets.

LAKE CHAMPLAIN BASIN PROGRAM
       Since the Second Report to Congress, the Lake Champlain Basin Program (LCBP) has continued
to develop and implement a comprehensive pollution prevention and restoration plan for the lake and its
watershed, as called for by the Lake Champlain Special Designation Act of 1990. In October 1996, the
LCBP finalized Opportunities for Action, An Evolving Plan for the Future of the Lake Champlain Basin
(LCBP 1996a, b).  The final plan differs little from the draft plan, which was described in detail in the
Second Report to Congress. Environmental issues addressed by the plan include high phosphorus levels,
toxic substances (most notably PCBs and mercury) in biota and sediment, and invasive non-native
species. Atmospheric deposition of mercury to Lake Champlain basin is the subject of research efforts
described in Chapter II.

       The LCBP supported and published several technical reports on the Lake Champlain basin and
the Lake Champlain ecosystem. For example, in October 1997, the LCBP published Phase II of the Lake
Champlain Sediment Toxics Assessment Program (Mclntosh et al. 1997).  The first phase, which was
discussed in the Second Report to Congress, accomplished a lakewide screening  of surface sediments for
an array of organic and inorganic trace contaminants, more intensive evaluations at nine sites with
elevated contaminants levels, and an assessment of PCB bioaccumulation from sediment by the
macroinvertebrate Mysis  relicta.  Phase II further targeted investigations to the three most contaminated
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areas of the lake: Cumberland Bay, Malletts Bay, and Burlington Harbor. Results of the Phase II
investigation are presented in Chapter II above.

       Other recent research projects sponsored by LCBP include development and compilation of
Geographic Information Systems data for the basin (VCGI1996, Millette 1997); hydrodynamic and
water quality modeling and monitoring  (ASA 1996, Lake Champlain Basin Program 1998); food web
modeling (LeBar and Parrish 1996); and, other ecological subjects. Numerous other LCBP-supported
publications address economic, educational, recreational, and other resource management subjects.
Future research will focus on environmental indicators. In addition, the Lake Champlain Steering
Committee, which evolved from the Management Conference, includes the Province of Quebec as a
member.  Involvement of Quebec will ensure that both U.S. and Canadian concerns are addressed.

CHESAPEAKE BAY PROGRAM
                                                           Chesapeake Bay Program Partners

                                                          «s> State of Maryland
                                                          e> Commonwealth of Virginia
                                                           Commonwealth of Pennsylvania
                                                          «s> District of Columbia
                                                          e> Chesapeake Bay Commission
                                                          «a> U.S. EPA (representing all Federal
                                                             agencies, e.g., NOAA, U.S. FWS)
       The Chesapeake Bay Program (CBP) is a unique
regional partnership (see sidebar) that has been responsible
for directing and implementing the restoration of the
Chesapeake Bay since 1983. Since that time, the highest
priority has been placed on restoring the living resources of
the bay, including finfish, shellfish, bay grasses, and other
aquatic life and wildlife. Examples of specific actions
undertaken by the CBP include agricultural best management
practices, pesticide collection and disposal programs, public
education, Biological Nutrient  Removal at wastewater
treatment facilities, and a phosphate detergent ban (Chesapeake Bay Program 1998d).  In addition, the
CBP is working withNOAA's Chesapeake Bay Environmental Effects Committee which supports
research on contaminated sediment to better understand issues related to the management of
contaminated sediments.
       As discussed in the Second Report to Congress, the 1994 Chesapeake Bay Basinwide Toxics
Reduction and Prevention Strategy is an integral part of the CBP. The primary goal of the strategy is a
"Chesapeake Bay free of toxics by reducing or eliminating the input of chemical contaminants from all
controllable sources to levels that result in no toxic or bioaccumulative impact on the living resources
that inhabit the bay or human health." The strategy contains commitments in the following five areas: (1)
regional focus — calls for assessing the status of chemical contaminant effects on the living resources of
the bay and its tidal waters and implementing reduction and prevention activities in those areas; (2)
directed toxic assessments — calls for the characterization of chemical contaminant conditions in the bay,
the assessment of low level toxics exposure to living resources as well as the update of the Toxics
Loading and Release Inventory to identify toxics sources; (3) regulatory program integration - calls for
Chesapeake Bay Program activities to complement and enhance Federal, State, and local regulatory
programs; (4) pollution prevention — includes facility-based pollution prevention, pesticide management,
and consumer/household hazardous waste activities and goals; and, (5) strategy implementation -
outlines how the strategy will be implemented.

       The strategy addresses non-point source pollution,  committing the CBP signatories to "establish
more complete loadings baselines and source identification for storm water runoff, atmospheric
deposition, and acid mine drainage, and set reduction targets from that baseline to be achieved over the
next decade." The CBP will use the updated 1999 Chesapeake Bay Basinwide Toxics Loading and
Release Inventory, which provides updated chemical contaminant loadings estimates for atmospheric
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    Reducing Pesticide Use in the Chesapeake Bay
                    Watershed

   The CBP has been working toward goals to reduce
   pesticide use in the Chesapeake Bay watershed.
   Recent accomplishments include the following:

   • Pesticide collection and disposal programs have
   been offered in all Virginia and Pennsylvania
   counties and 75 percent of Maryland counties in the
   watershed.  Over 1.1 million pounds of pesticides
   have been collected;

   • Between 1993 and 1998, nearly 600,000 pesticide
   containers have been collected and recycled.

   • Integrated Pest Management is now used on
   nearly 4.4 million acres (61 percent) of agricultural
   cropland in the watershed.
                                                   deposition and other point and non-point sources
                                                   to address this commitment. The inventory
                                                   reports atmospheric deposition loads from
                                                   chemical contaminants in the air that are
                                                   deposited onto the bay and its tidal rivers. These
                                                   estimates are updated and expanded using recent
                                                   field measurements and improved theoretical
                                                   understanding of deposition processes.
                                                   Volatilization of organic contaminants from the
                                                   surface waters to the air is considered for the
                                                   first time in calculating a "net" atmospheric
                                                   loading to the bay and tidal rivers. Initial
                                                   estimates of the contribution of urban areas to
                                                   atmospheric deposition loads to the bay and tidal
                                                   rivers are also reported.  Only loads to tidal
                                                   waters (below the fall line) are reported. The
                                                   TRI database for industrial air releases was not
                                                   included in this inventory, as it was in 1994,
since the improved and expanded atmospheric loadings data (to tidal waters) are based on measured data
and are a much better representation of loads than the TRI data estimates of releases. The inventory
reports that atmospheric deposition loads to the tidal waters increase in areas of the bay and tidal rivers
adjacent to urban areas (Chesapeake Bay Program 1999a).

       To focus toxic reduction and prevention efforts, the CBP developed a list of Chesapeake Bay
toxics of concern (i.e., chemicals that cause or have a potential to cause adverse impacts on the bay
system, such as mercury, PAHs, and PCBs -- see
sidebar). By 2000, the CBP is directed to
reevaluate and revise the 1994 toxics strategy.
Future plans for the Chesapeake Bay Program
include research in support of regional action
plans for areas with known toxics problems, with
a particular emphasis on how to deal with
contaminated sediment.  In addition, data
collected over the past decade will continue to be
analyzed to determine which chemicals have been
detected in water, sediment, shellfish, and finfish
to identify other toxics problems in the bay
(Chesapeake Bay Program 1998c).
                                                    Chesapeake Bay Program Toxics of Concern
                                                  Atrazine
                                                  Benz[a]anthracene
                                                  (PAH)*
                                                  Benzo[a]pyrene (PAH)*
                                                  Cadmium
                                                  Chlordane*
                                                  Naphthalene (PAH)*
                                                  Tributyltin
Chromium
Chrysene (PAH)*
Copper
Fluoranthene (PAH)*
Lead*
Mercury*
PCBs*
                                                         ' Great Waters pollutants of concern
        Nitrogen reduction in the bay is an
ongoing focus of the CBP. Recent modeling efforts indicate that approximately 21 percent of the
nitrogen entering the bay is from atmospheric deposition. Therefore, the CBP is working to quantify and
address atmospheric nitrogen and toxics emissions and sources along with their associated impacts on the
bay resources. A current effort involves assessing the benefits that will be experienced due to the
implementation of the CAA. The CBP is also supporting scientific research which is being conducted to
better understand the integrated, multimedia relationships of the ecosystem.  In addition, the Chesapeake
Bay Program is developing a strategy to better understand and quantify the various forms of nitrogen
which may be affecting living resources and water quality in the Chesapeake Bay.  Part of an integrated
basinwide monitoring  effort, this strategy will help to fill in gaps in our knowledge of atmospheric
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deposition of nitrogen compounds, focusing in the near term on measuring deposition of ammonia and
ammonium in the coastal areas (Chesapeake Bay Program 1998a).

       In addition, recent actions taken under the Clean Water Act resulted in listing portions of the
Chesapeake Bay and its tidal rivers as impaired waters. These actions have emphasized the regulatory
framework of the Clean Water Act along with the ongoing cooperative efforts of the Bay Program as the
means to address the nutrient enrichment problems within the Bay and its rivers. In response, the Bay
Program partners have committed to a process for integrating the cooperative and statutory programs of
the Chesapeake Bay and its tributaries. In the new Chesapeake Bay Agreement, the partners are
committed to developing goals for improving water quality in the Bay and its tributaries so these waters
may be removed from the impaired waters list prior to the timeframe when regulatory mechanisms under
section 303(d) of the Clean Water Act would need to be applied.

       The CBP is helping bay partners to incorporate air pollution impacts in the management of
lakes, rivers, and streams. For example, the CBP is encouraging States to account for air deposition in
TMDL development (for background information on TMDLs, see the TMDL discussion on page III-5)
and helping bay States account for atmospheric deposition of nitrogen compounds in developing tributary
strategies to protect the bay.  Tributary strategies are "clean-up plans" for each major river that flows into
the bay. The Commonwealth of Virginia is developing tributary strategies for their southernmost bay
tributaries, and the CBP is providing modeled information on how different management scenarios for
atmospheric nitrogen emissions  will affect deposition loads. This will give States an idea of different
options for cleaning up lakes, rivers, and streams. For example, an understanding of how much nitrogen
will not enter the bay by implementing certain air controls will allow States to count the cost of all of the
options of reducing nitrogen inputs.  In comparing methods of nutrient reduction in waters in the
Chesapeake Bay area, it may be that cleaning up the air is more cost-effective than some water-based
controls, such as additional storm water management in cities.

        Despite the progress made to date in reducing inputs of nitrogen to the Chesapeake Bay, the
Chesapeake Executive Council announced that unless current efforts are accelerated, the nitrogen
reduction goal of the Chesapeake Bay Agreement will not be met by the year 2000. In 1997, the
Executive Council developed three new directives to accelerate the reduction of nitrogen inputs to the
bay.
 1.      The Baywide Nutrient Reduction
        Progress and Future Reductions
        directive outlines a series of actions
        aimed to further commitments made in
        the Chesapeake Bay Agreement. One of
        the actions is to "Work toward additional
        reductions of airborne nitrogen delivered
        to the Bay and its watershed from all
        sources including States outside the
        watershed, and seek improved
        understanding of how airborne nitrogen
        affects the Bay and its watershed.." The
        directive includes a time line for
        completing refinements of computer
        modeling as well as water quality
        monitoring. Outputs from monitoring
        and modeling efforts will be used to help
                              Growing Attention to Sources of Ammonia and
                                      Urea to the Chesapeake Bay

                            Ammonia and urea are other forms of nitrogen that
                            are receiving increased attention from researchers
                            and regulatory agencies, in part because these forms
                            are more biologically available.  One of the sources
                            of ammonia and urea is manure from animal farming
                            operations. With the increase in animal farming in
                            the bay watershed and surrounding States,
                            particularly hog and poultry farming, it is important to
                            investigate pollutant emissions to the air and the
                            distances they travel in the air before being deposited
                            to land or water surfaces. The CBP sponsored a
                            workshop on atmospheric organic nitrogen (e.g.,
                            urea) and is coordinating with NOAA to determine
                            atmospheric concentrations of ammonia, estimate
                            ammonia deposition to land and water surfaces, and
                            evaluate the importance of ammonia transport and
                            deposition.
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        set nutrient goals for Virginia tributaries and to develop a protocol to determine whether nutrient
        reduction efforts can be further targeted to areas of persistent high loadings.

 2.      The Wetlands Protection and Restoration Goals directive provides quantifiable wetland
        restoration goals to assure no net loss of wetlands and to move in the direction of a net gain of
        wetland areas.
 3.      The Community Watershed Initiative will develop a community watershed strategy to ensure
        that Chesapeake Bay Program goals and objectives are integrated at the community watershed
        scale (Chesapeake Bay Program 1998b).
                                                                      National Aeronautics
                                                                      and Space Administration
                                                                                     Louisiana
                                                                                       Mississippi
 GULF OF MEXICO
 PROGRAM

        The Gulf of Mexico Program
 emphasizes community-based,
 ecosystem management approaches to
 environmental protection, including
 (1) equal partnership among
 government agencies and private and
 non-government interests to define
 problems and implement solutions, (2)
 use of the best science and knowledge
 available to support decisions and
 guide actions, and (3) public
 involvement in all phases of the
 program to generate the consensus
 needed for action.  The Gulf of
 Mexico Program is not a regulatory
 program, although some of the partner
 agencies at the Federal and State
 levels have regulatory responsibilities.
 The program provides a forum whereby issues that cross political or social boundaries can be clearly
 identified, discussed, and collaboratively resolved to benefit the ecological and economic resources of
 the Gulf of Mexico.

        Given the vast geographic scope of the gulf, protection of these critical resources requires a long-
 term commitment and focused attention.  A strategic assessment process is being implemented to focus
 future efforts, identify resources at greatest risk, and establish quantitative goals to measure progress.
 Currently, the Gulf of Mexico Program is addressing four priority environmental concerns, two of which
 are relevant to the Great Waters program: (1) protecting the public from contaminated shellfish and
 recreational waters, and (2) excessive nutrient enrichment.

       Excessive nutrient enrichment is attributable to a multitude of terrestrial and atmospheric sources
throughout the Gulf States and the watersheds (e.g., the Mississippi River basin) that drain into the gulf.
The Gulf of Mexico Program, as a multiagency effort, is working with State and community partners on
 several projects to protect the gulf from the deleterious effects of nutrient enrichment.
                                        Department of
                                        Health & Human
                                          Services
                                                  Environmental
                                                   Protection
                                                    Agency
Agricultural
 Interests
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       For example, the Gulf of Mexico Program is working with the Gulf States to address nutrient
enrichment problems in the gulf, such as a zone of hypoxia along the Louisiana coast. Hypoxia in the
northern gulf represents one of the largest zones of oxygen-deficient bottom waters in the western
Atlantic Ocean. Nitrate and other nutrients discharged from the Mississippi River are the probable cause,
making agricultural and municipal runoff and atmospheric deposition potential sources to investigate.

       In addition, the Gulf of Mexico Program is supporting two initiatives of a multiagency scientific
team established by the White House's Committee on Environment and Natural Resources (CENR). In
particular, the Gulf of Mexico Program is supporting studies to characterize the ecological and economic
consequences of hypoxia in the gulf and nutrient sources and loads to the gulf from the Mississippi
River. Further discussion of the CENR process can be found in Chapter IV of this report.

NATIONAL ESTUARY PROGRAM
                                                                   NEPs Conducting
                                                             Atmospheric Deposition Studies

                                                             Albemarle-Pamlico Estuary (NC)
                                                             Casco Bay (ME)
                                                             Charlotte Harbor (FL)
                                                             Coastal Bend Bay and Estuary (TX)
                                                             Delaware Inland Bays (DE)
                                                             Indian River Lagoon (FL)
                                                             Long Island Sound (NY, CT)
                                                             Massachusetts Bay (MA)
                                                             Maryland Coastal Bays (MD)
                                                             Mobile Bay (AL)
                                                           •f New York/New Jersey Harbor (NY, NJ)
                                                           4- Peconic Bay (NY)
                                                           + San Francisco Bay (CA)
                                                           + Santa Monica Bay (CA)
                                                           + Sarasota Estuary (FL)
                                                           + Tampa Bay (FL)
       Coastal waters addressed by the Great Waters
program include all estuaries covered by the National
Estuary Program (NEP). In 1987, Congress established the
NEP as part of the Clean Water Act. The NEP's mission is
to protect and restore the health of the estuaries while
supporting economic and recreational  activities. The EPA
periodically calls for nominations of estuaries to the NEP
from State governors. If an estuary meets the Agency's
criteria, EPA may then designate it as  an estuary of national
significance. As depicted hi Figure 1-2, there are currently
28 estuaries around the country and in Puerto Rico in the
National Estuary Program.

       To date, at least 19 NEPs have identified
atmospheric deposition of pollutants as a threat to the health
of their estuaries. Many of these NEPs either have initiated
studies on the contribution of atmospheric deposition to
annual loadings of nitrogen and/or other pollutants, or have
expressed serious interest to EPA in conducting such
projects. In 1999, EPA provided funds to establish new
atmospheric deposition monitoring sites in five NEPs, expanding the National Atmospheric Deposition
Network in the coastal waters and improving the ability to compare coastal data to data collected from
inland sites. Peconic Bay NEP and Maryland Coastal Bays NEP are monitoring for nitrogen and sulfur
compounds, San Francisco Bay is monitoring for mercury compounds, and Mobile Bay NEP is
monitoring for sulfur, nitrogen, and mercury compounds. In addition, a site measuring dry deposition of
sulfur and nitrogen compounds (part of the CASTNet monitoring network) is being established near
Indian River Lagoon NEP.  The following describes other NEP sites and their associated atmospheric
deposition research activities to date.

•       Albemarle-Pamlico Estuary (NC). Nitrogen deposition studies in eastern North Carolina are
        primarily focusing on the emissions and deposition of ammonia. Concern has been spurred by
        the explosive growth of large-scale hog farming operations in the coastal plain over the last few
        years.  For example, long-term analysis of National Atmospheric Deposition Program (NADP)
        data from a site near the center of an intensive animal operations (i.e., Sampson County, NC)
        indicate at least a doubling of NH4+ deposition since the early 1980s (Paerl 1997b). Monitoring
        efforts led by researchers from the University of North Carolina at Chapel Hill (UNC-CH) and
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        North Carolina State University (NCSU) are aimed at quantifying atmospheric levels of both gas
        and aerosol forms of ammonia to aid in the development of regional-scale, air quality models
        (Robin Dennis, NOAA/EPA). Monitoring began in fall 1998, but data obtained in the 1999
        summer season will be critical in understanding seasonal emission and deposition patterns.
        Additional efforts are aimed at developing nitrogen budgets for the Neuse River basin.  These
        projects began with State funding and, when completed, will put the atmospheric contribution
        into the context of the overall nitrogen load to the Neuse River basin (W. Robarge, NCSU; H.
        Paerl, UNC-CH). The EPA is also funding research to examine the biological ramifications (e.g.,
        eutrophication) of atmospheric nitrogen inputs in the Neuse River basin and the adjacent coastal
        waters.

        Casco Bay (ME). The Casco Bay Air Toxics Deposition Study, begun in 1998, is a multiyear
        collaborative effort by the Casco Bay Estuary Project, the Maine Department of Environmental
        Protection, EPA Region I, and university research scientists (University of Massachusetts,
        Lowell). The study focuses on atmospheric deposition of five contaminant groups (i.e., mercury,
        toxic trace elements, PAHs, nitrogen, and fine particulates) and is funded by the Great Waters
        program as part of the national strategy to determine the environmental health and status of key
        NEP ecosystems. The objectives of the study are to characterize seasonal and annual
        depositional patterns of toxic air compounds to Casco Bay and to develop a generic assessment
        method that can be used by other community-based programs.

        Charlotte Harbor (FL). The Charlotte Harbor NEP atmospheric deposition study received
        funding in 1999 and will begin activities in 2000.

        Coastal Bend Bay and Estuary Program (TX). The concentrations of nutrients and organic
        contaminants (including PAHs, PCBs, and some pesticides) in wet and dry atmospheric
        deposition is being measured or  calculated at two representative sites on Corpus Christi Bay. An
        EPA grant expanded the pollutants measured at one station to include organic contaminants. The
        wet nutrient deposition data are comparable to other air monitoring programs, including the
        NADP, but this is one of the only NEP studies that measures the deposition rate of organic
        contaminants. This study is being conducted in conjunction with other studies in the area
        (including EPA's Environmental Monitoring and Assessment Program (EMAP) and NOAA's
        National Status and Trends Program) to measure the inputs to the bay and estuary of organic
        pollutants, trace metals, and nutrients from other sources (e.g., other non-point sources, point
        sources).  This will allow the Coastal Bend Bay and Estuary Program to calculate the importance
        of atmospheric deposition for each pollutant and target control measures where they are most
        effective.

        Delaware Inland Bays (DE). The University of Delaware Graduate College of Marine Studies
        is undertaking three studies to address atmospheric deposition issues related to the Delaware
        Inland Bays. The first study, currently in progress and funded by the Delaware Department of
        Natural Resources and Environmental Conservation (DNREC), has two primary objectives: (1)
        to accurately quantify the atmospheric loading of nitrogen to the Delaware Inland Bays; and (2)
        to assess, in cooperation with the University of Delaware Center for Climatic Studies, the
        meteorological transport patterns which contribute to the observed nitrogen deposition.  The
        second study, also funded by the DNREC, will examine the episodic impact of large precipitation
        events on the loading of nitrogen to the Delaware Inland Bays by both direct (deposition to the
        water surface) and indirect (via watershed transmission) pathways.
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       The third study, which is funded by the EPA National Estuary Program, will address the impacts
       of local sources (e.g., a coal-fired power plant, poultry-rearing facilities) on nitrogen deposition
       to the Delaware Inland Bays and distinguish the impacts of local sources from the impacts of
       regional sources. Research to date indicates a 60 percent increase in the wet deposition of
       ammonia over the past two decades. Although the explanation is uncertain, the working
       hypothesis is that the increase is related to the large increase in poultry production on the
       Delmarva Peninsula. The NEP grant will test this hypothesis. An analogous situation exists in
       coastal North Carolina where the approximate doubling of the concentration of ammonia in
       precipitation over the past 10 years has been attributed to the proliferation of hog farms in the
       region (Paerl 1997b). Such increases in atmospheric ammonia deposition are not only important
       because of the additional sources of nitrogen to surface waters, but also because ammonia
       represents the most readily-available form of nitrogen for most aquatic organisms.

       Long Island Sound Estuary Program (NY, CT).  The Long Island Sound Study (LISS) Estuary
       Program has been evaluating atmospheric nitrogen sources leading to the development of a final
       nitrogen control plan. Wet and dry deposition monitoring studies have expanded in recent years
       through a cooperative effort with the Connecticut Department of Environmental Protection
       (CTDEP) and the University of Connecticut (UConn).  The UConn now maintains eight
       sampling stations spread throughout Connecticut where wet and dry monitoring of nutrients and
       mercury is conducted. The data have been key to estimating nitrogen deposition loads, which are
       about 10 Ib/acre-year in the Long Island Sound region.  The anthropogenic component of the
       atmospheric deposition delivered to Long Island Sound is estimated to be around 6,700 tons  of
       nitrogen annually including about 3,700 tons that fall directly on the sound.  This combined
       direct and indirect deposition represents about 15 percent of the total load of nitrogen to Long
       Island Sound from the New York and Connecticut portions of the watershed. Additional
       nitrogen loadings come from atmospheric deposition onto the Long Island Sound drainage basins
       north of Connecticut, the watersheds of the New York/New Jersey Harbor and Narragansett Bay,
       and from direct deposition on the Atlantic Ocean that currents transport into Long Island Sound.
       In February 1998, the States of New York and Connecticut and EPA agreed to a reduction target
       of 58.5  percent below a 1990 baseline for point and terrestrial non-point source enrichment.
       While achieving that target will greatly improve oxygen conditions in the sound, it will not attain
       existing State water quality standards for dissolved oxygen. In a TMDL analysis being prepared
       by Connecticut and New York, additional actions are identified, including atmospheric
       reductions of nitrogen planned under the CAA. The analysis identifies that reducing atmospheric
       sources of nitrogen will be key to long term efforts to attain water quality standards.

       Massachusetts Bays (MA).  Wet and dry deposition of toxic compounds, including metals and
       PAHs, were measured from September 1992 to September 1993 at two sites, one in the northern
       bay and one in the southern bay on Cape Cod.  Dry deposition was greater at the northern site
       (close to Boston) for most metals.  Wet deposition, on the other hand, was greater at the southern
       site for the metals. The high dry deposition rates at the northern site are probably due to its
       proximity to Boston. The high wet deposition rates on Cape Cod are probably from sources
       upwind in southern New England, New York, and New Jersey. Both dry and wet deposition of
       PAHs were higher at the northern site, also probably from sources in the Boston metro area,
       including Logan Airport. Dry deposition was highest at both sites in the winter.  No PCBs were
       found at either site.

       Wet nitrogen deposition data from four regional (three in Massachusetts and one in coastal
       Maine) NADP sites were also analyzed from the early 1980s (1980,  1981, or 1982, depending on
       the site) through 1993. Dry deposition data were collected from a literature search.  Direct
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        deposition to the bays was estimated to be 6-8 percent of the total nitrogen load.  Approximately
        two-thirds were in the form of wet deposition. The percentage of nitrogen in the surface layer,
        where a large portion of the biological activity occurs, was also estimated in an attempt to
        quantify the biological availability of atmospherically deposited nitrogen. Direct deposition was
        estimated to be approximately 2 percent of this surface-layer nitrogen during the winter months.
        However, this is probably the lowest percentage that occurs during the year, and deposition may
        be an important source of nitrogen in the summer months.  Uncertainties related to in situ dry
        deposition sampling and wet dissolved organic nitrogen sampling require additional research.

        New York/New Jersey Harbor Estuary Program (NY, NJ). New York-New Jersey Harbor is
        currently the focus of several studies relating to sources of nutrient and toxic pollution loadings
        to the harbor.  These studies will help to quantify pollutant loadings under the TMDL
        determination. As part of that effort, four air deposition monitoring stations were set up in the
        harbor area for limited monitoring for PCBs, PAHs, dioxin, heavy metals, and nitrogen. This
        information will then be available to determine the total loadings of contaminants that are not
        meeting criteria from all sources. Control options for meeting the TMDLs may include a
        reduction of air sources.  This work is being conducted in cooperation with the New Jersey
        Department of Environmental Protection and the Hudson Pviver Foundation.

        San Francisco Estuary (CA). The San Francisco Estuary Project (SFEP) is working with the
        Bay Area Stormwater Management Agencies Association (BASMAA) to identify sources of air
        emissions resulting in deposition of pollutants onto the land and to quantify the contribution of
        air pollutants reaching the estuary in storm water runoff. The pollutants of concern are primarily
        toxics, including copper, mercury, PCBs, and PAHs. This study is being coordinated with the
        San Francisco Estuary Regional Monitoring Program for Trace Substances (see page 11-76). The
        San Francisco Estuary Institute (SFEI) coordinates the Regional Monitoring Program, which
        includes water, sediment, and tissue monitoring and is now being expanded to monitor air
        deposition. The SFEI is conducting a pilot study to evaluate pollutants which are being
        deposited from the air directly onto the estuary waters.  Based on these studies, local and State
        agency partners will be able to assess the cost-effectiveness of emission reduction options and
        quantify the benefits associated with emission reduction strategies.

        Santa Monica Bay (CA).  The Santa Monica Bay NEP has proposed an air transport/deposition
        study to (1) quantify emissions of the toxic materials and nitrogen in the Los Angeles air basin
        that are subsequently deposited in the bay and its watershed; (2) identify pollutant sources and
        their relative contributions to total pollutant loading to  the bay; and, (3) evaluate the relative
        impacts of air deposition and the benefit of various emission reduction options in order to
        recommend the most cost-effective measures to control the identified sources. Initially, the Santa
        Monica Bay study will quantify the wet and dry toxic and nitrogen deposition to the bay surface.
        Indirect deposition over the landscape will be calculated using a model developed locally for the
        region that uses air concentrations, local meteorology, and surface types (trees,  pavement) to
        calculate deposition velocities and loadings. This study will measure air concentrations over
        water, a difficult process that is not often done but that is necessary to improve the understanding
        of direct deposition processes. The study will also measure the impact of air deposition during
        "events" (fire storms, rain storms, Santa Ana winds) to understand how these weather patterns
        contribute to local air deposition.
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       Sarasota Estuary (FL). The Sarasota Bay NEP is involved in four large research projects.

       Atmospheric Monitoring Site on Sarasota Bay. For the average rainfall year, it is estimated that
       atmospheric deposition directly to the water surface provides 26.5 percent of the total nitrogen
       load to the bay. Under cooperative agreements with EPA, the Southwest Florida Water
       Management District (SWFWMD), and local governments, the Sarasota Bay NEP initiated an
       intensive, 1-year atmospheric deposition monitoring effort (within the national NADP/AIRMoN
       program) in September 1998. The intensive monitoring program is designed to establish
       relationships between emission sources or source regions and deposition to specific receptors.

       Atmospheric Transport and Dispersion Model. Preliminary modeling by EPA using the
       Regional Atmospheric Deposition Model (RADM) at an 80 km grid suggested that 70 percent of
       the atmospheric nitrogen deposited to Sarasota Bay may originate from outside the watershed.
       Therefore, the Sarasota Bay NEP contracted with the University of South Florida to develop a
       regional atmospheric transport and dispersion model to determine the impact of NOX emissions
       on Sarasota Bay water quality.  Investigators modeled atmospheric dispersion, transport,
       chemical transformation, and deposition of NOX, nitric acid, and nitrate from stationary and
       mobile sources using CALMET/CALPUFF, a Lagrangian puff model. A regional domain of 250
       km by 500 km with a 20 km grid was modeled and included emissions from the metropolitan
       areas of Tampa, Orlando, Miami, and Fort Myers.  The model indicated that Sarasota Bay shared
       the same airshed as Tampa Bay and the airshed encompassed the entire modeling domain. The
       model further  indicated that mobile source emissions may be responsible for the majority (81
       percent) of atmospheric nitrogen sources to Sarasota Bay. One caveat of the modeling, however,
       was that modeled wet deposition was approximately a factor of five lower than measured fluxes.
       Furthermore, utilities were found to contribute disproportionately to wet deposition. Therefore,
       the total contribution of utilities to atmospheric deposition may be underestimated and that of
       mobile sources may be overestimated.

       Biological Effects of Atmospheric Deposition. Areas of the Sarasota Bay that receive the greatest
       percentage of nitrogen loading  from atmospheric sources are also associated with the highest
       water quality;  however, total nutrient loads to these segments are lower. Therefore, an
       investigation of the effects of atmospheric deposition on algal assemblages was initiated by the
       Sarasota Bay NEP through cooperative funding by SWFWMD and is being conducted by Mote
       Marine Laboratory. The growth response of phytoplankton to rainwater and nutrient additions is
       being determined by changes in major taxon composition, changes in particle size distribution,
       and through high performance liquid chromatography of photosynthetic pigment composition.
       The final results of this study should yield information on the major taxon composing a nutrient-
       rich (nearshore) and nutrient-depleted (offshore) algal regime, changes in growth rates as a result
       of rainfall and nutrient additions, and the potential of rainfall to act as a trigger for algal blooms
       in each regime. This research should provide information on the biological effects of
       atmospheric deposition.

       Stable Isotopes to Trace Nitrogen Sources. This on-going study funded by EPA will use stable
       nitrogen isotope ratios (15N/14N) to determine the relative contributions of different types of
       sources (e.g.,  wastewater treatment plant effluent, fertilizer runoff, animal waste, and combustion
       processes), including air deposition of nitrogen. Both nitrogen isotopes are naturally-occurring,
       but the ratio of 15N/14N varies depending on the source.  Measuring the ratio in emissions from
       different sources, in rainwater (wet deposition), and in phytoplankton, macroalgae, seagrasses,
       and the water column will help researchers identify the sources of atmospherically-deposited
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        nitrogen and its effects once it reaches the estuary. This is the only NEP air deposition study that
        measures nitrogen in the food web.

        Tampa Bay Atmospheric Deposition Projects (FL). The EPA and its partners in the Tampa
        Bay NEP (TBNEP) are currently working on eight separate but related projects to characterize
        the sources and impacts of atmospheric deposition to Tampa Bay and its watershed. A brief
        summary and status for each of these projects follows:

        (1)    An intensive monitoring site, sponsored by TBNEP and EPA's Great Waters program,
               was created to quantify nitrogen loading from atmospheric deposition to the surface of
               Tampa Bay, estimate relative contributions from wet and dry deposition, assess temporal
               variability of wet and dry deposition, and assess the relative contribution of different
               nitrogen species to atmospheric deposition in Tampa Bay. Preliminary results indicate
               that atmospheric deposition directly to the bay's surface accounts for approximately
               one-third of the new nitrogen delivered from all sources to the bay.

        (2)    The TBNEP initiated a study to estimate the contribution of atmospherically-deposited
               nitrogen to storm water loading from residential basins and estimate attenuation of
               nitrogen from atmospheric deposition in residential basins. The results indicated that
               approximately 15-20 percent of atmospherically-derived nitrogen was discharged from
               these basins per rainfall event.

        (3)    Toxic materials sampling, sponsored by TBNEP, EPA, Florida Department of
               Environmental Protection (FDEP), and the Environmental Protection Committee of
               Hillsborough County (EPCHC),  is being initiated to quantify metal concentrations and
               other contaminants in ambient air and to estimate potential loadings to water and the
               watershed.

        (4)    The TBNEP and the Great Waters program will fund ammonia sampling to map the
               pattern of ambient air ammonia concentrations.  Initial results from a pilot study indicate
               a strong gradient in ambient ammonia from the highly industrialized east bay to
               background levels at the existing intensive monitoring site. The overall objective is to
               develop a surface map showing relative concentrations of ammonia across the northern
               Hillsborough Bay area.

        (5)    Beginning in the fall of 1998, the FDEP funded a study in which the Florida State
               University and the University of Virginia used N-isotopic ratios to identify nitrogen
               source types affecting Tampa Bay. In particular, the researchers  are using isotopic ratios
               to attribute the relative contribution from different source types to atmospheric nitrogen,
               including combustion engines, coal-fired power plants, and diesel engines.

        (6)     Local governments and the TBNEP have cooperatively developed and are operating a
               long-term spatial monitoring network for atmospheric deposition in the Tampa Bay
               region. The purpose of the monitoring network is to track the contribution and temporal
               trends of atmospheric nitrogen loading throughout the region.

        (7)     The EPA is using RADM to identify relative contributions to nitrogen deposition in
               Tampa Bay from near and far sources. This effort also examines deposition to the bay
               and watershed.
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       (8)     In 1999, the FDEP is scheduled to initiate the Bay Regional Atmospheric Chemistry
              Experiment (BRACE) to (1) refine estimates of annual deposition of nitrogen species
              (HNO3, NH3, NH4NO3) to Tampa Bay and its watershed; (2) predict urban ambient ozone
              andPM2.5 concentrations; and, (3) estimate contributions of primary emissions from
              motor vehicles and stationary sources. This project will include high resolution
              deposition-daily event samples analyzed for nutrients and trace metals (including
              mercury), and a 1-year field monitoring program using a Differential Optical Absorption
              Spectrometer to measure sulfur dioxide, ozone, nitric oxide, nitrogen dioxide or nitrite,
              benzene, toluene, organics, metals, pesticides, and xylenes.

NOAA ACTIVITIES

National Estuarine Research Reserve System

       Under the 1972 Coastal Zone Management Act, Congress created the National Estuarine
Research Reserve System (NERRS) to enhance the scientific understanding and management of the
Nation's estuaries and coastal habitats.  The NERRS is a network of protected estuarine areas in which
Federal, State, and local partnerships work to promote stewardship, education, and research. As of
1999,23 reserves were designated as NERRS sites, encompassing about 960,000 acres of estuarine
waters, wetlands, and uplands. Four additional sites have been proposed and are in the process of
development and designation. See Figure 1-2 for the location of NERRS sites.  All NERRS estuaries are
included in the definition of "Great Waters."

       The NOAA's Estuarine Reserves Division is working with all NERRS  sites to implement a
System-wide Monitoring Program (SWMP) to track the status and trends in coastal ecosystem health.
This national monitoring program will be coordinated with other national and regional programs (i.e.,
NEP, EMAP, National Status and Trends). The overall goal of SWMP is to identify and track short-term
variability and long-term changes in the integrity and biodiversity of representative estuarine ecosystems
and coastal watersheds for the purpose of contributing to effective national, regional, and site specific
coastal zone management.

       Currently, SWMP is focusing on compiling water quality and weather data. Within 22 reserves
in the system  (Kachemak Bay NERR, Alaska was designated in February 1999 and is not yet
implementing SWMP), two locations - one non-impacted (baseline) and one non-point source impacted -
are designated as water quality monitoring sites where water quality parameters are measured every 30
minutes.  In addition, meteorological data collection began at each NERRS site in February 1998 to
allow local weather events to be related to water quality conditions (NOAA NERRS 1998).  Although
SWMP does not include atmospheric deposition monitoring, it will provide data useful for tracking the
ecological health of the coastal Great Waters.

Assessing Relative Nitrogen Inputs to Coastal Waters From the
Atmosphere

       With  funding from EPA's Office of Water and Great Waters program, NOAA's Air Resources
Laboratory (ARL) is performing a comprehensive assessment of nitrogen deposition to estuaries. In
1998, NOAA held two workshops involving experts from government, academia, and other institutions to
assemble and evaluate nitrogen deposition data and assessment procedures for approximately 40
estuaries on the Atlantic and Gulf of Mexico coasts. Workshop participants evaluated the adequacy of
existing nitrogen deposition data and attempted to develop standard nitrogen loading and mass balance
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 assessment methods.  Standard assessment methods are needed to improve comparisons between studies
 and locations.  The report is being produced in 2000.

 Coastal Zone Management Program

        The Coastal Zone Management Act of 1972 established the national coastal zone management
 (CZM) program, a voluntary partnership between the Federal government and the coastal States and
 territories of the U.S., with the following goals:

 •       Preserve, protect, develop, and (where possible) restore and enhance the resources of the
        Nation's coastal zone for this and succeeding generations;

 •       Encourage and assist the States and tribes to effectively exercise their responsibilities in the
        coastal zone to achieve the wise use of land and water resources of the coastal zone, giving full
        consideration to ecological, cultural, historic, and aesthetic values as well as the needs for
        compatible economic development;

 •       Encourage the preparation of special area management plans to provide increased specificity in
        protecting significant natural resources, reasonable coastal-dependent economic growth,
        improved protection of life and property in hazardous areas, and improved predictability in
        governmental decision making; and,

 •       Encourage the participation, cooperation, and coordination of the public, Federal, State, tribal,
        local, interstate, and regional agencies and governments affecting the coastal zone.

 Since 1974, at least 32 Federally-approved CZM State programs have protected more than 99 percent of
 the Nation's 95,000 miles of oceanic and Great Lakes coastline.

        As a component of the overall CZM effort, NOAA and EPA are currently developing a Coastal
 Non-Point Pollution Control Program for each CZM State program. The EPA has created pollution
 management and control measures for five non-point source categories: agricultural runoff, urban runoff,
 forestry runoff, marinas, and hydromodification.

 OZONE TRANSPORT COMMISSION (OTC)

        Section 184 of the CAA delineates a multistate ozone transport region (OTR) in the Northeast
 and requires specific additional NOX and VOC controls for areas in this region, including attainment
 areas.  In addition, section 184 of the CAA established the Ozone Transport Commission (OTC) to assess
 the degree of ozone transport in the OTR  and to recommend strategies to mitigate the interstate transport
 of pollution. States in the OTR include Connecticut, Delaware, Maine, Maryland, Massachusetts, New
 Hampshire, New Jersey, New York, Pennsylvania, Rhode Island, Vermont, parts of northern Virginia,
 and the District of Columbia.  The OTC has concluded that regional reductions of NOX emissions are
particularly important in reducing ozone.

       To further control NOX emissions in the OTR, the OTR States agreed to implement RACT on
major stationary sources of NOX and to a phased approach for additional controls, beyond RACT, for
power plants and other large fuel combustion sources.  This agreement, the OTC Memorandum of
Understanding (MOU) for stationary source NOX controls, was approved on September 27, 1994. All
 OTC States, except Virginia, are signatories to the MOU. The MOU establishes an emissions trading
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system to reduce the costs of compliance with the control requirements. In addition, in developing State
budgets for the NOX SIP call, EPA considered the NOX reductions each OTR State committed to in the
MOU.
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III.C
STATE, LOCAL, AND TRIBAL ACTIVITIES
       This section describes State, local, and tribal activities that will make significant contributions to
understanding or reducing atmospheric deposition of toxic air pollutants to the Great Waters. Unlike the
regional and waterbody-specific programs and activities described in Section III.B, these programs are
led by State, local, or tribal agencies, not Federal agencies. However, EPA and other Federal agencies
are partners in some of the programs.
STATE AND LOCAL ACTIVITIES

       The projects described below are examples of State and local projects that support the goals of
the Great Waters program. It is likely that there are many additional relevant State and local programs
that were not identified for this report.

Ammonia Study in North Carolina: An Example of Progress in
Understanding

       The State of North Carolina recognizes nitrogen enrichment and eutrophication as a serious
environmental concern for certain coastal plains, nitrogen-sensitive estuaries, and coastal waters (see, for
example, the discussion of the Albemarle-Pamlico Estuary on page 111-42). Atmospheric emissions and
deposition of ammonia from intensive livestock operations are the subject of particular attention, in
addition to atmospheric nitrates and water-borne discharges and runoff. A workshop on atmospheric
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nitrogen compounds was held at North Carolina State University (NCSU) in March 1997 (Aneja et al.
1998).

       The State of North Carolina Department of Environment and Natural Resources, in conjunction
with NCSU, University of North Carolina at Chapel Hill, U.S. Department of Agriculture, and EPA, has
begun a coordinated research program on ammonia emissions from large-scale livestock operations, and
on the transport and deposition of ammonia, with possible effects of eutrophication in aquatic systems
and on forest and crop production.  Ammonia and other NHX compounds have much different
atmospheric lifetimes and interactions in the environment than do oxidized nitrogen compounds or NOX
(primarily NO and NO2).  The research program on nitrogen compounds will quantify the emissions,
verify or improve existing emission factors, and begin modeling studies of deposition patterns, especially
in the Coastal Plains of North Carolina.

       Several aspects of the research program are already under way. New data on emissions of
ammonia from waste lagoons and animal barns/houses have been gathered and are under review. Studies
of deposition, deposition velocities, and movements of ammonia in the environment have begun, and a
nitrogen balance is being developed to better understand sources, sinks, and exchanges of nitrogen
compounds.  Emissions data for ammonia and NOX sources have been produced. Modeling using the
Regional Atmospheric Deposition Model (RADM) and Models-3 is under way. A general conference on
ammonia and other atmospheric nitrogen compounds was held in June 1999,  in addition to intensive
reviews of the North Carolina research program as individual studies are completed. These analyses will
contribute to an understanding of which sources or source categories are generating the most
environmental impact and which should be the focus of additional management efforts (Personal
Communication with George Murray, NC DENR, September 9,  1998).

Maryland's Power Plant Research Program

       The Maryland Department of Natural Resources (DNR), Power Plant Research Program, in
cooperation with other partners, has several projects ongoing in the Chesapeake Bay watershed. These
include applying the CALPUFF model to develop estimates of Maryland's contribution of atmospheric
deposition of nitrogen to the Chesapeake Bay; using CALPUFF to assess the implications of possible
utility emissions trading under title I of the CAA and impacts of deregulation on power plant emissions.
The DNR also supports studies on air toxics, particularly mercury from coal-fired power plants, the
migration of metals and nitrate through watersheds (including coastal wetlands and forests), and
economic resource valuations associated with implementation of the CAA.

Florida's Mercury Rule: Progress in Reducing Atmospheric Mercury
Emissions

       The amount of mercury in Florida's municipal solid waste stream has been dropping rapidly due
to the implementation of statutes and rules designed to reduce or replace mercury in the manufacture of
widely used products, recycle mercury-containing items such as fluorescent lamps, and control mercury
at the point of release. One tool the Florida Department of Environmental Protection uses to reduce
atmospheric mercury emissions is a rule (i.e., "The Mercury Rule") adopted in 1993 that limits mercury
emissions from municipal waste combustors (MWCs) to a level that is more stringent than the applicable
EPA standard.  Florida's strict mercury emissions standard is currently being met by over half of the
MWCs in the State, and all MWCs in the State are expected to meet the standard in the year 2000. The
rule also requires that every MWC unit perform a mercury stack test at least once each year. With over 5
years of test data available, it is clear that the uncontrolled (i.e.,  no up-front sorting of waste and no fine
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participate control) MWC units in Florida are emitting about 65 percent less mercury than just 5 years
ago. With post-combustion controls (e.g., carbon injection) designed to capture mercury, the stack
emission rates at some Florida MWCs have been reduced an additional 80 percent.  In 1997, the average
mercury emission rate for south Florida MWC units was 31 u.g/dry standard m3 at 7 percent oxygen
(Memorandum from Michael M. Hewett to Howard L. Rhodes, August 26,  1998).

South Florida Mercury Science Program
        Mercury bioaccumulation in wildlife
is extensive in Florida (FDEP 1996). High
levels of mercury in several species offish
have resulted in bans or restrictions on their
consumption in over half of the fresh waters of
the State.  The entire Florida Everglades is
covered by fish consumption bans.  In
addition, the mercury problem places at risk a
variety of wildlife within the Everglades, most
notably top predators such as the endangered
Florida  Panther. The contribution of
atmospheric deposition of mercury to this
regional environmental problem is a subject  of
several current research efforts.
 Participants in the South Florida Mercury Program

Florida Department of Environmental Protection
Florida Game and Fresh Water Fish Commission
South Florida Water Management District
U.S. EPA
U.S. Geological Survey
National Park Service
U.S. Fish and Wildlife Service
U.S. Army Corps of Engineers
Florida Electric Power Coordinating Group
Electric Power Research Institute
Florida Power & Light Company
Florida International University
Florida State University
University of Florida
        The South Florida Mercury Science
Program is a broad, multidisciplinary effort by scientists from State and Federal agencies, State
universities, industry groups, and others (see sidebar) working together to understand and address
mercury bioaccumulation in South Florida  (FDEP 1996). The program is designed to determine the
following:

        Potential risks to humans and wildlife from mercury in South Florida;

        How mercury enters the aquatic food chain and concentrates in predators;

•       Chemical and biological pathways for transformation of inorganic mercury into methylmercury;

•       The origin of mercury in South Florida's atmosphere and waters;

•       How mercury moves through air, water, and soil; and,

•       Actions that could be taken to reduce levels of mercury in fish and wildlife.

        The Florida Everglades is currently the focus of the most in-depth and comprehensive research
on mercury in the environment.  Scientific findings in the areas of atmospheric mercury deposition,
aquatic chemistry and cycling of mercury, and bioaccumulation of mercury in food chains have broad
application to many of the Great Waters (see Chapter II for information on mercury in the Great Waters).
In addition, scientists studying mercury in South Florida hope to incorporate their findings into a model
that could be applied to other ecosystems.
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       Studies to date identified the atmosphere as the primary source (>95 percent) of mercury
impinging on the Everglades. Much remains to be learned, however, about the sources of mercury as
well as its fate in the environment.  Several of the key projects currently under way are described below.

       Florida Atmospheric Mercury Study (FAMS)

       The FAMS was a large, regional-scale study conducted from 1992-1996 and designed to measure
long-term temporal and spatial trends in atmospheric mercury transport and deposition in Florida. While
most of the sites were remote, some were extremely close to or in urban areas (e.g., the Fort Meyers site).
Data were collected over a 3-year period at nine sites  (seven in South Florida), including monthly
integrated samples of mercury in rainfall and weekly integrated vapor phase and particulate phase
mercury samples. Preliminary analysis of the FAMS  data indicated the following:

•      More than 90 percent of the mercury found in the Everglades was from atmospheric deposition,
       while less than 10 percent was from agricultural runoff;

•      Wet deposition of mercury to South Florida was high - approximately double what has been
       observed at other North American remote sites;

•      Particulate mercury levels were relatively low;

•      Mercury deposition exhibited a strong seasonal trend — 85 percent of annual deposition occurs in
       the summer; and,

•      Slight spatial trends were evident in South Florida.

       Although the FAMS study design limited its ability to differentiate between local, regional, and
global sources of atmospheric mercury, the researchers conducting the study suggested that local source
contributions of mercury to the Everglades are less dominant (<30 percent) than regional and/or global
contributions (Guentzel et al. 1995).

       South Florida Atmospheric  Mercury Monitoring Pilot Study (SoFAMMS)

       The SoFAMMS was a short-term, very intensive pilot study focused on determining the ability of
state-of-the-art sampling, measurement, and modeling techniques to track mercury from sources to
receptors. As a complement to FAMS, SoFAMMS was carried out to  assess the influence  of local
mercury sources in the developed Southeast Florida Coast on the atmospheric deposition of mercury to
the Everglades. Over a 1-month period (August 6, 1995 - September 6, 1995), SoFAMMS measured
mercury emissions from three source  types (municipal waste incinerator, medical waste incinerator, and
coal-fired cement plant), meteorological conditions across the study area (surface and upper air), and
several forms of atmospheric mercury and deposition at 17 ambient monitoring sites. The data were
subjected to extensive dispersion, receptor, elemental composition, and meteorological modeling. The
study found a wide range in spatial variability of mercury wet deposition. Volume weighted mean
concentrations ranged from 13 to 31 ng/1 across the 17 sites. The highest mercury concentrations were
observed in the urban areas (19-31  ng/1). The sites in the Everglades were lower but still elevated,
ranging from 13-20 ng/1. Those precipitation events in the Everglades with high mercury concentrations
were also found to contain elevated concentrations of other trace element species known to be tracers for
anthropogenic sources.  The precipitation data were subjected to extensive meteorological, atmospheric
dispersion, and source apportionment modeling.  The results of the modeling indicated that greater than
70 percent of the mercury wet deposited to the Everglades were accounted for by waste incineration and
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oil combustion sources, contrary to the preliminary FAMS results that indicated that local sources
contribute less than 30 percent (Dvonch et al. 1998).  Furthermore, monitoring data from these three
sources were the first data to indicate that a high percentage of emissions from incinerators are in the
form of divalent (reactive) mercury. Based on these results, EPA's Office of Research and Development
has begun methods development efforts for ambient and source mercury speciation techniques.

       Mercury Cycling in the Florida Everglades Project

       The overall objective of this project is to provide resource managers scientific information on the
hydrological, biological, and geochemical processes controlling mercury cycling in the Everglades
(Krabbenhoft 1996).  Specific areas of research include geochemical studies of mercury, mercury
methylation and demethylation studies, interactions between dissolved organic carbon and mercury,
mercury accumulation in sediments, physical and chemical processes in peat, sulfur cycling studies,
biological uptake of mercury and lower food chain transfer pathways, and groundwater/surface water
exchange. The USGS is leading this research effort, and participating scientists are from USGS,
SFWMD, FDEP, EPA, Wisconsin Department of Natural Resources, and University of Wisconsin-
Madison.

       South Florida Ecosystem Assessment Project

       This project is part of the EPA Region IV Regional Environmental Monitoring and Assessment
Program (R-EMAP), which was designed to monitor the condition of ecological resources in South
Florida (Stober et al. 1996). The project was intended to address several issues that threaten the
Everglades ecosystem, including mercury contamination.

       The project assessed mercury concentrations (e.g., in water, soil, algae, mosquitofish) at
approximately 700 sampling sites.  Interim findings provide an indication of the spatial distribution of
mercury within the Florida Everglades as well as the levels of mercury contamination at various trophic
levels in the food chain (Stober et al. 1996).  The spatial distribution of mercury within the Everglades is
relevant to the Great Waters research because it helps define the environmental conditions under which
methylation and bioaccumulation occur.  For example, the highest concentrations of methylmercury were
found in fish, birds, and algae from the marsh sites between Alligator Alley and Tamiami Trail. North of
Alligator Alley, the organic compounds and reduced sulfate are believed to bind the mercury and
methylmercury so it is not available for uptake by organisms. South of Tamiami Trail, lower
concentrations of sulfate and total phosphorous probably limit microbial methylation and organic
production rates, respectively.  In addition, researchers have found methylating bacteria associated with
periphyton (attached algae) mats, which are more common in the marsh sites between Alligator Alley  and
Tamiami Trail.

       Additional sampling has been conducted, and an updated report is expected soon. The study
results will be used to answer the seven questions identified for mercury. The EPA Region IV is also
studying the complex interactions between mercury contamination and other issues, such as
eutrophication, habitat alteration, and hydropattern modification.

Midwestern Pollution Prevention Activities

       Since the Second Great Waters Report to Congress, State and local pollution prevention
activities have helped to reduce releases of Great Waters pollutants of concern. Six such activities in the
Midwest are described below.
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State Pesticide Clean Sweep Programs

       Over time, unwanted pesticides have accumulated in the barns, sheds, and storage areas of
farmers, ranchers, golf courses, pest control operators, and other pesticide users. The pesticides may be
unwanted for a variety of reasons - the products could be banned, unusable, or not needed. Farmers and
other small businesses may have difficulty determining how to properly manage these pesticides since
some (but not all) may be hazardous wastes when they are disposed.

       States have addressed the problem of accumulated unwanted pesticides by establishing waste
pesticide collection and disposal programs, commonly called "Clean Sweeps." These programs provide a
simple way to properly dispose of unwanted pesticides at little or no cost to the participants.  Because
each State has designed its program to fit its own needs and funding sources, there is no single "typical"
Clean Sweep program.  Some of the variations include the following:

•      Format - The pesticides may be collected by holding single-day collection events, picking up
       pesticides from individual farms, or establishing permanent collection sites;

•      Type of waste collected— Waste pesticide collections may be combined with household
       hazardous waste programs either by consolidating all of the waste or by collecting both waste
       types at a single site but handling them separately;

•      Organizer — The programs may be run by a State regulatory agency, the agricultural extension
       service, a county, or a combination of these;

•      Funding source — Clean Sweep programs may be funded through State pesticide registration
       fees, State legislature appropriations, Federal grants, or fees assessed to participants; and,

•      Participants — Some programs are limited to farmers, while others are open to households and/or
       small businesses.

       State Clean Sweep programs have been extremely successful in removing pesticides from the
environment and ensuring the proper management of these materials. A few highlights of their
accomplishments through 1997 include the following:

•      Clean Sweep programs have collected and disposed of more than 12 million pounds of
       pesticides;

•      Over 40 States have collected and disposed of some pesticides;

•      About 20 States have had on-going Clean Sweep programs since 1995 (or earlier); and,

•      The collections bring in an average of 200-300 pounds of pesticide per participant (where 100
       pounds is equivalent to about 11 gallons of liquid pesticide).
In addition, Table III-7 presents the amounts of pesticides that have been collected nationwide based on
the limited data that have been collected. Despite this progress, efforts in this area need to continue.
There is a large, but unquantified, amount of unused and/or unwanted pesticides that needs to be
collected.
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                                         Table 111-7
       Pounds of Pesticides Collected through Clean Sweep Programs Nationwide
Pesticide
DDT
Toxaphene
Chlordane
Mercury
Dieldrin
Average Percent (per
collection)
3.86
2.98
1.46
1.53
0.48
Total Amount in
U.S. (pounds)
463,200
357,600
175,200
183,600
57,600
Illinois Clean Sweep Partners for PCB and Mercury Wastes

       The presence of mercury and PCBs in the environment is partially attributable to their
widespread use in commercial and consumer products, particularly electrical equipment. While newer
technologies in products, such as transformers, capacitors, thermostats, and switches, are PCB and
mercury free, older products are not and still pose potential health and environmental risks. Currently,
much of the PCB- and mercury-containing equipment encountered during maintenance, remodeling, and
demolition work is disposed of in the municipal solid waste stream.  Because mercury and PCBs may be
released into the environment throughout the disposal process - from the point of disposal, the garbage
truck, a transfer station, and the solid waste landfill - the PCB and Mercury CleanSweep Partnership in
Cook County, Illinois is attempting to reduce the amount of PCB- and mercury-bearing equipment
entering the municipal solid waste stream.

       The Cook County PCB and Mercury CleanSweep Partnership is a nonregulatory program
sponsored by public and private entities. The CleanSweep Partners have joined resources to help small
businesses and local governments identify and properly manage PCB- and mercury-containing materials
through a convenient and cost saving program. Through literature and training, the CleanSweep
Partners' goal is to educate and assist small businesses and local agency field personnel in a voluntary,
public-private initiative to educate and motivate small business operators, particularly electrical and
demolition contractors, to manage and dispose of mercury- and PCB- bearing equipment in identifying,
handling, transporting, and disposing of mercury- and PCB-bearing equipment. For more information,
call the CleanSweep Partners hotline at 1-888-SWEEP22 or visit the web site at
www.erc.uic.edu/cleansweep.

       The CleanSweep Partners are Commonwealth Edison, Electric Association, City of Chicago
Department of the Environment, Cook County Department of Environmental Control, Metropolitan
Water Reclamation District of Greater Chicago, Illinois Environmental Protection Agency, EPA, Clean
Harbors Environmental Services, National Oil Recyclers Association, Safety-Kleen Corp., North
Business - Industrial Council (NORBIC), and the University of Illinois at Chicago School of Public
Health.

Michigan Mercury Pollution Prevention Task Force

       The Michigan Mercury Pollution Prevention task force, which first convened in August 1994,
has been active in many mercury pollution prevention activities throughout Michigan.  Significant
accomplishments include (1) a household hazardous waste collection program in 22 counties sponsored
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Major Programs and Activities
by the Michigan Department of Environmental Quality (MDEQ), resulting in the collection of 200
pounds of mercury; (2) distribution of 16,000 copies of the "Merc Concern" brochure throughout
Michigan; (3) development of a mercury pollution prevention web page at http://www.deq.state.mi.us/
ead/p2sect/mercury; and, (4) distribution of mercury outreach materials to science teachers.  Additional
accomplishments of the Michigan Mercury Pollution Prevention task force are described below.

•      The Michigan Mercury Pollution Prevention task force worked with the automobile
       manufacturers to phase out the use of mercury in automobiles, including identification of several
       uses of mercury in automobiles (e.g., in switches, anti-lock brakes, active ride control devices).
       To date, the manufacturers have made great progress in eliminating mercury switches from
       automobiles.

•      A cooperative effort initiated by the Detroit Wastewater and Sewage Department that included
       the National Wildlife Federation, the Michigan Dental Association, and MDEQ collected
       approximately  1,400 pounds of elemental mercury from 400 dentists at 11 drop-off sites.

•      The MDEQ, Michigan Department of Agriculture, Michigan Farm Bureau, Michigan
       Department of Community Health, Michigan Milk Producers Association, Independent
       Cooperative Milk Producers, and Michigan State University collaborated on a dairy farm
       mercury manometer pilot collection effort in two counties in Michigan.  A total of 16 out of 18
       manometers were replaced with a mercury-free substitute, and 12 pounds of mercury were
       collected and properly disposed. This program may be expanded Statewide.

•      Detroit Edison identified 1,500 pounds of mercury used in current product applications and
       eliminated its use. Consumers Energy identified over 2,900 pounds of mercury used in product
       applications in 1996 and is now replacing mercury-containing products with mercury-free
       alternatives.

Indiana Statewide Mercury Awareness Program

       The Indiana Statewide Mercury Awareness Program is a State and local partnership dedicated to
identifying commercial uses of mercury, investigating pollution prevention opportunities, and developing
and implementing outreach strategies. In October 1998,  the Indiana Department of Environmental
Management initiated an effort to collect and recycle household items containing mercury.

Minnesota Mercury Reduction Initiative

       In 1997, the Minnesota Pollution Control Agency (MPCA) began the Mercury Contamination
Reduction Initiative, aimed at reducing mercury contamination in fish in Minnesota lakes. A major part
of this effort is to receive advice and comments from the public regarding the goals of the initiative. The
MPCA established a Mercury Advisory Council that includes representatives from government, business,
and environmental groups.

       The council's charter is to devise a package of recommendations to reduce mercury
contamination in the environment. In January 1999, the  council agreed to adopt a goal of reducing
mercury releases to Minnesota's air and water by 70 percent (compared to 1990 levels) by 2005, to be
established in statute in the upcoming legislative session.
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                                                               Major Programs and Activities
       The recommendations that the council voted to forward to the MPCA include the following:

•      Encouragement of voluntary commitments on the part of sources of mercury emissions (e.g.,
       power plants, taconite facilities, sewage sludge incinerators) to reduce or work toward reducing
       mercury emissions;

       Development of a package of seven strategies that the State will advance at the national level to
       encourage States and the Federal government to act in concert to reduce national mercury
       emissions; and,

       Development of a package of strategies to persuade consumers to reduce their purchases and use
       of mercury-containing products and encourage counties to collect more mercury-containing
       waste in their household hazardous waste pickups.

Western Lake Superior Sanitary District (WLSSD) Pollution
Prevention Efforts

        The WLSSD is the largest wastewater treatment facility that discharges to the Lake Superior
watershed.  The WLSSD developed a multimedia mercury zero discharge pilot project with hospitals,
clinics, educational institutions,  laboratories, and dental practices. As part of this effort, WLSSD
partnered with the Northeast District Dental Society to develop recycling procedures for materials
containing amalgam particles. In the first year of the project, over 500 pounds of waste material
containing amalgam was  collected for recycling. Based on the results of the WLSSD pilot project,
WLSSD compiled the Blueprint for Mercury Elimination, which is a document designed for use by other
wastewater treatment facilities in developing and implementing mercury reduction programs.

Northeast States and Eastern  Canadian Provinces Mercury Study

       During 1996 and 1997, the Northeast States (i.e., Connecticut, Maine, Massachusetts, New
Hampshire, New Jersey, New York, Rhode Island, Vermont)  and Canadian Eastern Provinces (i.e., New
Brunswick, Newfoundland and Labrador, Nova Scotia, Prince Edward Island, and Quebec) held a series
of meetings and workshops to address shared mercury pollution issues. In June 1997, the New England
Governors and Premiers of Eastern Canada subsequently signed a Mercury Resolution that called for
cooperative efforts including the completion of the Northeast Mercury Study. The study, which was
completed in February  1998, reflects the combined contribution of State and provincial air, waste, and
water management agencies throughout the northeastern U.S. and eastern Canada. It is an informational
resource and serves as the foundation for future regional activities, including the development of a
coordinated action plan (see below) to reduce the environmental and public health impacts of mercury
pollution.

       The study reports on emission inventories, transport and deposition modeling, multimedia
monitoring  and assessment, communication (public and political outreach), and control strategies and
effectiveness of controls.  The report recommends (1) identifying mercury as a hazardous air contaminant
under State air regulations to achieve the most stringent emission rate; (2) conducting an emissions
inventory of airborne sources of mercury; (3.) implementing the Federal standards for municipal waste
combustors and medical waste incinerators by the year 2000;  and, (4) forming in-State task forces to
assess, evaluate, and communicate mercury-related public health and environmental information.
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Chapter III
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Northeast Mercury Action Plan

       In June 1997, the Conference of New England Governors and Eastern Canadian Premiers
charged its Committee on the Environment with developing a regional Mercury Action Plan.  The plan
was released in May 1998 with the endorsement of the New England Governors and Eastern Canadian
Premiers.  The Mercury Action Plan identifies steps to address those aspects of the mercury problem in
the Northeast that are within the control or influence of the region. The ultimate goal of the plan is the
virtual elimination of anthropogenic mercury releases in the northeastern U.S. and eastern Canadian
Provinces. In all, the plan lays out 45 specific recommendations addressing the following:

•      The establishment of a Regional Mercury Task Force to coordinate the implementation of the
       plan;

•      Mercury emission reduction targets for identified sources such as municipal solid waste
       combustors, medical waste incinerators, sludge incinerators, utility and non-utility boilers, and
       industrial and area sources;

•      Source reduction and safe waste management practices, including recycling;

•      Outreach and education, especially for high-risk populations;

•      Research, analysis, and strategic monitoring to further identify and quantify sources of mercury
       deposition and to monitor deposition patterns and develop meaningful environmental indicators
       to measure and track progress; and,

•      Mercury stockpile management.

TRIBAL ACTIVITIES

       Deposition of toxic air pollutants to the Great Waters adversely affects resources (e.g., fisheries)
that are of particular cultural and economic importance to many Native American tribes. This section
describes partnerships between tribal, State, and Federal governments that have enabled tribes to better
assess the ecological and human health risks posed by exposure to the Great Waters pollutants of
concern.  Financial and/or technological support from Federal and State sources (through projects such as
the Effects on Aboriginals from the Great Lakes Environment (EAGLE), the Baseline Assessment
Project, and the American Indian Lands Environmental Support Project) and programs initiated by tribal
governments (such as aquaculture, CWA section 106 programs, or educational programs) are enabling
tribes to successfully conduct better quality assessments of their environment.

Effects on Aboriginals from the Great Lakes Environment (EAGLE)

       The EAGLE, a partnership between the Assembly of First Nations and the Medical Services
Branch of Health Canada, is  a community-based epidemiological project to research health effects of
environmental contaminants potentially affecting approximately 100,000 people in 63 First Nation
communities in the Great Lakes basin.  The EAGLE's main activities to date include (1) a survey offish
and wild meat consumption in Great Lakes First Nations communities, (2) a program to establish safe
fish consumption guidelines  for First Nations communities, and (3)  a health survey accompanied by
blood and tissue sampling. Recognizing that even the perception of contamination can have a
tremendous impact on the relationship that First Nation communities have with the land, studies to assess
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                                                                                   Chapter III
                                                                Major Programs and Activities
the socio-cultural impact of environmental contamination are also being conducted.  Future activities for
the EAGLE project will focus on communication/outreach strategies and helping communities develop
environmental plans.

Baseline Assessment Project
                                                             Draft Baseline Assessment
                                                                 Priority Data Sets

                                                         Ambient air monitoring
                                                         Air toxics
                                                         • Point and non-point source loadings
                                                         • Fish consumption advisories
                                                         Ecological status of wetlands
                                                         • Contaminated sediment
                                                         Pesticide use
                                                         • Blood lead screening
                                                         PCB ballast in buildings
       The EPA initiated a Baseline Assessment of
Indian Country in order to provide easy-to-use and
accessible environmental data to assist tribal governments
and EPA in making sound environmental decisions. A
work group, led by the American Indian Environmental
Office (AIEO), is gathering and analyzing the existing
information on environmental conditions in Indian
country.  In addition, EPA's program offices have
identified 37 priority data sets that need to be developed
to track environmental management activities (see sidebar
for priority data sets relevant to the Great Waters
program). Next, EPA will develop a data management
system to meet the data needs. In addition, EPA's Office of Water is reassessing the 2,200 hydrologic
unit basins of the U.S.  so that tribal lands can be geographically located within specific watersheds.13
Therefore, environmental conditions on tribal lands, as evaluated through the baseline assessment, will
be comparable to conditions on non-tribal lands within the same watersheds.

American Indian Lands Environmental Support Project

       Established by EPA's Office of Enforcement and Compliance Assurance, the American Indian
Lands Environmental Support Project (AILESP) is designed to assess the impact of toxic chemicals from
permitted point sources on tribal lands.  The AILESP integrates release data for multiple sources and
media, and information on the potential impact of a variety of contaminants with compliance histories of
facilities within 3.1 miles of tribal lands. The information is assembled into a geographic information
system (GIS) to help users understand the sources and impacts of pollutants on tribal lands.  Preliminary
AILESP  data include release of trace metals (including cadmium, lead, and mercury) and nitrogen
compounds (including nitrogen dioxide, ammonia,  nitrate, and NOX) from certain facilities.

Aquaculture

       Interest in aquaculture in tribal communities has recently been stimulated by the desire to
preserve  ancestral traditions while avoiding health risks associated with the consumption of contaminated
fish. Aquaculture is based on the premise that uncontaminated fish can be obtained by breeding and
rearing them at uncontaminated sites (e.g., isolating them from contaminated  sediments) and feeding
them high-quality commercially-supplied food (i.e., circumventing the contaminated food chain).
Buttner (1997) aided aquaculture efforts by three tribal communities: Akwesasne Mohawks (St. Regis
Mohawks), Mohawks of the Bay of Quinte, and Ojibway of Sucker Creek.  Although the programs had
varying degrees of success, it was clear that aquaculture had the potential for  producing "clean" fish,
while creating jobs and minimally impacting the environment.
 ' Personal Communication with Ed Liu, EPA. October 26, 1998.
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Chapter Eff
Major Programs and Activities
Tribal Air Quality Programs

       In 1998, EPA issued a rule that authorizes tribes to develop air quality programs under the CAA.
The EPA has also increased its financial support and technical assistance to tribes that choose to adopt
air quality programs. Numerous tribes have begun to develop these programs, including programs for
collecting air quality monitoring data and programs that address toxic pollutants that are generated in
Indian country. The EPA will regulate larger sources of air pollution in Indian country until tribes
develop their own regulatory programs.  The EPA is also updating data on the number, type, and location
of sources of toxic pollutants that are located in Indian country.
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III.D
INDUSTRY ACTIVITIES
       A number of industry activities currently contribute to reduced emissions of Great Waters
pollutants of concern.  These industry activities were developed by cooperative partnerships involving
industry groups, EPA, and other agencies. Some of the activities are noted under other sections of this
chapter, such as under the Michigan Mercury Pollution Prevention Task Force. The EPA has found that
nonregulatory partnerships can be an effective means of achieving or surpassing environmental goals. In
addition, industry is phasing out the use of some Great Waters pollutants of concern in the manufacture
of certain products.  For example, the amount of mercury used for the manufacture of electric switches
and thermostats has been decreasing because of the shift to solid state devices and other alternatives (see
Volume II of EPA's 1997 Mercury Study Report to Congress (U.S. EPA 1997e)).
CHLOR-ALKALI INDUSTRY MERCURY REDUCTION GOAL

       In July 1997, the Chlorine Institute, on behalf of its members, committed to reduce mercury use
in the chlor-alkali industry by 50 percent to help the U.S. achieve the mercury reduction goals of the
Binational Toxics Strategy (see page 111-66). The baseline average annual mercury usage by mercury cell
chlor-alkali plants for the 1990-1995 period was 160 tons per year. The industry's goal is to reduce
mercury usage to 80 tons per year by 2005. In addition, as part of the agreement, the Chlorine Institute
will submit an annual progress report to EPA. The first annual report was submitted to EPA in May
1998.

       To ensure that appropriate oversight is provided for monitoring the progress in achieving the
commitment, the Chlorine Institute's Board of Directors established ad hoc committees for technical and
management issues. All chlor-alkali producers using mercury cell technology are represented on both
committees. In addition, seven technical task groups were formed to address specific issues such as
identification of new mercury reduction control techniques and preparation of guidance documents to
assist industry members in achieving mercury reduction goals.
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Chapter VI
Major Programs and Activities
VOLUNTARY MERCURY AGREEMENT WITH NORTHWEST
INDIANA STEEL MILLS

       On September 25, 1998, the Lake Michigan Forum, the Indiana Department of Environmental
Management (IDEM), and EPA signed a voluntary agreement with three northwest Indiana steel mills,
including Bethlehem Steel Burns Harbor, Ispat Inland Inc. Indiana Harbor Works, and U.S, Steel Gary
Works. The mills agreed to inventory mercury in equipment, materials, storage, and waste streams, and
to develop facility-specific plans for mercury pollution prevention. The companies signed the agreement
as part of the Lake Michigan Primary Metals Project, which is a pollution prevention effort initiated by
the Lake Michigan Forum. The Lake Michigan Forum is a stakeholder group that provides input to EPA
on the Lake Michigan Lakewide Management Plan and includes representatives from academia,
business, environmental and sportfishing groups, and local governments.

       The agreement will result in facility-specific reduction plans outlining pollution prevention
activities through equipment substitutions, purchasing practices, recycling, better management, and
employee education.  The EPA (including the Mercury Work Group of the Binational Toxics Strategy)
and IDEM will provide the companies with information on typical mercury sources, substitutions for
mercury in equipment, and recycling options.  Both agencies and the Lake Michigan Forum will receive
progress reports from the mills.  The reports will also be available to the public. The forum will promote
the initiative and its results throughout the Lake Michigan basin. This effort could serve as a model for
other companies and industries that use mercury-containing devices.

AMERICAN HOSPITAL ASSOCIATION MOU
       On June 24, 1998, the American Hospital
Association (AHA), which consists primarily of
health care provider organizations, established a
Memorandum of Understanding (MOU) with
EPA's Office of Prevention, Pesticides, and
Toxics and EPA Region V. The MOU is intended
to provide AHA members with enhanced tools for
minimizing the production of pollutants and
reducing the volume of waste generated. The
information should also reduce the waste disposal
costs incurred by the health care industry.
                                  Hospitals Produce Mercury Wastes

                            "Medical waste incinerators are the fourth largest
                            releasers of mercury to the environment, constituting
                            approximately 10 percent of all emissions sources,
                            and hospitals are responsible for producing 1 percent
                            of the total municipal solid waste in the entire
                            country." (U.S. EPA 1998d)
       The MOU outlined multiple primary goals and activities designed to aid in the exchange of
information between EPA and the health care industry. Highlights include the following:

•      Development of a Mercury Waste Virtual Elimination Plan to eliminate mercury-containing
       waste from the health care industry waste stream by the year 2005;

•      Development of a Total Waste Volume Reduction Plan to reduce the volume of waste generated
       by the health care industry by 33 percent by 2003 and by 50 percent by the year 2010; and,

•      Investigation of pollution prevention opportunities with respect to ethylene oxide and other
       persistent, bioaccumulative, and toxic pollutants.
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                                                                                     Chapter III
                                                                  Major Programs and Activities
       This MOU specifically supports the goals and objectives of the PBT Initiative, the Mercury
Action Plan, and the Waste Minimization National Plan, and is also expected to help reduce atmospheric
deposition of mercury and other persistent toxic pollutants to the Great Waters (U.S. EPA 1998d).

ELECTRIC POWER RESEARCH INSTITUTE STUDIES

       The Electric Power Research Institute (EPRI) has a broad-based research program which
conducts a large amount of research cooperatively with Federal and State agencies. Research sponsored
by EPRI  on air toxics and nitrogen is the largest privately-funded program in the U.S. Current air toxics
studies focus on mercury, nickel, dioxins, and arsenic. These studies include atmospheric global,
regional, and plume modeling of mercury; measurement of natural mercury fluxes; historic patterns of
mercury deposition (sediment and peat cores); environmental effects and mercury cycling in lakes;
human health effects of mercury exposure; and, mercury and multimedia risk assessment. Research
characterizing emissions of air toxics has,  and is, leading to better emission inventories relevant to a
number of air quality issues.  The EPRI also conducts or sponsors research in atmospheric chemistry and
physics, including atmospheric modeling and measurement of PM, ozone, and their precursors (including
nitrogen species). On-going nitrogen research of specific interest to the Great Waters includes a small
study on  measurement of organic nitrogen in precipitation near the Chesapeake Bay; development of a
nutrient model for the Chesapeake Bay airshed, watershed, and bay; a study on the feasibility of using
isotopic composition of ammonium in wet deposition for source attribution; and, research on the effects
of nitrogen speciation in atmospheric deposition on phytoplankton community composition and
productivity.  In addition, EPRI is a contributor to a study with substantial funding from EPA and NOAA
that is being carried out by the Ocean Studies Board and Water Science and Technology Board of the
National  Research Council's Commission on Geosciences, Environment, and Resources to assess
eutrophication, coastal processes, and watershed management. The study report, due in spring 2000, will
review existing knowledge and make recommendations for action and research to reduce eutrophication
in coastal ecosystems through more effective watershed management.
                                      Businesses for the Bay

  Since its launching by the Chesapeake Executive Council in 1996, more than 230 businesses have joined the
  Businesses for the Bay.  This includes not only private industries, but State and local government facilities as
  well. Under this voluntary program, businesses commit to pollution prevention  activities and goals. In 1998,
  member facilities voluntarily reported that they had reduced or recycled 222 million pounds of waste.  Of these,
  13 facilities reported a resulting cost savings of $1.4 million, and 15 of the facilities offered pollution prevention
  training to 6,300 employees.  Businesses have also volunteered more than 70 of their technical experts to act
  as mentors to offer pollution prevention advice to other companies on an as-needed basis. In 1998,
  Businesses for the Say received 2 national awards from the National Pollution Prevention Roundtable and the
  National Environmental Education and Training Foundation for its successes as a model program.
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Chapter III
Major Programs and Activities
III.E
WORK WITH OTHER COUNTRIES
       The U.S. works with other nations on many issues concerning shared resources (e.g., the Great
Lakes) and transboundary environmental problems. A number of international activities concern the
Great Waters and Great Waters pollutants of concern. International activities relevant to air deposition
of pollutants to the Great Waters are discussed below.
CANADA - U.S. BINATIONAL TOXICS  STRATEGY

       On April 7, 1997, the U.S. and Canada signed the Great Lakes Binational Toxics Strategy (BNS).
The BNS sets forth a collaborative process by which Canada and the U.S. will work toward the goal of
virtual elimination of persistent toxic substances resulting from human activity from the Great Lakes
basin, in order to protect and ensure the health and integrity of the Great Lakes ecosystem. The goal of
virtual elimination will be achieved through a variety of programs and actions that encourage cooperation
among all relevant sectors of society and which place primary emphasis on pollution prevention.

       This coordinated strategy provides the framework to achieve quantifiable goals in a specified
timeframe. As noted in the discussion of the PBT Initiative (see page III-4), there are 12 Level I
pollutants that represent an immediate priority and are targeted for reduction and eventual elimination
through pollution prevention and other incentive-based actions. Nine of these 12 pollutants are Great
Waters pollutants of concern.
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                                                                                       Chapter III
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        Both the U.S. and Canada have set
"challenge" goals to achieve reductions in
releases of the targeted pollutants. One of these
challenges is the commitment of both countries to
work together to assess atmospheric inputs of
persistent toxic substances to the Great Lakes
with the goal of evaluating and reporting jointly
on the contribution and significance of long-range
transport of these substances from worldwide
sources. In  addition, Environment Canada will
complete inventories often selected air pollution
sources to support assessment of environmental
impacts of air toxics by 1999 and will
demonstrate alternative processes to reduce
emissions from five predominant sources by
2001. The BNS includes several specific
reduction goals or challenges for the Level I
pollutants. For the U.S., these reductions will be
based on the most recent and appropriate
inventory for each pollutant (e.g., the mercury
inventory is based on 1990 levels). Canada plans
to use an inventory from 1988.

        At the initial June 1997 BNS stakeholder
meeting, participants developed a plan to
implement the strategy, which applied the
following steps to  address each priority substance
or category of substance:  (1) information
gathering, (2) assessment of current regulations
and programs, (3) identification of cost effective options for further reductions, and (4) recommendations
and implementation of actions.

        Since the initial stakeholder meeting, substance-specific work groups have been established and
are gathering information about baseline levels and sources of pollutants, as well as current programs
affecting the pollutants.  In addition, some work groups are attempting to identify cost-effective options
to achieve reductions. Specific highlights of the mercury work group activities include the AHA MOU
(see page 111-64), work with the chlor-alkali industry (see page 111-63), and an agreement with the steel
industry (see page 111-64). The PCB work group has supported Clean Sweep programs (e.g., the Illinois
Clean Sweep Program described on page 111-57) to reduce existing stockpiles.  With the International
Joint Commission, the BNS participants developed a draft report on sources, pathways, and
transformations of the BNS compounds.  This report, Identifying Source Regions of Selected Persistent
Toxic Substances in the U.S., identifies and ranks source regions for BNS pollutants, identifies regulatory
and voluntary programs to control emissions of these compounds,  and determines the emissions
inventory and control gaps that exist for the BNS compounds. In addition, EPA's Great Lakes National
Program Office released a Draft Pesticides Report in Response to  the Great Lakes Binational Toxics
Strategy in December 1998 (see sidebar).  Many additional activities that support the Binational Strategy
have been implemented by a wide variety of stakeholder groups and are outlined in the Draft Great Lakes
Binational Toxics Strategy: Activities by Partners (U.S. EPA and Environment Canada 1998).   Table
III-8 describes the  BNS challenge goals for the U.S. for each Level I substance and summarizes recent
activities with respect to those goals.
       BNS Pesticides in the Great Lakes

In December 1998, EPA's Great Lakes National
Program Office (GLNPO) released a draft report
entitled, Draft Pesticides Report in Response to the
Great Lakes Binational Toxics Strategy. A final
report will be released in fall 1999. The report
presents and analyzes data on the environmental
presence of five banned pesticides (i.e., chlordane,
aldrin/dieldrin, DDT, mirex, toxaphene) in the Great
Lakes, along with probable and suspected sources.
The report fulfills a "challenge" created by the
Binational Toxics Strategy for EPA to confirm by
1998 the elimination of uses and releases of the
pesticides from sources  that enter the Great Lakes.

The report concludes that although environmental
concentrations of the pesticides in the Great Lakes
basin have gradually declined for 20 years, they
remain at levels of concern in water, sediment, and
fish. The EPA found no  evidence of environmentally-
significant, purposeful releases of the pesticides in
the U.S. and concluded that continuing inputs to the
Great Lakes are likely to originate from remaining
stockpiles of the pesticides held by consumers, long-
range transport from countries where the pesticides
are not banned, and releases of the pesticides from
reservoir sources (e.g., contaminated sites). Based
on these findings, EPA concluded that there is  a
continuing need to pursue activities set forth under
the Binational Toxics Strategy.
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Chapter IH
Major Programs and Activities
                                              Table 111-8
               U.S. BNS Challenge Goals and Activities for Level I Substances
   Level I Substance
     U.S. Challenge Goal
               Progress/Activities
  Mercury and
  Compounds
 By 2006, a 50 percent
 reduction in deliberate use
 and a 50 percent reduction in
 release from human-activity
 sources. This release
 reduction applies to the
 aggregate releases to the air
 nationwide and to releases to
 the water in the Great Lakes
 basin.
BNS work group activities are focusing on voluntary
actions. Formal collaborative efforts are under way
with the chlor-alkali industry, the American Hospital
Association, and three Indiana steel mills.  Outreach
projects are ongoing with manufacturers and users of
mercury relays and switches, utilities, and laboratories.
  Dioxins and Furans
 By 2006, a 75 percent
 reduction in total releases
 from human-related activities.
 This release reduction applies
 to the aggregate releases to
 the air nationwide and to
 releases to the water in the
 Great Lakes basin.
The BNS dioxin work group is coordinating closely with
the PBT Initiative dioxin efforts, including a Great
Lakes State pilot to target air emissions using cross-
media authorities. Voluntary reduction efforts are also
planned.
  PCBs
 By 2006, a 90 percent
 reduction nationally of high-
 level PCBs (>500 ppm) used
 in electrical equipment.
 Ensure that all PCBs retired
 from use are properly
 managed and disposed of to
 prevent accidental releases.
The BNS PCB work group is developing a work plan.
Voluntary actions are being pursued through
expanding EPA Region V's PCB phasedown program,
encouraging national replication of the phasedown
program, implementing a clean sweep pilot in Chicago,
and encouraging a national PCB reduction effort.
  Chlordane, DDT,
  Aldrin/Dieldrin,
  Mirex, Toxaphene,
  Octachlorostyrene
 Confirm, by 1998, that there is
 no longer use or release from
 sources that enter the Great
 Lakes basin.  If ongoing long-
 range sources from outside
 the U.S. are confirmed, use
 existing international
 frameworks to reduce or
 phase out releases.
A final BNS status report on use and release from
Great Lakes basin sources is due fall 1999. The BNS
work group is also developing a work plan. The EPA
will continue clean sweeps to reduce stockpiles in the
Great Lakes basin and will work with stakeholders and
Great Lakes States to reduce pesticide reliance.  The
BNS octachlorostyrene work group is focusing on
defining sources, releases, and environmental loadings
(and, to some extent, toxicity and bioaccumulation).
  Alkyl Lead
 Confirm no use in automotive
 gasoline by 1998. Support
 and encourage stakeholder
 efforts to reduce alkyl lead
 releases from other sources.
The EPA issued a "confirmation of no use in
automotive gasoline" report under the BNS in
December 1998, broaden stakeholder involvement,
encourage stakeholder minimization of use/release
from other sources (e.g., aviation, racing,) and track
efforts to develop unleaded alternatives for aviation
and racing fuel.
  Hexachlorobenzene
 Seek, by 2006, reductions in
 releases that are within or
 may have potential to enter
 the Great Lakes basin from
 sources resulting from human
 activity (percentage goal not
 yet established).
An initial step under the BNS is to quantify loadings to
set a realistic percentage goal.  The BNS work group
will consider approaches to reduce releases during
pesticide manufacturing and use, chlorinated solvent
manufacturing, and possibly aluminum manufacturing.
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                                                                                   Chapter III
                                                                Major Programs and Activities

Level 1 Substance
Benzo[a]pyrene
U.S. Challenge Goal
Seek, by 2006, reductions in
releases that are within or
may have potential to enter
the Great Lakes basin from
sources resulting from human
activity (percentage goal not
yet established).
Progress/Activities
The BNS work group was developing a work plan in
1998.
INTERNATIONAL JOINT COMMISSION

        Originally created in 1909 for the purpose of resolving disputes between the U.S. and Canada,
the International Joint Commission (IJC) is charged with the responsibility of evaluating and assessing
the progress of commitments made by Canada and the U.S. under the 1978 Great Lakes Water Quality
Agreement (GLWQA).  In keeping with this responsibility, the IJC prepares a biennial report outlining
its findings and recommendations.  These recommendations are based on information compiled from the
Great Lakes Water Quality Board (WQB), Science Advisory Board (SAB), International Air Quality
Advisory Board (IAQAB), Council of Great Lakes Research Managers, various task forces, and through
a variety of public consultation activities. In 1985, the WQB established a list of 11 critical pollutants
which remain the focus of IJC's efforts today. Nine of the critical pollutants overlap with the Great
Waters pollutants of concern and the PBT Initiative: DDT/DDE, dieldrin, hexachlorobenzene, lead,
mercury, PCBs, dioxins and furans, and toxaphene.

        The IJC's Ninth Biennial Report on Great Lakes Water Quality, published in June 1998, focused
on the issue of persistent toxic substances in the Great Lakes ecosystem, which has been the major focus
of IJC's biennial reports since  1990. The IJC continues to stress the importance of eliminating these
substances.  As in previous biennial reports, IJC developed targeted recommendations to aid Canada and
the U.S. to achieve the objectives under the GLWQA. Historically, these recommendations have been
incorporated into existing or planned programs, and a few have achieved specific and direct results,
including The Great Lakes Binational Toxics Strategy. Recommendations to the U.S. and Canada from
the 1998 report include the following:

•       Accelerate the development of integrated, binational programs to reduce and eliminate sources of
        persistent toxic substances to the atmosphere;

•       Develop and communicate a comprehensive strategy for reducing mercury and NOX emissions
        associated with energy production and use;

•       Expand research into endocrine disrupting chemicals in humans and wildlife;

•       Support the development and application of ecosystem models;

•       Identify, assess, and support surveillance and monitoring programs essential to track contaminant
        loadings to, and concentration trends for, each of the Great Lakes; and,

•      Focus reduction and elimination efforts on dioxins, furans, mercury, and PCBs.

The IJC presented additional recommendations on agricultural practices, communication of scientific
information, radioactivity, ecological economics, and contaminated sediment in areas of concern
(AOCs).
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter in
Major Programs and Activities
UNITED NATIONS ECONOMIC COMMISSION FOR EUROPE LRTAP
PROTOCOLS ON HEAVY METALS AND POPS

       In 1979, members of the United Nations Economic Commission for Europe (UN-ECE) created
the Long-Range Transboundary Air Pollution (LRTAP) convention to provide a framework for
participating countries to limit, gradually reduce, and eventually prevent air pollution. Today, the 57
countries included in the UN-ECE region are the Russian Federation, the Newly Independent States,
Central and Eastern Europe, Western Europe, Canada, and the U.S.  Protocols to the LRTAP convention
negotiated since its creation establish more specific and legally-binding controls and emission reduction
targets for certain air pollutants.

       In June 1998, the members of the UN-ECE signed protocols on persistent organic pollutants
(POPs) and heavy metals.  The POPs are defined as organic substances that possess toxic characteristics,
are persistent, bioaccumulate, are prone to long-range transboundary transport and deposition, and are
likely to cause significant adverse human health and environmental effects. The POPs protocol bans the
production and use of eight compounds (i.e., aldrin, chlordane, dieldrin, endrin, hexabromobiphenyl,
kepone, mirex, and toxaphene) and limits the production and use of five compounds (i.e., DDT,
heptachlor, hexachlorobenzene, lindane, and PCBs).  In addition, the POPs protocol requires countries to
apply best available technology methods to limit air emissions from stationary sources of dioxins, furans,
PAHs, and hexachlorobenzene. The protocol on heavy metals regulates cadmium, lead, and mercury.
The protocol bans the use of lead in gasoline and the use of mercury in batteries and requires the
application of best available technology to limit air emissions from major stationary sources of all three
metals.

       Both of these protocols to the LRTAP convention incorporate less stringent obligations for
countries with economies in transition, and the protocols offer alternative compliance options to allow
some parties to apply different control strategies, provided these strategies achieve equivalent emission
reductions. The protocols also commit participating parties to reduce total national air emissions to
below the levels reported for a reference year (between 1985 and 1995).

       Most recently, in December 1999, the U.S. and Canada, along with European members, signed
the LRTAP Protocol to Abate Acidification, Eutrophication and Ground-level Ozone. This Protocol is
the most sophisticated environmental agreement so far because its creates the first comprehensive,
multinational structure to simultaneously reduce the long range transport of the various pollutants that, in
different combinations, cause acid rain, smog and other serious air pollution problems. The signing of
this agreement also initiates a new phase within LRTAP to increase emphasis on implementation,
compliance, review and extension of existing protocols.  In order to accommodate the domestic (acid
rain) and bilateral (ozone) processes which are currently under way in both countries, both Canada and
the United States will incorporate their emission reduction commitments for sulphur dioxide, nitrogen
oxides and volatile organic compounds into the Protocol at the time of its ratification. This
accommodates the tuning of the bilateral initiative to complete negotiations in the year 2000 of an ozone
annex to the U.S. - Canada Air Quality Agreement (see below).

       Further information on the LRTAP Convention and its Protocols can be found at
http://www.unece.org/env/lrtap.
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                                                                                Chapter III
                                                              Major Programs and Activities
 UNITED NATIONS ENVIRONMENT PROGRAM GLOBAL POPS
 INITIATIVE

       At its 19th session in February 1997, the United Nations Environment Program (UNEP)
 Governing Council concluded that international action, including a global, legally-binding instrument, is
 needed to reduce the risks to human health and the environment arising from the release of 12 POPs:
 aldrin, dieldrin, DDT, endrin, chlordane, hexachlorobenzene, mirex, toxaphene, heptachlor, PCBs,
 dioxins, and furans. The Governing Council decided that immediate international action should be
 initiated to reduce and/or eliminate the emissions and discharges of the 12 POPs, and, where appropriate,
 eliminate production and subsequently the remaining uses of those POPs that are internationally
 produced. Accordingly, the first session of the Intergovernmental Negotiating Committee (INC) for an
 International Legally Binding Instrument for Implementing International Action on Certain Persistent
 Organic Pollutants was held in Montreal in June 1998.  The INC is expected to complete an
 Internationally Legally Binding Instrument by the middle of the year 2000.

       Currently, the INC is establishing an expert group for the development of science-based criteria
 and a procedure for identifying additional POPs as candidates for future international action. In addition,
 UNEP has initiated a number of immediate actions, such as studies to identify alternatives to POPs,
 current PCB inventories, sources of dioxins and furans, and available POP destruction capacity.

 NAFTA COMMISSION ON ENVIRONMENTAL COOPERATION
 SOUND MANAGEMENT  OF CHEMICALS PROGRAM

       On January 1, 1994, the U.S., Canada, and Mexico officially established the North American
 Agreement on Environmental Cooperation (NAAEC) to foster greater cooperation on environmental
 issues, including the management and control of several Great Waters pollutants of concern.
 Subsequently, the NAAEC created the Commission on Environmental Cooperation (CEC) to address
 regional environmental concerns, prevent potential trade and environmental conflicts, and promote
 effective enforcement  of environmental law. One of the CEC's first activities was to develop a program
 to identify, measure, and mitigate the  environmental impacts of the North American Free Trade
 Agreement (NAFTA) (NAAEC 1999).
       In 1995, the CEC established a Sound
Management of Chemicals (SMOC) Work
group to address the issues of persistent toxic
substances and their effects in and transport
between the North American countries. The
original duties of the work group members
included the development of a North American
Regional Action Plan (NARAP) for the
management and control of PCBs (Commission
for Environmental Cooperation 1998).  Since
1995, NARAPs have been developed for PCBs,
DDT, chlordane, and mercury. The CEC is
currently developing a Phase II NARAP for
mercury, which represents an amendment to
the first mercury NARAP.  The CEC is developing NARAPs for dioxins and furans, and
hexachlorobenzene. Draft and final NARAPS and additional information related to this effort is
available at www.cec.org/programs_projects/pollutants_health/smoc/smoc-rap.cfm?varlan=english.
         Recent Developments on the
  Mercury North American Regional Action Plan

In October 1998, the North American Implementation
Task Force on Mercury held a Science Experts
Workshop that focused on mercury source
identification, fate, transport, and monitoring and the
identification of research needs in these areas. The
workshop resulted in a Strategy for the Development
of a Trinational North American Mercury Baseline for
mercury concentrations and fluxes (Draft Agenda,
October 6-8, 1998, Science Experts Workshop on
Mercury, Las Vegas, NV).
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Chapter in
Major Programs and Activities
U.S.-CANADA AIR QUALITY AGREEMENT

       The U.S.-Canada Air Quality Agreement, which was signed in March 1991, addresses
transboundary air pollution between the two countries.  The agreement focuses on acid rain and ozone
transport issues, prevention of deterioration of air quality and visibility, development of emissions
monitoring systems, notification and assessment of major projects which could affect transboundary air
quality, and coordinated research activities. The two countries established the Air Quality Committee
(AQC) to help implement the agreement. In the past, the AQC focused primarily on acid rain and
notification issues and is currently expanding the focus to address transboundary ground-level ozone and
fine particles (U.S. EPA 1998s).

       The agreement includes commitments by the U.S. and Canada to reduce SO2 and NOX emissions.
Specifically, for NOX, the U.S. and Canada agreed to reduction goals amounting to about 10 percent of
the national NOX emissions for both countries by 2000. This is equal to approximately two million tons
in the U.S. and ioO,000 tons in Canada. The U.S. expects to meet this goal through mobile and
stationary source NOX emission measures, a large part of which will be realized through Acid Rain
Program reductions of emissions  from coal-fired electric power plants.  After 2000, the U.S. expects to
achieve additional reductions in NOX from implementation of the ozone NAAQS and the NOX SIP call
(see page 111-27).  Canada has measures in place to reduce NOX emissions from stationary sources by
100,000 tons by 2000 through national emissions limits for new  fossil-fueled power plants, retrofits at
several existing power plants, new source standards for boilers, process heaters, and cement kilns, and
reconstruction of a metals smelter.  In addition, by 2010, Canada anticipates a 10 percent decline in NOX
emissions from 1990 levels as a result of improved emission standards for vehicles.

       In April 1997, the Canadian Minister of the Environment and the EPA Administrator reiterated
their commitment to addressing transboundary air pollution by signing a Joint Plan of Action for
Addressing Transboundary Air Pollution.  The commitment focuses on the common concern of both
countries for ground-level ozone  and fine particles and for protecting public health on both sides of the
U.S. - Canada border. Currently, the U.S. and Canada are negotiating an ozone annex to the U.S. -
Canada Air Quality Agreement which is expected to be completed by December 2000. This annex will
fulfill the two countries' obligations under the LRTAP Protocol  to Abate Acidification, Eutrophication
and Ground-level Ozone (see discussion above).
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                                    CHAPTER IV
                             SCIENCE  AND TOOLS
        In addition to the environmental progress discussed in Chapter II and the program progress
discussed in Chapter III, there has been significant advancement since the Second Great Waters Report to
Congress in the development and use of new scientific methods and tools needed to understand the
problem associated with Great Waters pollutants of concern.  This includes improved understanding and
assessment capabilities in some areas and a clearer picture of remaining uncertainties and future research
needs in other areas.

        This chapter highlights recent advancements in scientific research, as well as new and improved
monitoring and modeling capabilities and databases that are improving our understanding of and abilities
to address public health and environmental risks posed by the pollutants of concern in the Great Waters.
Unlike Chapter II, which focuses on the results of new research and monitoring for the purpose of
defining the overall problem, the discussion in this chapter focuses on developments and new findings
that improve our understanding of more narrow issues related to pollutant emissions, transport, loadings,
and effects.  It also discusses the status and directions of research and information sources that will be
useful in future assessments of the Great Waters. Finally, the chapter identifies additional research and
tools that are necessary to address remaining uncertainties related to atmospheric deposition in the Great
Waters. This discussion is not intended to be comprehensive, but rather to highlight some of the key
scientific advancements since the Second Report to Congress.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter IV
Science and Tools
WHAT MAJOR ADVANCEMENTS  HAVE OCCURRED SINCE THE
SECOND REPORT?

       This section summarizes a number of major advancements in scientific research, models, and
databases that are and will be useful in better understanding atmospheric deposition of the Great Waters
pollutants of concern. Recent developments in emissions inventories are presented first, followed by a
discussion of changes in programmatic direction and progress of several ambient air and deposition
monitoring networks and environmental monitoring networks. The last two main subsections provide a
discussion of recent scientific advancements in environmental fate and transport modeling, and exposure
and effects research and modeling.

EMISSION INVENTORIES

National Toxics Inventory

       Developing estimates of how much of a pollutant is being emitted is an important key to
characterizing the extent of the air toxics problem in the U.S., including persistent, bioaccumulative
toxics that are of concern to the Great Waters program. For about 20 years, EPA has routinely collected
emissions inventory data for criteria pollutants, such as lead, carbon monoxide, and particulate matter.
For air toxics, however, scientists have had to rely on indirect estimates of emissions that are based on
emission factors and other imprecise methods.  With the air toxics program in the CAA amendments of
1990 came a new focus on air toxics emissions inventories. This information can be used to estimate and
characterize risk and develop strategies to reduce risks from air toxics.  These pollutants are emitted by
major, area, and mobile sources, and emission estimates from these sources can vary from the national-
level to regional- and county-level estimates, and to facility- and process-specific emissions data that can
be used in air dispersion models.

       The dispersion and exposure modeling used to estimate and characterize risks from air toxics
requires a model-ready emissions inventory. As a result, EPA has  compiled and continues to  update and
refine the National Toxics Inventory (NTI). To date, EPA has compiled an inventory data set for the
1990 to 1993 period (called the 1993 NTI) and another for 1996. The 1993 NTI data, where available for
Great Waters pollutants of concern, are presented in Chapter II to characterize emissions and  sources on
a national level. The NTI does not include emissions of air toxics from natural sources  (e.g., plants,
volcanoes).

       The 1996 NTI was completed in early 2000, but was not available in time to be included in this
report. It represents a substantial improvement over the 1993 NTI in that it is more complete in its
coverage of pollutants and their sources, and it carries a higher degree of spatial resolution owing to  its
development from source-specific information (i.e., the "bottom-up" approach to inventory development)
and contains HAP emission estimates for major (facility-specific),  area, and mobile on-road and non-road
sources. In these 1996 NTI efforts, a majority of the State and local air pollution control agencies have
provided direct emission information or a critical review of EPA-developed emissions in a coordinated
effort to develop the best inventory in the available timeframe.  This approach provides estimates of
emissions at the county-level of resolution (or better, in many cases), which subsequently allows the
1996 NTI to be used to develop screening-level modeling assessments of ambient concentrations and
inhalation exposures down to the county-level. As such, the 1996 NTI represents the most recently
verified and complete emissions inventory available for national assessments.
Page IV-2
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                                                                                     Chapter IV
                                                                              Science and Tools
        The EPA has been compiling the 1996 NTI using five primary sources of data:

        State and local toxic air pollutant inventories (developed by State and local air pollution control
        agencies);

•       Existing databases related to EPA's air toxics regulatory program;

•       The EPA's Toxic Release Inventory (TRI) database;

•       Estimates developed using mobile source methodology (developed by EPA's Office of
        Transportation and Air Quality); and,

•       Emission estimates generated from emission factors and activity data. (NOTE: While major
        sources were not estimated using emission factors and activity data, 30 area sources were in the
        1996 NTI.)

        Preference is given to State- and locally-generated information, where available.  Where such
data are not available, existing data from EPA's regulatory development databases are utilized. If neither
of these data sources contains information for a known stationary source, EPA uses data from the TRI.
The EPA also gives preference in inventory development to emissions data resulting from direct
measurements over those generated from emissions factors and activity data.

        The TRI database contains national inventory data submitted by individual facilities that meet
certain reporting criteria. The TRI does not account for smaller sources within a source category that do
not meet the reporting criteria. Although the TRI data are limited in source category coverage, in many
cases, TRI data are used because they are the only available means to estimate emissions from certain
source categories. For the missing States and for sources not included in the State inventories, MACT
data, or the TRI, EPA estimated air toxic emissions using air toxic emission factors and corresponding
activity data.

        The compilation of such a large data set presents a significant challenge to EPA and introduces
several limitations.  In terms of consistency, the NTI is a composite of emissions estimates generated  by
State and local regulatory agencies, industry, and EPA.  Because the estimates originated from a variety
of sources and estimation methods, as well as for differing purposes, they vary in quality, included
pollutants, level of detail, and geographic coverage.  Also, the accuracy of emissions estimation
techniques varies with pollutants and source categories. In some cases,  an estimate may be based on few
(or  only one) emissions measurements at a similar source. The techniques used and quality of the
estimates will vary between source categories (e.g., some have been better studied than others) and
between major, area, and mobile source sectors. Another limitation of the NTI is that emissions from
reservoir sources, such as volatilization from soils  where chemicals were previously spilled or applied (in
the  case of pesticides), are either missing or poorly quantified.  If such sources are a major component of
the  total emissions for a given chemical, NTI could under report total emissions for that chemical.

       Future updates of the NTI are scheduled every 3 years. However, similar to other inventories,
the  NTI is dynamic and is subject to change (via periodic updates) as new, more reliable data become
available for the year it represents. Further, EPA continues to work with the State and local agencies to
promote consistency and accuracy in estimating and reporting emissions information for future years.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter IV
Science and Tools
The Great Lakes Regional Air Toxics Emissions Inventory

       Under the auspices of the Great Lakes Commission, the eight U.S. Great Lakes States and the
Canadian province of Ontario have been engaged since the early 1990s in creating and updating a
regional air toxics emissions inventory of the Great Lakes pollutants of concern — the Great Lakes
Regional Air Toxics Emissions Inventory. The inventory covers 86 pollutants from point, area, and
mobile sources. The emissions estimates are at the process level, and the data are model-ready. The
inventory is compiled according to a regional protocol designed to provide data of consistent quality and
format throughout the Great Lakes region. The inventory data are supplied to the NTI; data for the 1993
reporting year were released in the summer of 1998.

AMBIENT AIR AND DEPOSITION MONITORING NETWORKS

       Figure IV-1  displays the monitoring sites for all ambient air and deposition monitoring networks
that measure Great Waters pollutants of concern in the regions of the Great Waters and throughout the
U.S. and parts of Canada.

National  Atmospheric Deposition Program/National Trends
Network

       The National Atmospheric Deposition Program (NADP) began in 1978 as a cooperative program
between Federal and State agencies, universities, electrical utilities, and other industries to determine
geographical patterns and trends in wet deposition of sulfate, nitrate, hydrogen ion, ammonium, chloride,
calcium, magnesium, and potassium. The NADP was renamed as NADP/NTN (National Trends
Network) hi the mid-1980s when the program had grown to almost 200 monitoring sites (Figure IV-1).
The monitoring sites are located in rural areas, and data are collected on a weekly basis. The collected
data provide insight into natural background levels of pollutants. The network of NADP/NTN
monitoring sites allows for the development of concentration and wet deposition maps to describe the
trends and spatial patterns in the constituents of acid precipitation.  The Mercury Deposition Network
(MDN), which is another component of the NADP, measures mercury levels in wet deposition at over 40
NADP sites (U.S. EPA 19981). The data that are currently available from NADP/NTN and NADP/MDN
are presented in Chapter II to characterize the deposition of nitrogen and mercury, respectively.

Clean Air Status and Trends Network

       The Clean Air Status and Trends Network (CASTNet) was initiated in 1987 to estimate dry
acidic deposition, to provide data on rural ozone levels, and to determine the effectiveness of national
emission control programs.  The CASTNet is comprised of about 70 monitoring stations across the U.S.
(Figure IV-1). Data on atmospheric concentrations of sulfate, nitrate, ammonium, sulfur dioxide, and
nitric acid  are collected weekly, and ambient ozone concentrations are collected hourly. Most of the
stations are operated by EPA's Office of Air and Radiation; 19 stations are operated by the National Park
Service in  cooperation with EPA (U.S. EPA 19981).
Page IV-4
Deposition of Air Pollutants to the Great Waters - 3r Report to Congress 2000

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Chapter IV
Science and Tools
Atmospheric Integrated Research Monitoring Network

       Established in 1992, the Atmospheric Integrated Research Monitoring Network (AIRMoN),
which is sponsored by the NOAA Air Resources Laboratory, conducts research on both wet and dry
deposition based on measurements taken at a subset of NADP and CASTNet sites (Figure IV-1).  The
primary AIRMoN objectives are determining the effectiveness of emission controls mandated by the
CAA, evaluating potential impacts of new sources of emissions on protected areas, and identifying
source/receptor relationships in atmospheric models. One notable distinction of the AIRMoN-wet
network is that sampling is conducted on a daily basis, whereas NADP/NTN data are collected on a
weekly basis. Daily sampling allows for the application of source-receptor models to individual storm
systems and reduces the storage artifact for ammonium.  The AIRMoN-dry network has yielded direct
measurements of dry deposition that have been used to support inferred dry deposition measurements at
other NOAA and CASTNet stations. In the future, AIRMoN data will also be used to characterize spatial
variability around current deposition stations, which will improve NOAA's ability to construct regional
deposition loadings estimates.

Integrated Atmospheric Deposition Network

       The Integrated Atmospheric Deposition Network (IADN) is a joint U.S.-Canada program begun
in 1990 under a formal 6-year implementation plan. The lADN's mandate, which is derived from Annex
15 of the Canada-U.S. Great Lakes Water Quality Agreement of 1987, is to determine atmospheric
loadings of toxic substances, including Great Waters pollutants of concern, to the Great Lakes and their
temporal and spatial trends. The IADN collects data that can be useful in assessing the relative
importance of atmospheric deposition. Under IADN, trends in pollutant concentrations in air and
precipitation are assessed and loading estimates of atmospheric deposition and volatilization of pollutants
are made every 2 years. The IADN network currently consists of one master station per Great Lake and
14 satellite stations (Figure IV-1). Stations are located in remote areas and do not assess urban sources
of pollution. The  satellite stations do not meet the original siting criteria but are subject to quality
assurance and quality control requirements (U.S./Canada IADN Scientific Steering Committee 1998).

       Detailed results from IADN are presented in Chapter II by pollutant group. General conclusions
include the following:

•      Levels in  air and precipitation appear stable for current-use pesticides such as endosulphan, but
       levels for  most other pesticides, PCBs, and lead are decreasing;

•      Gas absorption appears to be the dominant deposition process for delivering semi-volatile
       organic compounds (SVOCs), including PCBs and PAHs, to lake surfaces, while wet and dry
       deposition dominate for the trace elements and higher molecular weight PAHs;

•      For some  IADN substances, like dieldrin and PCBs, the surface waters are behaving like a source
       since the amount that is volatilizing from the water is greater than the amount being deposited to
       the water;

•      The lakes are sensitive to the atmospheric concentration of IADN chemicals, and this points out
       the fragility of these resources given that long-range transport from other regions may be a
       significant source of toxic pollutants; and,
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                                                                                   Chapter IV
                                                                            Science and Tools
        Air trajectory analyses indicate that many SVOCs are potentially originating from outside the
        Great Lakes basin, whereas trace metals and PAHs may be associated with local sources
        (U.S./Canada IADN Scientific Steering Committee 1998).

        In 1998, the Second Implementation Plan for 1998 to 2004 was developed based on a review of
 the program from 1990 to 1996.  No major changes are anticipated under the Second Implementation
 Plan. The IADN will continue surveillance and monitoring activities, related research, and provision of
 information for intergovernmental commitments and agreements. Additional work to be completed under
 the Second Implementation Plan is the development of a database for all U.S. and Canadian data.
 Potential modifications will be discussed in relation to the placement of satellite stations to assess urban
 inputs and air-water gas exchange, criteria for changes to the IADN chemical list, coordination with other
 research activities, quality assurance and control of IADN operations, and communication of IADN
 results (U.S./Canada IADN Scientific Steering Committee 1998, U.S. EPA 1998m).

 Chesapeake Bay Atmospheric Deposition Study

        The Chesapeake Bay Atmospheric Deposition Study (CBADS) network was established by a
 team of scientists from the University of Maryland, Virginia Institute of Marine Sciences, University of
 Delaware, and Old Dominion University. In June 1990, CBADS began collecting data from three rural
 (i.e., at least 50 km from urban areas) shoreline monitoring sites at Wye Institute and Elms Institute,
 Maryland, and Haven Beach, VA. Measured parameters included wet and dry deposition and gas
 exchange  of elements (including lead and cadmium), individual PAHs, and total PCBs.  Results of data
 collected from June/July 1990 to the end of 1991 were reported in the 1994 Chesapeake Bay Basin
 Toxics Loading and Release Inventory (1994 TLRI) (Chesapeake Bay Program 1994) and in the Second
 Report to  Congress (U.S. EPA 1997b).  The 1994 TLRI results did not include any  data on mercury or
 current-use agrichemicals, nor did it provide information on wet deposition to urban areas in the
 Chesapeake Bay watershed. An additional 21 months of CBADS wet deposition data were  collected and
 reported in the 1999 TLRI (making the total study period from June/July 1990-September 1993). This
 new information on Great Waters pollutants of concern is presented in Chapter II by pollutant group.

        Other atmospheric deposition studies were also reported in the 1999 TLRI,  including data
 collected for wet deposition and loadings of mercury and agrichemicals; however, only initial data were
 available at the time of the report generation to estimate wet deposition loadings to urban areas.  For the
 1999 TLRI, urban wet deposition fluxes of metals, PAHs, PCBs, and mercury were assumed to be
 enriched two-, four-, ten-, and two-fold over regional background levels, respectively. Analysis of
 monitoring data collected by CBADS and other studies not included in the 1999 TLRI will be available
 for the next report.

Air Toxics Monitoring

        The EPA is currently developing a concept for an air toxics monitoring network and beginning
 implementation. Ambient air toxics data would be useful to characterize ambient concentrations and
 deposition in representative areas, to provide data to support and evaluate dispersion and deposition
 models, and to establish trends and evaluate the effectiveness of strategies to reduce air toxics emissions.
 The goal is to build on monitoring already in place in State, local, and tribal programs as well as other
 national networks. For example, in the near future, fine particulate matter speciation monitors will
provide ambient air measurements of several air toxic metals (including lead and cadmium compounds)
 at over 50 urban locations in the country. Rural and remote monitoring of these metals takes place as
part of EPA's efforts to assess regional haze. As the air toxics network is phased in, the pollutants to be
monitored are expected to include several of the compounds of concern to the Great Waters, such as
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Science and Tools
mercury, POM, and metals. Information about the monitoring strategy can be found at
\v\v\v.epa.gov/tm/amtic/airtxfil.html.

       The EPA has also begun a research effort for ambient air monitoring of dioxin and dioxin-like
compounds called the National Dioxin Air Monitoring Network (NDAMN).  It is designed with several
objectives:

•      To provide data useful for calibrating regional-scale, long-range transport models used in
       estimating air concentrations of dioxin as a function of dioxin source emissions;

•      To provide air monitoring capability for the occurrences and levels of dioxin-like compounds in
       areas where animal feeds (used to feed domestic livestock) are primarily grown;

•      To provide for the long-term monitoring of dioxin-like compounds in different regions of the
       U.S. and over different seasons; and,

•      To provide data on potential transboundary import of dioxins and furans into the U.S.

       The network is being developed in phases. Phase 1 consists of up to 20 air monitoring stations;
Phase 2 is expected to consist of about 30-40 stations. Additional  information about the network can be
found at www.epa.gov/nceawwwl/lpage.htm.

OTHER ENVIRONMENTAL MONITORING NETWORKS AND
DATABASES

The EPA's Environmental Monitoring and Assessment Program
(EMAP)

       In 1988, the EPA Science Advisory Board (SAB) recognized a deficiency in the documentation
of the status of the Nation's natural environment and recommended that EPA develop a program to
monitor ecological status and trends in the U.S. The EPA responded with the initiation of the
Environmental Monitoring and Assessment
Program (EMAP) in 1989.  The EMAP program
also collaborates with other agencies, including
NOAA.
       The primary goal of EMAP is to
"monitor the condition of the Nation's
ecological resources, to evaluate the cumulative
success of current policies and programs, and to
identify emerging problems before they become
widespread or irreversible" (U.S. EPA 1997i, j,
k). Knowledge from the EMAP process will
give decision makers the ability to make
informed environmental management decisions,
set rational priorities, and make known to the
public the costs, benefits, and risks of
                               Condition of the Mid-Atlantic Estuaries
                           The EPA's Office of Research and Development and
                           the Environmental Monitoring and Assessment
                           Program (EMAP) issued a report, The Condition of
                           the Mid-Atlantic Estuaries Report, that is the first in a
                           series of State-of-the-Region Reports for the Mid-
                           Atlantic. The report discusses the adequacy of
                           current protective measures, the present condition of
                           natural resources, and the extent and possible
                           causes of ecological problems. These issues are
                           addressed through the evaluation of the best
                           available scientific information, including data from
                           large sampling programs throughout the estuaries,
                           and use of the latest scientific tools. Although the
                           Mid-Atlantic estuaries are being impacted by human
                           activities, active management by the States and EPA
                           has had positive results. Future State-of-the-Region
                           Reports for the Mid-Atlantic will address streams,
                           forests, and other resources (U.S. EPA 1998b).
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proceeding or refraining from implementing specific regulatory actions. Four operational objectives
guide EMAP:

1.     Estimate the current status, trends, and changes in selected indicators of the Nation's ecological
       resources on a regional basis with known confidence;

2.     Estimate the geographic coverage and extent of the Nation's ecological resources with known
       confidence;

3.     Seek associations between selected indicators of natural and anthropogenic stresses and
       indicators of ecological resources; and,

4.     Provide annual statistical summaries and periodic assessments of the Nation's ecological
       resources.

       These four objectives create an innovative approach for EMAP, which adopts a comprehensive,
multimedia perspective of the Nation's natural resources rather than the traditional single-pollutant or
single-location approach to environmental assessment.

        The EMAP's strategy also includes the development of a Regional Environmental Monitoring
and Assessment Program (R-EMAP) to test the effectiveness of the EMAP approach on answering
questions about regional and local ecological conditions. The R-EMAP has three main objectives:

•      To evaluate and improve EMAP concepts for State and local use;

•      To assess the applicability of EMAP indicators at differing spatial scales; and,

•      To demonstrate the utility of EMAP for resolving issues of importance to EPA Regions and
       States.

Since 1990, EPA has funded at least two R-EMAP projects in each of the ten EPA Regions. One of these
studies addressed mercury deposition levels and geographic trends in the Great Lakes region, as
mentioned in Chapter II.

National Sediment Inventory

       The EPA established the National Sediment Inventory (NSI) to prepare the first biennial National
Sediment Quality Survey (NSQS) Report to Congress (U.S. EPA 19971, j, k) (see also page III-8).
National-level results from the NSQS on sediment contamination are presented in Chapter II. The NSI is
intended to have applications far beyond supporting subsequent NSQS biennial reports. The NSI is the
largest set of sediment chemistry and related biological data ever compiled by EPA. In addition to
sediment chemistry data, the NSI includes tissue residue and sediment toxicity data.
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       The NSI includes data from ten existing
Federal databases (see sidebar). Minimal data
requirements for the NSI include monitoring
program, sampling date, latitude and longitude
coordinates, and measured units.  Additional data
fields such as sampling method and other quality
assurance/quality control information are
included when available. At present, the NSI
contains approximately 2 million records for
more than 21,000 monitoring stations across the
country. More than 230 chemicals and chemical
groups are included. Only data from 1980 to
1993 were used for the first NSQS. However,
older data are available in the NSI.
                                        NSI Federal Databases

                            O EPA's Storage and Retrieval System (STORE!)
                            @ NOAA's Coastal Sediment Inventory (COSED)
                            © EPA's Ocean Data Evaluation System (ODES)
                            O EPA Region IV Sediment Quality Inventory
                            © The Gulf of Mexico Program's Contaminated
                              Sediment Inventory
                            0 EPA Region X/USACE Seattle District's
                              Sediment Inventory
                            O EPA Region IX Dredged Material Tracking
                              System (DMATS)
                            © EPA's Great Lakes Sediment Inventory
                            © EPA's Environmental Monitoring and
                              Assessment Program (EMAP)
                            ® USGS's Massachusetts Bay Data
       Although the NSI provides broad
geographic coverage, the 21,000 monitoring stations currently represented in the data are not randomly
distributed. Most of the monitoring programs used to compile the NSI are located in areas with known or
suspected contaminant impacts.

National Contaminated Sediment Point Source  and Non-point
Source Inventories

       The EPA's mandate to investigate sediment contamination in the Nation's water included a
directive to identify potential pollutant sources.  With future biennial NSQS Reports to Congress, EPA
will inventory point and non-point sources and estimate loadings. The first NSQS Report to Congress
evaluated point sources (i.e., direct discharges to waterbodies) only (see also page III-8). The National
Contaminated Sediment Point Source Inventory (U.S. EPA 1997k) provided a relative ranking of
industrial categories and discharged chemicals for their potential contribution to sediment contamination.
The EPA developed the "load score," a unitless index of the magnitude of potential sediment
contamination based on chemical/facility-specific releases, physical and chemical properties, and
potential environmental risks. A screening analysis of the load scores indicated that the point sources
most likely to contribute to sediment contamination were sewerage systems, metals products and
finishing, primary metals industries, industrial organic chemicals, public utilities, petroleum refining, and
other chemical products. Metals were associated with higher load scores than other contaminant groups
because point source releases are more prevalent.  Additional analyses are needed to assess the
bioavailability  and toxicity of metals in sediments.

       Although the NSQS did not inventory specific non-point sources, it examined the land uses in
watersheds containing areas of probable concern (APCs)  to identify potential relationships between
sediment contaminants and human activities.  In general,  EPA found that diversified land uses were
associated with diversified pollutants.  However, a high percentage of agricultural land use corresponded
with markedly  higher contamination from pesticides.  Most chemical classes increased with higher
percentages of urban land use.  The analysis suggested that mercury and PAHs in urban sediments may
be attributable  to atmospheric deposition from local sources.

       Although the National Contaminated Sediment Point Source Inventory identified metals as the
leading contaminants based on load scores, the NSQS identified PCBs, mercury, pesticides, and PAHs as
most often responsible for contamination levels of concern in sediment (see also page 11-73). This
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 suggests that non-point sources and historical releases (including atmospheric deposition) contribute
 largely to contamination in the Nation's waters.

 NOAA's National  Status and Trends Bioeffects Assessments

        The National Status and Trends (NS&T) Program under NOAA (see page 11-70) conducts
 bioeffects assessment studies, which include sediment toxicity surveys and the development of effect-
 based numerical guidelines for use in evaluating the toxicological relevance of sediment contamination,
 among other factors.  The sediment toxicity surveys are conducted in coastal areas where data from
 NS&T's Mussel Watch and Benthic  Surveillance Projects indicate the potential for substantial
 environmental degradation and biological effects. Bioeffects assessments have been or are being
 conducted in 16 coastal areas.  Reports and data sets are available on the Internet for several of these
 locations at http://seaserver.nos/noaa.gov/projects/bioeffects/pagel.html.

 ENVIRONMENTAL TRANSPORT AND FATE

Available Environmental Transport and Fate Models

        Models-3 Community Multi-Scale Air Quality (CMAQ) Modeling System

        The Models-3 community multi-scale air quality (CMAQ) modeling system is a flexible software
 system designed to simplify the development and use of environmental assessment and decision support
tools for applications ranging from regulatory and policy analysis to understanding the interactions of
 atmospheric chemistry and physics. This newest generation of environmental modeling software has
been under development for the past 7 years. Models-3, in combination with CMAQ, form a third
generation air quality modeling and assessment system. First generation air quality models dealt with
tropospheric air quality with simple chemistry at local scales using Gaussian plume formulation (i.e., the
model assumes that the plume spreads from an emission source laterally and vertically in accordance
with a Gaussian distribution) as the basis for prediction. Second generation models covered  a broader
range of scales (i.e., local, urban, regional) and pollutants, addressing each scale with a separate model
and often focusing on a single pollutant. Third generation models treat multiple pollutants
simultaneously up to continental scales and incorporate feedback between chemical and meteorological
components. Models-3 has a unique  framework and science design that enables scientists  and regulators
to build their own modeling systems to suit their needs. The CMAQ system has capabilities  for urban to
regional-scale air quality simulation of tropospheric ozone, acid deposition, visibility, toxics, and fine
particles. The Models-3 framework contains components that assist the model developer with creating,
testing, and performing comparative analysis of new versions of air quality models and enables the user
to execute air quality simulation models and visualize the results. The overall goal of Models-3 is  to
simplify and integrate the development and use of complex environmental models, beginning with air
quality and deposition models (U.S. EPA 1998e). It is expected that the Models-3 framework and
CMAQ will be useful tools for research related to the Great Waters program.

       The initial public release of the Models-3 framework occurred in June 1998. This framework
provides a unifying foundation for continued evolution of environmental modeling and assessment tools
with the ability to extend the capabilities beyond the current air quality implementations. One area of
investigation has been a basic integration of the Chesapeake Bay Water Quality Model (CBWQM) into
the Models-3 framework to explore multimedia model linkages. Future development toward a fourth
generation system will extend linkages and process feedback to include air, water, land, and biota to
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provide a more holistic approach to simulation of transport and fate of chemicals and nutrients
throughout an ecosystem (U.S. EPA 1998e).

       Total Risk Integrated Methodology (TRIM)

       The Total Risk Integrated Methodology (TRIM) is a comprehensive framework for
characterizing human health and ecological risk. It is being designed by EPA's Office of Air Quality
Planning and Standards (OAQPS) for use in CAA programs (e.g., the Residual Risk Program) as a way to
consistently estimate the impacts of air pollutants. The TRIM will have the following characteristics: (1)
ability to perform multimedia assessments; (2) ability to perform human health and ecosystem risk
assessments; (3) ability to perform multipollutant assessments; (4) capability to address
uncertainty/variability; and, (5) ability to provide a readily available, user-friendly tool that will assist in
risk management decisions (U.S. EPA 1999e).

       The EPA is attempting to create a system that is scientifically defensible, flexible, and user
friendly.  The format of input data sets to TRIM are consistent with Models-3. When complete, TRIM
will contain three separate modules, including (1) fate and transport, (2) exposure, and (3) risk
characterization.  The most complex module is the multimedia fate and transport module, which is
entitled TRIM.FaTE.  This is the module on which EPA has been concentrating most of its effort (U.S.
EPA 1999e).

       The TRIM.FaTE module is a multimedia, chemically mass-balanced model. In the model, the
ecosystem scale of interest (landscape) is divided into compartments. The model tracks the mass of the
pollutant transported between compartments (rather than a set of one-way fate algorithms). The model is
being designed so that a wide variety of pollutants can be addressed. The TRIM.FaTE module will have
the capability to (1) simulate steps in a time series and (2) resolve mass distribution spatially. A
prototype  version of TRIM.FaTE has been developed by EPA; however, significant work remains on this
module, including comparisons of output to monitoring data for case studies and other model evaluation
exercises. A version of TRIM, including TRIM.FaTE, is expected to be released in 2000 (U.S. EPA
1999e).

       Models for Atmospheric Mercury

       Because of the need to identify the emission reductions required to meet water quality and other
criteria, systems are being developed that use emissions data with atmospheric chemistry and transport
models and meteorological models.  A report, .,4 Computer-Based Framework to Model Acceptable
Loadings  of Mercury to the Atmosphere to Protect Water Quality, was prepared for EPA Region IV by
Nicola Pirrone and Gerald J. Keeler, at the University of Michigan (Pirrone and Keeler 1997). This
report discusses the coordination of available computer models for atmospheric mercury - its transport,
chemical-physical dynamics, and deposition (wet and dry) to water surfaces and terrestrial receptors.
The analysis of model capabilities and critical data inputs is applicable nationwide. In addition, some
specific discussions are provided for the South Florida Everglades hi comparison to forested watershed
and lake systems.

       This report presents a framework linking models that relate  data on mercury emissions into the
air to subsequent mathematical modeling of atmospheric transport, chemistry, and deposition processes
(Pirrone and Keeler 1997). The modeling framework is designed so that regulatory agencies can define
target load reductions from local and regional sources that are needed to meet water quality goals. In
order to correctly relate water quality criteria and bioaccumulation of mercury in the food chain to the
atmospheric and other inputs, this modeling framework needs to be  coupled to an aquatic modeling
system utilizing mercury transport and fate processes in similar timeframes. The set of models in the
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framework will need inputs including watershed-specific information or default assumptions and
chemical species released from the major pollutant sources, along with meteorological data and
mesoscale models (such as RAMS from Colorado State University or MM5 from Pennsylvania State
University).  This conceptual framework of models is being used as part of the design and analyses in a
State/EPA pilot project to develop a TMDL for mercury in a specified section of the Florida Everglades,
as discussed in Chapter III.

       The  Electric Power Research Institute (EPRI) has developed and continues to develop
environmental mercury cycling models (MCMs) to assess the transport and fate of atmospheric mercury
(Watras and Huckabee 1994, Leonard et al. 1995, Logan 1998, Pai et al. 1999). The MCMs have been
used to predict the fate of mercury in the Great Lakes (Leonard et al. 1995).  The Maryland Department
of Natural Resources reviewed two EPRI models, the Lake MCM (L-MCM) and the Regional MCM (R-
MCM), and concluded that they had the potential for use in Maryland to investigate cycling of
environmental mercury and bioaccumulation in fish (Logan 1998). The L-MCM was  developed for
predicting the biogeochemical behavior of mercury in the Mercury in Temperate Lakes Study of seepage
lakes in Wisconsin. The L-MCM is a dynamic, mechanistic simulation model that tracks processes and
changes in concentrations through time. The R-MCM is a steady-state, mechanistic simulation model.

Recent Environmental Transport And Fate Modeling Results

       Atmospheric Exchange Over Lakes and Oceans Surfaces (AEOLOS)

       The Atmospheric Exchange Over Lakes and Oceans Surfaces (AEOLOS) project, administered
through the EPA Great Lakes National Program Office and the Office of Research and Development, was
designed to study atmospheric deposition in the Great Waters. Begun in 1993 by EPA and scientists
from the Universities of Minnesota, Michigan, Maryland, Delaware, and the Illinois Institute of
Technology, the project's objectives were to determine (1) the dry depositional fluxes of critical urban
contaminants to the northern Chesapeake Bay near Baltimore and southern Lake Michigan near the
Chicago urban area, (2) the contributions of urban source categories to measured atmospheric
concentrations and deposition, and (3) the air-water exchange of contaminants and their partitioning into
aquatic phases (U.S. EPA 1997b).  The AEOLOS project proceeded under the hypothesis that emissions
of HAPs into the coastal urban atmosphere enhance atmospheric depositional fluxes to the adjacent Great
Waters such as Lake Michigan in the vicinity of Chicago and Gary, Indiana, and the Chesapeake Bay
near Baltimore (Simcik et al. 1997). Results of some AEOLOS studies are reported in Chapter II for
PAHs and PCBs as  well as below.

       A study under the AEOLOS project found that urban air emissions have an effect on the average
coastal atmospheric concentrations of PAHs and PCBs above continental background, increasing them by
factors of 12 and 4,  respectively.  As part of AEOLOS, air concentrations of PCBs and PAHs were
measured in the urban/industrial complex of Chicago, over the southern portion of Lake Michigan, and in
a non-urban location, in May and July 1994 and January 1995. Gas-phase PAH and PCB concentrations
over the lake were much lower than urban air concentrations.  The highest concentrations were
associated with winds that first crossed-over the urban/industrial area from Evanston, Illinois to Gary,
Indiana. Concentrations were near regional background for winds from any other direction. Seasonal
variation of PCB occurred, with volatilization being higher during the summer (Simcik et al. 1997).

       In another AEOLOS study in the Chicago area, PCB concentrations in  wet precipitation collected
over southern Lake  Michigan ranged from two to as high as 400 times greater than the measured regional
background concentration, indicating that the "urban plume" of Chicago increases atmospheric
deposition of contaminants to Lake Michigan over tens of kilometers. Concentrations of PCBs in urban
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precipitation were dominated by particle-bound congeners, indicating PCB enrichment in rainwater due
to efficient scavenging of contaminated particulate matter in the urban atmosphere (Offenberg and Baker
1997).

       Simcik et al. (1998), under the AEOLOS project, investigated gas-particle partitioning of PCBs
and PAHs in the Chicago urban area and over Lake Michigan and found that PCBs and PAHs in the
Chicago/Lake Michigan atmosphere were at equilibrium between the gas and particle phases.
Understanding gas-particle partitioning is important because it can be used to help determine the mode of
atmospheric deposition (i.e., wet deposition, dry deposition, air-water exchange).

       Chesapeake Bay NOX Modeling with RADM

       The Regional Acid Deposition Model (RADM) has been used to develop estimates of the
primary airshed of NOX emissions that are contributing nitrogen deposition to the Chesapeake Bay
watershed. The RADM was originally developed to address policy and technical issues associated with
acidic deposition. The model is designed to provide a scientific basis for predicting changes in
deposition resulting from changes in precursor emissions, to predict the influence of sources in one
region on acidic deposition in other sensitive receptor regions, and to predict the levels of acidic
deposition in certain sensitive receptor regions (Dennis 1997).

       In the RADM, the concentrations of gaseous and particulate species are calculated for specific
fixed positions in space as a function of time. The geographic extent, or domain, of the model is 2,800
by 3,040  km and extends south from James Bay in Canada to the southern tip of Florida and westward to
central Texas.  This domain is partitioned into 80 km-by-80 km grid cells.  The space is three-
dimensional, having 15 logarithmically-spaced vertical layers, covering the distance from ground level to
16 km in altitude. The RADM has a chemistry component that consists of 140 reactions among 60
species.  Chemical decomposition by solar radiation and aqueous-phase reactions that occur in clouds are
both included in the model's chemistry. For each grid cell, predictions are generated at dynamically
determined time steps of seconds to minutes that are output hourly by the model.  The species predicted
by RADM include ambient concentrations (SO2, NO, NO2, HNO3, O3, H2O2, NH3, PAN, HCHO, CO, and
SO^), wet deposition (SO^ NOj as HNO3, NH4+ as NH3, and H+), and dry deposition (SO2, SO^, HNO3,
O3, and NOa).  The meteorological fields that are used to determine the turbulent motion of the
atmosphere, which in turn affects the transport of species by wind into and out of the grid in three
dimensions, are from the Pennsylvania State University, National Center for Atmospheric Research
Mesoscale Model (MM4). The MM4 is a weather model used to recreate historical meteorology.

       Recent analysis with RADM shows that the range of influence of nitrogen emissions is similar to
the range for sulfur emissions — on the order of 600 - 800 km.  However, results suggest that the nitrogen
range given is too short (Dennis 1997). This implies the range  for nitrogen should be longer than that for
sulfur. In other words, the RADM results and analysis used to  define the airshed for the Chesapeake Bay
watershed is producing an estimate of the boundary of the airshed that is conservative, that is, one  that is
too small.

       In the original 1995  study (Dennis 1997), the extent of the Chesapeake Bay airshed was
approximately 900,000 km2, or more than 51A times larger than the watershed. The NOX emissions in the
airshed account for approximately 75 percent of the anthropogenic nitrogen deposition to the Chesapeake
Bay watershed. More recently, using the same methodology, Dennis conducted a more refined analysis
of the subregions within the RADM domain, resulting in a revised estimate of the Chesapeake Bay
airshed.  This revised airshed, presented in Figure IV-2, is approximately 1,081,600 km2, making it about
6l/2 times larger than the watershed (see http://www.chesapeakebay.net/data/niodel/mod_gis/
air_dom.gif). This larger airshed estimate results in only a slight increase (76 percent) of the amount of

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NOX emissions from the airshed which are deposited to the watershed. The contribution from utility and
mobile sources are roughly equal and make up the majority of the emissions which are eventually
deposited. However, when model simulations are used to compare these emission sources to nitrate
deposition a significant pattern emerges. Utilities, which are heavily concentrated to the west of the Bay,
tend to contribute a majority of the nitrate that deposits on the western side of the watershed. Moving
across the watershed from west to east, nitrate deposition from utility emissions shows a decreasing
trend. In contrast, a large amount of the mobile source emissions take place in cities and heavily
developed areas relatively close to the Bay. Thus, mobile emissions tend to contribute a majority of the
nitrate that deposits along the Delmarva Peninsula, the Chesapeake Bay itself, and the lower portions of
the western shore tidal tributaries. Nitrate deposition from mobile emissions shows a decreasing trend
moving from east to west across the watershed (Dennis 1997).

                                         Figure IV-2
                     Revised Principal Airshed for the Chesapeake Bay
      (Developed by R. Dennis, Atmospheric Sciences Modeling Division: ARL, NOAA, and NERL U.S. EPA)

       Lake Michigan Mass Balance Study

       The Lake Michigan Mass Balance Study (LMMBS) was developed and is being implemented by
the Great Lakes National Program Office in cooperation with five U.S. Federal agencies (i.e.,
Department of Energy, NOAA, U.S. Geological Survey, U.S. Fish and Wildlife Service, U.S. Army
Corps of Engineers), one foreign agency (i.e., Environment Canada), two State agencies, and eight
academic institutions. The LMMBS was initiated to address the objectives of the Lake Michigan
Monitoring Program, as well as to assist EPA in implementing section 112(m) of the CAA by
characterizing the loadings, transport, and fate of selected pollutants through monitoring and modeling.
The Second Great Waters Report to Congress describes the project in more detail and describes the
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atmospheric monitoring efforts, a system often stations situated around Lake Michigan. Additional
information can be found at www.epa.gov/ghipo/lmmb. The ultimate goal is to develop a predictive
model that forecasts impacts on lakes based on inputs of toxics to the system from a variety of sources
(sediments, atmospheric deposition, tributaries). Preliminary modeling results for mercury are presented
in Chapter II. Additional results are expected in 2000 that will support, in addition to section 112(m),
such efforts as the Binational Toxics Strategy and LaMPs.

       The LMMBS model is constructed for a limited group of pollutants: PCBs, chlordane, total
mercury, and atrazine. For mercury and atrazine, an emissions inventory either existed or could be
developed, so comprehensive modeling is being conducted for these two pollutants. For PCBs and
chlordane, a comprehensive modeling approach was not attempted because a comprehensive emissions
inventory did not exist. In addition, monitoring data were collected for an extended suite of chemicals,
including additional pesticides, PAHs, and heavy metals.  Currently, a multimedia database is being
developed to house all the data and quality assurance information for use by the modelers.  In the future,
the data will be available upon request.

       Atmospheric loadings of the LMMBS pollutants are being calculated for input into the models.
A major finding of the LMMBS to date is that traditional  atmospheric loading estimation techniques are
not adequate to describe the variability and source influence on deposition to the lake. New techniques
have been developed to better characterize the impact of atmospheric deposition on large lake systems.
Efforts have also been made to coordinate with ongoing fate and transport modeling activities and to
support the most advanced developments. The LMMBS is contributing a major amount of resources to
the CMAQ model system (page IV-11) for use in estimating emissions and transport of atrazine and
mercury to Lake Michigan. In addition, this project has assisted in the development of an atrazine soil
emissions model that could also be used to develop emissions inventories in other regions.

       Recent REMSAD Applications

       The Regulatory Modeling System for Aerosols and Deposition (REMSAD) was originally
developed in part to address the issue of atmospheric deposition of HAPs to the Great Waters. The
REMSAD is a grid model designed for use on workstation-class computers. As currently configured,
REMSAD (version 4.0) tracks the transport, transformation, and deposition (both wet and dry) of
nitrogen, mercury, cadmium, dioxin, polycyclic organic matter (POM), atrazine, speciated primary and
secondary fine particles, photochemical oxidants, acids, and ammonia. All of these substances are
treated simultaneously for a single integrated emission inventory, so that the effects of proposed policy
options on multiple pollutants with common sources may be analyzed at the same time. The model
extends vertically all the way to the tropopause, so that long-range transport of pollutants in the upper
troposphere can be captured.

       The model is  capable of nesting finer (i.e., higher resolution) grids within an overall coarse grid,
which makes it possible to focus on deposition to a particular watershed within the context of a broad
regional distribution of emission sources.  The EPA recently sponsored the 1990 Base Case Evaluation
Study (Guthrie et al. 1999a, b) in which the National Emission Trends 1990 inventory was used, along
with a calendar 1990 meteorological data set produced by the Interagency Working Group on Air Quality
Models (IWAQM). This model run was conducted for a full year (less 5 days) for the contiguous U.S.
with adjacent portions of Canada and Mexico.  The run was carried out on a coarse grid of approximately
60 km resolution, but included seven nested sub-grids at approximately 20 km resolution. These nested
sub-grids focused on the eastern seaboard (especially around the Chesapeake Bay), the  Lake
Michigan-Lake Superior region, the northern Gulf of Mexico, Puget Sound, southern Florida, and the
Houston-Galveston region of Texas.
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       The annual deposition pattern of total wet and dry nitrogen deposition (as nitrate) as simulated in
the 1990 Base Case is very similar to that reported by Dennis (1997) for the eastern U.S., given
differences in emissions. The REMSAD results indicate a significant seasonal variation, however,
especially in the wet deposition fraction, as might be expected. The pattern of mercury deposition from
the same model run is similar overall to that seen in the RELMAP simulations reported in the Mercury
Study Report to Congress (U.S. EPA 1997e), but the localized "hot spots" are more prominent.

       In another context, REMSAD has been used in a study to assess the most efficient combination
of NOX controls designed to reach specified reduction levels in nitrogen reaching the Chesapeake Bay via
atmospheric deposition.  In this application, the total reduction desired is held fixed, but the combination
of air quality health benefits attributable to NOX in various locations is combined with specific costs of
NOX reductions in those locations. This forms the basis for both a least-net-cost analysis and for a
potential emission trading approach based on spatially differentiated values for NOX emission reductions
(Krupnicketal. 1998).

Recent Environmental Transport and Fate Research

       The Fate of Mercury in the Lake Superior Basin

       This project, which began in 1998, is designed to examine mercury sources and deposition in the
Lake Superior basin, particularly the contribution of a coal-fired power plant to the mercury loading of
local and regional ecosystems. The research is being conducted at the Minnesota Power and Light's Clay
Boswell Station and at the Wisconsin Electric Power Company's Presque Isle Power Plant and is
expected to answer questions about what forms of mercury are emitted, and how much mercury from the
power plant is deposited locally compared to regionally. The overall goal of the project is to determine
the  fate of anthropogenic mercury in the Lake Superior region, thereby allowing the prediction of the
effects of mercury reduction strategies on the bioaccumulation of methylmercury in fish. The project is
expected to be completed at the end of 2000.

       Sources and Impacts of Nutrient Enrichment in the Gulf of Mexico

       Nutrient enrichment in the northern Gulf of Mexico is responsible for one of the largest zones of
oxygen-deficient bottom waters in the western Atlantic Ocean.  To address this problem, the White
House's Committee on Environment and Natural Resources (CENR) established a multiagency scientific
team to review the extent and causes (including air pollution sources) of hypoxic waters, the ecological
and economic impacts  of hypoxia on the gulf,  and potential solutions. Specifically, the multiagency team
identified six topics of study:

       1.      Distribution, dynamics, and causes of hypoxia in the gulf;

       2.      Ecological and economic consequences of hypoxia in the gulf;

       3.      Sources and loads of nutrients to the gulf from the Mississippi River;

       4.      Effects of reducing nutrient loading to the Mississippi River and the
              gulf;

       5.      Methods to reduce nutrient  loads; and,

       6.      Social  and economic costs and benefits of nutrient reduction strategies.
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The scientific assessments for the above six topics of study are complete and available at
w\vw.nos.noaa.gov/products/pubs_hypox.html. The integrated assessment, which will address all six
topics together, is currently under review and will be available later in 2000. These assessments will be
used by the Gulf of Mexico Program, State agencies, and other involved agencies to combat nutrient
enrichment and hypoxia and measure progress toward the goal of a restored Gulf of Mexico ecosystem.

        Pollutant Exchange Mechanisms

        Many pollutants, depending on their specific chemical and physical properties, can be transferred
between environmental media.  In recent years, research has focused primarily on the exchange of
pollutants between air and water.  The major air-water transfer processes include wet and dry
atmospheric deposition, gaseous exchange, bubble stripping and bursting, and spray transfer (Gustafson
and Dickhut 1997).  In 1996, Hoff et al. reported on revisions to the estimates of atmospheric inputs of 11
organochlorine (OC) chemicals, five trace elements, and four PAHs to the Great Lakes based on IADN
data. Calculations include the flux for wet deposition, dry deposition, and vapor transfer across each of
the lakes, with highest confidence in the estimates for wet deposition and lowest confidence in the
estimates for gas transfer components.  Polychlorinated biphenyls, dieldrin, HCB,  DDE, phenanthrene,
and pyrene all showed net losses from the lakes to the atmosphere via volatilization, while p,p'-DDT was
loaded into the lakes from the atmosphere. Alpha- and y-HCH were near equilibrium with the
waterbodies and the atmosphere, with seasonal changes for a-HCH.  These results show that the waters
of the Great Lakes are close to long-term equilibrium with the atmosphere for most of these chemicals,
but that equilibrium is in a constant state of short-term seasonal displacement and  adjustment (Mackay
and Bentzen 1997). There is a need, however, for integrated assessments of air-water transfer (i.e.,
measuring both water and air simultaneously and over widely varying conditions)  for each lake to obtain
reliable estimates of distribution coefficients, deposition velocities, and loadings from other sources.

        More recently, Gustafson and Dickhut (1997) quantified the gaseous exchange fluxes for PAHs
across the air-water interface of the southern Chesapeake Bay and demonstrated that, for individual
PAHs, different particle characteristics influenced particle-gas distributions at the  urban and rural sites.
Atmospheric PAH concentrations were measured at four sites that were characterized as rural, semi-
urban, urban, and industrialized. Exponential increases in gaseous PAH concentrations with temperature
were observed at the non-rural sites, which the authors suggested was volatilization from contaminated
surfaces during warmer weather.  The PAH gas concentrations at the rural site exhibited little seasonal
variability. Aerosol particle-associated PAH levels were similar at all sites and increased in winter. This
was attributed to the temperature dependence of particle-gas partitioning, including the cold
condensation of gases to background aerosols as air masses were dispersed from source areas to remote
regions, and also increased emissions from combustion of fossil fuel and wood for home heating during
the wintertime. Indications were that either PAH partitioning is not at equilibrium or that different
distribution processes were operating in rural areas of southern Chesapeake Bay.

        Nelson et al. (1998) measured the dissolved- and gas-phase concentrations of nine PAHs and 46
PCB congeners at eight sites on the Chesapeake Bay at four different times of the  year to estimate the
diffusive exchange of gaseous PAHs and PCBs across the air-water interface. They found that PAH
fluxes varied both temporally and spatially in the Chesapeake Bay. Fluxes  were usually larger in the
northern bay as a result of higher gaseous concentrations. Gaseous PAHs were  absorbed into the bay's
surface waters during the spring, and lighter compounds revolatilized in the late summer and early fall
due to seasonal changes in surface water temperature and atmospheric PAH levels. On an annual basis,
Nelson et al. found that the atmosphere is a net source of volatile PAHs to the bay and that gas absorption
may be the largest external source of fluorene and phenanthrene, providing up to three times the
combined loadings from wet and dry aerosol deposition and from the tributaries. In contrast to PAHs,
PCBs volatilized from Chesapeake Bay throughout the year, with the largest fluxes occurring in

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 September due to high dissolved concentrations and warmer water, while the smallest fluxes occurred
 during stratification in June when both dissolved phase concentrations and wind speeds were low.

        A study by Ridal et al. (1997) found that as much as 60 percent of the a-HCH in the air above
 Lake Ontario was derived from the lake itself. Another study of air and water samples from the Bering
 and Chukchi Seas and on a transect across the polar ice cap to the Greenland Sea concluded that soils and
 surface waters containing HCH will be a diffuse, non-point source to the atmosphere that will likely
 maintain detectable atmospheric concentrations for some time into the future (Jantunen and Bidleman
 1996, Li et al.  1998).

        Hurley et al. (1998a) investigated partitioning and transport of total mercury and methylmercury
 in the lower Fox River in Wisconsin and found that resuspended sediments were the predominant source
 of mercury from the Fox River into the Green Bay. The researchers coupled time series data of total
 mercury at the river mouth with transect sampling in the Lower Fox River.  The researchers reported that
 concentrations of unfiltered total mercury were significantly elevated compared with other large
 tributaries to Lake Michigan.  The transect sampling revealed progressively increasing water column
 total mercury concentrations and total mercury particulate enrichment downstream, which the authors
 suggest were consistent with trends in sediment total mercury levels in the river.  Despite elevated total
 mercury concentrations, Hurley et al. (1998a) reported that methylmercury concentrations were relatively
 low, suggesting limited bioavailability of total mercury associated with sediments.

        The processes that take place in the water surface microlayer, particularly those related to
 pollutant exchange mechanisms at the air-water interface, are receiving increasing attention in the
 research literature as one of the most important regions of large surface waterbodies. The surface
 microlayer is the top 30 to 300 urn of a waterbody where atmospheric pollutants first deposit.
 Hydrophobic contaminants, such as PCBs, can adsorb at the air-water interface even without previous
 organic accumulations present due to the lower energy state of the interface. The accumulation of
 organic matter in the surface microlayer also causes a lowering of surface tension values, resulting in
 further enrichment of the organic matter in the surface microlayer as compared to the subsurface water.
 As a result of its organic nature, many pollutants concentrate in the surface microlayer, especially
 hydrophobic organic contaminants such as PAHs, PCBs, and other pollutants that adhere to particles or
 exhibit increased solubility with elevated dissolved organic matter. Yet, despite its importance, the
 surface microlayer is possibly the least understood and poorly characterized region of the aquatic
 environment.

        Liu and Dickhut (1997) compared PAH enrichment in the surface microlayer at an urban site
 (Elizabeth River) and a semiurban site (York River) in the southern Chesapeake Bay watershed and
 found particulate PAH concentrations in the surface microlayer of the Elizabeth River to be an order of
 magnitude higher than in the York River. In comparing the enrichment of PAHs in the surface
 microlayer relative to subsurface water, total PAH concentrations in the surface microlayer were found to
 be 1-4,900 times higher. The authors speculated that the difference in PAH concentrations in the surface
 microlayers of the two rivers was due to a greater contribution of atmospheric deposition of soot-like
 aerosols to the surface microlayer in the urban Elizabeth River.

        Liu and Dickhut (1998) concluded that wind-driven mixing is the principal mechanism that
 distributes suspended particles collected at the air-water interface into the surface microlayer. The
 researchers found a significant relationship (p < 0.05) between wind speed and the surface microlayer
 thickness at the York River site. Thicker surface microlayers result in greater enrichments of organic
 material. Liu and Dickhut (1998) also concluded that enrichment of suspended particles and organic
 carbon in the surface microlayer is related to the sources of these materials in aquatic ecosystems.  In the
 York River, where in situ production of organic matter plays a greater role than runoff and atmospheric
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deposition, enrichment of the surface microlayer appeared to be related to the buoyancy and density of
the particle types.  In contrast, in the Elizabeth River, where productivity is lower, small, dense particles
presumably derived from runoff and atmospheric deposition appeared to accumulate in the surface
microlayer.

MEASURING AND MONITORING TECHNIQUES

Ambient Mercury

       Some of the most important new developments made during the  last few years of atmospheric
mercury research were reliable methods developed to measure reactive (divalent) gaseous mercury
species (Hg+2). The importance of developing a reliable method for measuring ambient Hg+2 (in the
picogram per cubic meter range) was identified as the highest priority research topic at the expert panel
on Mercury Atmospheric Processes convened on March 16-18, 1994 in Tampa, Florida.  Researchers
from the U.S. and Europe reported observing significant spatial gradients in mercury deposition around
urban and industrial areas, indicating local anthropogenic influences. The panel considered improved
characterization of mercury species from sources and at impacted receptor locations to be vital to
elucidate source-receptor relationships.

       Over the past several years, three different methods to measure ambient Hg+2 have been
proposed, including impregnated filters (Gill et al. 1996), refluxing mist chambers (Lindberg and Stratton
1998), and thermal annular denuders (Stevens et al. 1998a). An instrument utilizing thermal denuder
technology recently has been introduced by Tekran Inc. that is capable of continuously measuring both
Hg° and Hg+2 (Stevens et. al. 1998b). Determining the applicability of this new Tekran instrument in
establishing a national automated mercury monitoring network was recommended at the October 1998
Tri-lateral Commission for Environmental Cooperation meeting in Las Vegas, Nevada. The EPA's
National Exposure Research Laboratory is presently evaluating the accuracy and precision of the
available ambient Hg+2 measurement technologies in order to determine  which may be better for routine
monitoring purposes.

       A method for collection and analysis of total particulate mercury (Hgp) was recently published in
the EPA Compendium of Methods for the Determination of Inorganic Compounds in Ambient Air
(Method IO-5). Air is pulled through a pre-fired glass filter, which is subsequently microwave digested
in nitric acid. The filter extract is then analyzed using cold vapor atomic fluorescence spectrometry
(CVAFS). A semi-continuous method for Hgp determination was developed by Lu et al. (1998).
Ambient samples are collected onto a quartz filter housed in a quartz chamber. The quartz chamber is
then heated to 900EC releasing the Hgp as elemental Hg°, which is quantified using CVAFS. Research is
currently under way to merge the thermal quartz filter Hgp technique with the Tekran automated mercury
instrument so that the three most prevalent forms of mercury can be measured at ambient concentration
levels.

Source-Receptor Linkages

       A combination of certain analytical techniques with appropriate modeling approaches has been
used on a number of occasions to ascertain sources contributing certain contaminants in receptor
matrices.  Some of these studies have been conducted in geographic locations  outside the Great Waters;
however, the methods may prove useful in linking sources and receptors in the Great Waters.

       Using a combination of statistical and radioisotope dating techniques, Huntley et al. (1998) found
that the majority of dioxin and furan loads in Newark Bay Estuary sediments were attributable to

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combustion sources and sewage sludge sources. Fifty sediment cores were collected throughout Newark
Bay and analyzed for dioxins and furans. In addition, the cores were dated using radioisotopic
techniques. The samples were grouped into three categories based on their estimated dates of deposition,
and polytopic vector analysis was performed separately on each group to determine the congener
fingerprint patterns. The congener fingerprint patterns were used to identify the source of contamination.

        Biegalski et al. (1998) used source-receptor modeling to attribute metal concentrations in the air
at three sites near Lake Ontario to sources including oil and coal combustion units, mines, incinerators,
and smelting operations. Air samples were collected at the three sites and analyzed for trace elements by
neutron activation analysis.  Factor analysis, elemental ratios, and enrichment factor analysis were used
to determine source-receptor relationships at the three sites.

        Another new technique used to trace persistent organic pollutants to their sources is the
measurement of the enantiomeric ratios of chiral pollutants in the environment (Ridal et al. 1997,
Jantunen and Bidleman 1996).  For example, information about the enantioselective degradation
organochlorine pesticides in soils (e.g., Aigner et al. 1998) could be coupled with data on the
enantiomeric composition of the compounds at the point of deposition to help determine pollutant
sources.

        Using the technique of chemical mass balance, Su and Christensen (1997) determined that coal-
fired power plants, municipal waste incinerators, and pentachlorophenol use areas were major sources of
dioxins and furans in the Housatonic River (CT), Lake Huron, and the Baltic Sea. Other studies reported
in recent years examining source-receptor linkages include an investigation of source-receptor
relationships for mercury in South Florida (Dvonch et al.  1998) and stable isotope analysis for
characterization of pollutants at high elevation alpine sites (Pichlmayer et al. 1998).

EXPOSURE AND EFFECTS  RESEARCH

Endocrine Disrupters

        Endocrine disrupters cause adverse effects by interfering with the normal operation of the
endocrine system. These chemicals can act in a variety of ways, such as by mimicking natural hormones
or by blocking natural hormones. For example, p,p'-DDE (a breakdown product of DDT) has been
shown to inhibit the binding of androgen, a male hormone, to receptors (U.S. EPA 1997b).  By
interfering with the endocrine system, endocrine disrupters may cause changes in homeostasis,
reproduction, and development.  Also, since the neural and immune systems are closely linked to the
endocrine systems, endocrine disrupters may also act as immunosuppressant and neurotoxins. The
Second Great Waters Report to Congress (U.S. EPA 1997b) provides more detail about the possible
mechanisms of endocrine disruption.

        The Second Report to Congress acknowledged that a growing body of animal and human data
suggests that a number of the Great Waters pollutants of concern potentially act as endocrine disrupters.
The report specifically identified 11 of the 15 Great Waters pollutants of concern as possible endocrine
disrupters in wildlife: chlordane, dieldrin, DDT/DDE, hexachlorobenzene, lead, lindane, mercury (in the
form of dimethylmercury), PCBs, dioxins, furans, and toxaphene. These 11 chemicals, as well as
polycyclic organic matter, were also listed as potentially affecting the endocrine system in humans.
Since the Second Report to Congress, scientific research on endocrine disrupters has continued to
provide evidence of their adverse effects in wildlife and humans.  In addition, EPA recently developed a
draft screening and testing approach for systematically identifying endocrine disrupters and quantifying
their effects.
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                                                 Workshop on Perinatal Exposure to Dioxin-like
                                                                Compounds

                                                The workshop, which was held June 13-15, 1993 in
                                                Berkeley, California, considered the effects of
                                                perinatal exposure to chemicals such as dioxins,
                                                furans, and PCBs on the reproductive, endocrine,
                                                neurodevelopmental, and immune systems.
                                                Lindstrom et al. (1995) concluded that many of the
                                                observed effects of these compounds suggest they
                                                act as endocrine disruptors. They further proposed
                                                that neurobehavioral effects (e.g., spatial
                                                learning/memory and motor deficits) may be caused
                                                by complex interactions between neuroendocrine and
                                                neurophysiological systems.
       Recent Research

       Some research on endocrine disruptors is
focused on the role of the endocrine system in
prenatal and perinatal development (see sidebar).
Development is under hormonal control, and a
precise integration of multiple endocrine systems
is required in all stages of development.
Developmental effects traditionally have been
thought of as physical birth defects; however, this
view has been expanded to consider the proper
functioning of the individual throughout its life
cycle. Environmental pollutants that mimic,
block, or modulate the chemical messengers of
the endocrine system can cause a variety of
functional developmental deficits (e.g., impaired learning, memory, motor skills). For example, the
Second Report to Congress describes several findings of a study of children whose mothers ate PCB-
contaminated fish from Lake Michigan. In this study, children born to mothers consuming the greatest
amount of contaminated fish exhibited impaired neurobehavioral ability (e.g., reflexes and response to
stimulation) as infants and impaired intellectual function (e.g., IQ, reading comprehension) at school age
(U.S. EPA 1997b).  The interim findings of two new epidemiology studies support the results of the Lake
Michigan  study.  These effects are important to the Great Waters program because the endocrine
disrupting pollutants found in Great Waters fish tissue may be entering the waterbody through
atmospheric deposition, among other pathways.

•      The Oswego Newborn and Infant Development Project was begun to examine the behavioral
       effects hi human newborns, infants, and children of maternal consumption of Lake Ontario fish
       that were contaminated with a wide range of persistent toxic chemicals, including several Great
       Waters pollutants of concern such as PCBs, hexachlorobenzene, dioxins, dieldrin, lindane,
       chlordane, cadmium, and mercury. Interim study results indicate that newborns of women who
       consumed high levels offish from Lake Ontario performed lower on tests of neurobehavioral
       ability (e.g., reflexes, physiologic responses to stress, and reactivity to stimulation) (Lonky et  al.
        1996).

•      A group of researchers in the Netherlands studied the effects of prenatal exposure to PCBs
       (estimated from levels in mother during pregnancy) and perinatal exposure to PCBs and dioxins
       (measured in breast milk) on the psychomotor and mental development of infants (Koopman-
       Esseboom et al. 1996).  At 3 months of age, infants with higher prenatal exposure to PCBs had
       slightly lower psychomotor scores. At 7 months of age, psychomotor development was
       negatively influenced by perinatal PCB and dioxin exposure. There was no significant influence
       of the perinatal PCBs and dioxin exposure on mental development at 3 and 7 months of age.

       Endocrine Disrupter Screening and Testing Advisory Committee

       The 1996 Food Quality Protection Act and the 1996 Safe Drinking Water Act Amendments
mandated that EPA "develop a  screening program, using appropriate validated test systems and other
specifically relevant information, to determine whether certain substances may have an effect in humans
that is similar to an effect produced by a naturally occurring estrogen, or other  such endocrine effect as
the Administrator may designate."  According to these mandates, EPA was required to develop this
screening  program by August 1998, implement the program by August 1999, and report to Congress on
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the program's progress by August 2000. In response, EPA formed the Endocrine Disrupter Screening
and Testing Advisory Committee (EDSTAC) and charged the committee with designing a screening and
testing program for endocrine disrupting chemicals.  The EDSTAC was composed of representatives
from EPA, other Federal agencies, State agencies, various sectors of industry, water providers, worker
protection organizations, national environmental groups, environmental justice groups, public health
groups, and research scientists.

       The EDSTAC's final report was released in August 1998 (U.S. EPA 1998c). The report outlines
a tiered approach for detecting endocrine disrupting chemicals and quantifying their effects. Under this
system, chemicals may be subjected to high throughput pre-screening, tier 1 screening, tier 2 testing,
and/or hazard assessment. In the report, EDSTAC recommended specific assays that would be
conducted at each step; however, at present, none of the assays are fully validated. The recommended
assays address the need to consider multiple species and endpoints because historic reliance on existing
test species and endpoints was insufficient to appropriately screen, test,  and characterize the risks from
endocrine disruption.

       The EDSTAC estimated that approximately 87,000 chemicals need to be considered for
endocrine disrupter screening and testing, including pesticides, commodity chemicals, naturally
occurring non-steroidal estrogens, food additives, cosmetics, nutritional supplements, and representative
mixtures.  Because simultaneous screening, testing, and evaluation of so many chemicals is far beyond
the capabilities of available facilities and resources, EDSTAC suggested that the universe of chemicals
undergo an initial sorting into four categories with recommended action as follows:

1.     Chemicals that are unlikely to have endocrine disrupting effects would be placed on hold
       initially;

2.     Chemicals with insufficient data would initially undergo high throughput pre-screening and tier 1
       screening;

3.     Chemicals with sufficient data to bypass tier 1 screening would go directly to tier 2 testing; and,

4.     Chemicals with sufficient data would go directly to hazard assessment.

       The EDSTAC estimated that following the sorting exercise, approximately 62,000 chemicals
would still require screening and/or testing. Therefore, EDSTAC recommended these chemicals should
be prioritized for further evaluation and that the Endocrine Disrupter Screening and Testing Program
should be implemented in a phased manner (i.e., high priority chemicals screened and tested during
Phase 1). The core priority setting process recommended by EDSTAC focuses on giving high priority to
chemicals with widespread exposure at the national level.  The EDSTAC also recommended a
nomination process to accommodate chemicals for which exposure is disproportionately high for specific
groups, communities, or ecosystems.

       As noted previously, some of the Great Waters pollutants of concern (e.g., PCBs, dioxins) are
already known to possess endocrine disrupting capabilities. These chemicals would most likely be
categorized into group 3 or group 4 using the sorting scheme recommended by EDSTAC.  Nevertheless,
at this time, it is uncertain what priority would be given to individual Great Waters pollutants of concern
for further evaluation under the Endocrine Disrupter Screening and
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Chesapeake Bay Toxicity Testing and Biological Community
Assessments

       A recent pilot project attempted to integrate an environmental ambient toxicity testing approach
with a biological community assessment approach to determine to what extent toxic pollutants affect fish
populations in Chesapeake Bay. The results are presented as tributary-specific ambient toxicity testing in
the framework of a toxicity risk ranking model developed specifically for contrasting complex
toxicological results with biological indicators of community health. The two tools that were combined
in this project include an ambient toxicity approach which provides a picture of biologically significant
environmental contamination and a toxicological risk ranking method which integrates an array of
toxicological data results into a site-specific "risk score" (Hartwell et al. 1995).

       Four tributaries of the Chesapeake Bay were chosen as test sites for this project.  Each tributary
represents a watershed impacted by different land uses.  The Curtis Creek watershed is dominated by
urban and commercial development and was selected as an example of a polluted area. The Rock Creek
watershed is dominated by urban development but does not have any major industrial areas. Fishing Bay
is located in a lightly developed area and is over 70 percent forest and wetlands. This area is considered
a relatively uncontaminated environment. The Wicomico River watershed is dominated by forest and
agriculture and represents a clean reference area with no direct point source pollution.  Fish community
and water column sampling was performed between May to September 1993.  For the ambient toxicity
program, a ranking scheme of five components (end-point severity, response proportion, test variability,
site consistency, and number of measured end-points) was developed to evaluate the toxicological results
on a site-by-site basis (Hartwell et al. 1995).

       The  results indicate that the assays are sensitive enough to identify biologically significant
contamination. Trends between the Index of Biotic Integrity (IBI) scores, which are an expression of the
overall condition of the structure and function of the fish community, and the toxicological  risk ranking
scheme exist; however, stronger statistical associations are observed between the risk scores and specific
metrics in the fish community database. As other studies advance, additional sites can be included in the
analyses. As more information is included in the toxicological database, correlations with a variety of
community databases will be possible (Hartwell et al. 1995).

ATSDR PCB/PAH Great Lakes Sensitive Population Studies

       The  Great Lakes Critical Programs Act, enacted in 1990, required EPA in consultation with the
Agency for Toxic Substances and Disease Registry (ATSDR) to assess the adverse affects of water
pollutants in the Great Lakes. In 1996, EPA and ATSDR published a Report to Congress that
summarized existing research on the human health  effects of Great Lakes pollutants. In addition,
ATSDR developed a Great Lakes Health Effects Research Strategy that the agencies used to guide a suite
of new epidemiological studies. In particular, EPA through ATSDR made ten grants to support research
related to potential adverse human health effects from consumption of contaminated Great Lakes fish.
Eight of the grants supported investigations focusing on susceptible populations (i.e., Native Americans,
sports anglers, the urban poor, pregnant women, and fetuses and nursing infants of mothers who eat
contaminated fish). The ninth and tenth grants supported the development of an interlaboratory quality
assurance and quality control program and the development of more sensitive methods for detecting
contaminants in biological samples (U.S. EPA 1999f).
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                                    CHAPTER V
    NEXT STEPS  FOR THE  GREAT WATERS PROGRAM
                                                          This report describes significant new
                                                   scientific and programmatic developments
                                                   relevant to the Great Waters program since
                                                   the Second Report to Congress (June 1997).
                                                   These developments support and build on the
                                                   three broad conclusions presented in the First
                                                   and Second Reports to Congress:

                                                   •      Atmospheric deposition can be a
                                                          significant contributor of toxic
                                                          chemicals and nitrogen compounds
                                                          to the Great Waters.  The relative
                                                          importance of atmospheric loading
                                                          for a particular chemical in a given
                                                          waterbody depends on many factors,
                                                          including characteristics of the
                                                          waterbody, properties of the
                                                          chemical, and the kind and amount of
                                                          atmospheric or water discharges.

                                                   •      A plausible link exists between
                                                          emissions into the air of Great
                                                          Waters toxic pollutants of concern,
                                                          the atmospheric deposition of these
                                                          pollutants (and their transformation
                                                          products), and the concentrations of
                                                          these pollutants found in water,
                                                          sediments and biota, especially fish
                                                          and shellfish. For mercury, fate and
                                                          transport modeling and exposure
       assessments predict that the anthropogenic contribution to the total amount of methylmercury in
       fish is, in part, the result of anthropogenic mercury releases from industrial and combustion
       sources increasing mercury body burdens (i.e., concentrations) in fish. Furthermore, the
       consumption offish is the dominant pathway of exposure to methyhnercury for fish-consuming
       humans and wildlife. However, what is known about each stage of this process varies with each
       pollutant (for instance, the chemical species of the emissions and its transformation  in the
       atmosphere).

       Airborne emissions from local as well as distant sources, both within and outside the U.S.,
       contribute pollutant loadings to waters through atmospheric deposition. Determining the relative
       roles of particular sources contributing to specific waterbodies is complex, requiring careful
       monitoring, atmospheric modeling, and other analytical techniques.
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 Chapter V
 Findings, Conclusions, and Recommendations
                                                Strategic Themes of EPA's Great Waters Program

                                               (1) The EPA will continue ongoing efforts to implement
                                               section 112 and other sections of the CAA and use
                                               results from this report in the development of policy that
                                               will reduce emissions of the Great Waters pollutants of
                                               concern.

                                               (2) The EPA recognizes the need for an integrated
                                               multimedia approach to the problem of atmospheric
                                               deposition of pollutants to waterbodies and will continue
                                               to pursue implementation of programs available under
                                               various Federal laws to reduce the human and
                                               environmental exposure to pollutants of concern.

                                               (3) The EPA is committed to supporting research
                                               activities that address the goals of section 112(m) of
                                               the CAA.
        As Chapter II showed, there has been
significant progress in environmental research
since the Second Report to Congress,
particularly in monitoring and modeling
pollutant transport and loadings at the regional
and national scale. As a result, spatial and
temporal trends in pollutant emissions,
loadings, and effects  are becoming clearer as
the identified research gaps are being
addressed.

        Chapter III described more than 60
relevant programs and activities, ranging in
scale from local to international, many of
which directly or indirectly contribute to
reducing loadings and exposures for many of
the pollutants of concern. Collectively, these
programs and activities show a high level of interagency, intergovernmental, and public-private
cooperation. In addition, those programs led or supported by EPA have advanced the strategic themes
and recommended actions developed in the First and Second Reports to Congress (see text box),
including pursuing integrated multimedia approaches to environmental protection. These programs have
also furthered the Agency's Clean Air, Clean Water, International, Pollution Prevention, and Sound
Science goals under the Government Performance and Results Act.

        Chapter IV summarized notable developments in science and tools since the Second Report to
Congress. Because of the large  scale and technical complexities of the problems, considerable time,
effort, and resources have been expended to develop tools to understand and resolve them.  In part
because of the efforts of the Great Waters program, there is now a greater level of coordination among
research agencies and institutions to target areas of critical uncertainty and suspected threats to human
health and the environment.  Some of the recently-developed tools and research programs will generate
important new data and findings that will be available for future Great Waters Reports to Congress and
will enable EPA to make further progress in reducing the harmful effects  of atmospheric deposition to
the Great Waters.

        Like the Second Report  to Congress, the key conclusions of this report and recommendations for
continued or further action are organized by the subject areas EPA is required to assess under the Great
Waters provisions of the CAA, namely the sources and loadings of the pollutants of concern to the Great
Waters, and their environmental and public health effects.  In addition, this chapter addresses the
description of any revisions to CAA and other Federal requirements, standards, and limitations, (if such
revisions are necessary), as well as whether the pollutants of concern have caused any exceedances of
water quality or drinking water standards.

        In general, deposition rates of the air pollutants of concern to the  Great Waters are decreasing or
remaining steady. Also, while we observe a trend toward reduced concentrations of these pollutants in
water and other media for many atmospherically deposited pollutants of concern, this is not the case for
all of them. Potential human health risks are greatest for those individuals who consume fish from
contaminated waterbodies. Some pollutants continue to contribute to significant and widespread
ecological problems in the Great Waters.
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        Substantial uncertainties remain about the extent, sources, fate and effects of atmospheric
deposition. This report supports continued research targeted toward addressing remaining uncertainties
and providing decisionmakers with the tools and information they need to assess potential risks and
determine whether further action is necessary to reduce them. The Agency believes that considerable
continued effort is justified to address critical remaining uncertainties, improve the characterization of
the contribution of atmospherically deposited pollution to the Great Waters, and to further reduce this
pollution.
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V.A  POLLUTANT SOURCES

       In the past 2 years, new models and model enhancements, tools, and emissions inventories,
including long range transport atmospheric modeling (e.g., RELMAP), source "fingerprinting," back
trajectory analysis, EPA's National Toxics Inventory, and the Great Lakes Regional Air Toxics Emission
Inventory, have provided new information to help identify sources of pollutants which are deposited to
waterbodies. Emissions of some Great Waters pollutants of concern have decreased, while others
remained constant or varied. Additional emission reductions are expected to result from continued
implementation of current regulations and nonregulatory programs, as well as development of future
regulations, pollution prevention initiatives, and voluntary actions.

FINDINGS AND CONCLUSIONS

•      Emissions and numbers of U.S. anthropogenic sources have declined for mercury, lead,
       dioxins and furans, and the banned and restricted use substances.  For example, lead
       emissions in the Great Lakes region declined at a rate of 6.4 percent per year from 1982 to 1993
       reflecting the national decline in lead emissions resulting from the phase-out of leaded gasoline
       in automobiles.

•      Emissions from U.S. anthropogenic sources for NOX have remained relatively constant.
       For cadmium, emissions in the Great Lakes region have not shown a trend since the 1980s.
       Trends for POM/PAHs are not known. For example, nationwide NOX emissions have
       fluctuated around 21 to 23 million metric tons per year from 1988 to 1997.

•      The sources of atmospheric deposition vary, depending on the pollutant.  As an example,
       sources of atmospherically-deposited mercury include emissions from industrial and combustion
       sources, emissions from natural sources such as volcanoes, and re-emission from mercury-
       contaminated soils and water. These sources can be in the U.S. or other countries, and the
       mercury emissions can be deposited near the source or transported long distances across
       international borders.  Some point sources emit significant amounts of reactive chemical forms of
       mercury which are deposited locally, near the source of emissions. Determining a more complete
       picture of atmospheric deposition to the Great Waters requires ascertaining the contributions of
       each of the relevant sources.

•      Local sources, including urban areas, can have a large impact on local pollutant deposition
       rates.  Recent research under the AEOLOS1 project continues to show that the diffuse  emissions
       of urban areas (i.e., urban plumes) can significantly affect nearby deposition rates. For example,
       deposition rates of PCBs and polycyclic aromatic hydrocarbons (PAHs) have been found to be
       elevated over southern Lake Michigan near the Chicago urban area. Therefore, estimates of
       pollutant loadings and net flux at the waterbody-scale (e.g., for Lake Michigan) may be sensitive
       to the placement of monitoring sites.

•      Loadings of banned pesticides to the Great Waters are primarily from sources that are
       difficult or may not be practical for EPA, States, or tribes in the U.S. to further regulate.
       Although there are no major sources of banned pesticides in the U.S., loadings continue from
       remaining consumer stocks, evaporation from soils, resuspension of contaminated sediments, and
        Atmospheric Exchange Over Lakes and Oceans Surfaces (see page IV-13)
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       airborne transport from other countries.  Future reductions must come from clean up of existing
       stockpiles and contaminated sites and reductions in airborne pollutants transported from other
       countries. Research continues at EPA and other institutions on soil remediation methods that
       will reduce emissions of these pollutants from contaminated sites.

•      Implementation of existing EPA regulations is expected to further reduce emissions of
       mercury, NOX, POMs, dioxins and furans, cadmium, lead, and hexachlorobenzene, and
       contribute to declines in deposition of these pollutants. The EPA regulations issued over the
       last few years will significantly reduce known sources of these Great Waters pollutants of
       concern.  For instance, the emission standards and guidelines for municipal waste combustors
       and for hazardous/medical/infectious waste incinerators will reduce mercury and dioxin
       emissions from these sources by greater than 90 percent from 1990 when fully implemented in
       2000 and 2002, respectively. Emission standards for hazardous waste-fired combustors were
       issued in 1999 and are expected to be implemented in 2002.  This rule will reduce dioxins and
       furans by 70 percent, as well as other pollutants such as mercury. In addition EPA's NOX SIP
       call, when implemented, is expected to reduce NOX emissions by about one million metric tons
       during the summer ozone season, contributing to a projected decline in NOX emissions through
       2005.

•      Developments in pollution models and source information are improving our ability to
       identify and quantify sources and deposition of pollutants. In recent years, EPA andNOAA
       have continued to develop and refine models and source information in order to improve
       emissions estimates and understanding of the relative importance of various sources to
       atmospheric deposition.  For example, the long range atmospheric transport model RELMAP2
       was used to estimate domestic and global mercury deposition and RADM3 was used to estimate
       coastal NOX deposition.  However, there is still a critical need for key inventory information on
       the pollutants of concern (e.g., ammonia, speciated data for metals, more accurate data for
       pollutants emitted in small quantities, locational data for area and mobile sources) in order to
       generate more effective model estimates that can be used in control strategy decisions.

RECOMMENDATIONS FOR CONTINUED AND FURTHER ACTION

•      Within any limitations imposed by court rulings, EPA will ensure the timely implementation of
       NOX control strategies already put in place, such as the NOX SIP call and emission standards and
       guidelines for municipal waste combustors, as well as the Tier II tailpipe standards, which are
       expected to significantly reduce on-road mobile source NOX emissions throughout the year. The
       EPA will proceed with full implementation of the section 126 rule to achieve the required NOX
       reductions by May 1, 2003. Finally, EPA will encourage innovative, nonregulatory approaches
       to reducing NOx emissions such as "Smart Growth" planning in urban areas and energy
       conservation programs.

•      The EPA will continue to develop and implement technology-based standards and guidelines
       under sections 111, 112, and 129 of the  CAA that will achieve further reductions of Great Waters
       pollutants of concern. For instance, EPA expects to complete MACT standards mandated by
       section 112 for source categories which emit pollutants of concern (e.g., chlorine manufacturing
        '' Regional Langragian Model of Air Pollution

        ' Regional Acid Deposition Model
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        [chlor-alkaliplants], coke ovens [pushing, quenching and battery stacks], industrial boilers,
        institutional and commercial boilers, iron and steel foundries, and refractory manufacturing) by
        2002. Also, EPA expects to complete regulations under section 111 and 129 for commercial and
        industrial waste incinerators by November 15, 2000, and for small municipal waste combustors
        by 2001.  In addition, EPA expects to finalize the list of area source categories by 2003 and
        expects to complete regulations by 2004 for the area source categories published in the
        integrated urban air toxics strategy on July 19, 1999.

        The EPA expects to complete collection and analysis of information on mercury emissions and
        controls for coal-fired utility boilers and issue the regulatory determination for air toxics from
        electric utilities by December 15, 2000.

        Under the residual risk program, EPA will assess risks associated with exposures from emissions
        of Great Waters toxic pollutants of concern, using risk, exposure, and other relevant public
        health and environmental information developed by EPA offices and its partners.  These
        assessments will focus on the risk remaining from categories of air toxics sources (or individual
        sources within the categories) for which MACTstandards have been applied, and include
        assessing the public health risk from eating fish contaminated by these sources and risks to
        ecosystems.  Where analyses indicate unacceptable adverse effects to public health or the
        environment from these sources of pollutants, EPA will pursue appropriate actions to reduce
        risks.

        The EPA will continue to explore ways to integrate the authorities within single media statutes
        and their programs (i.e., CAA, Clean Water Act) in order to support multimedia strategies to
        reduce pollutants of concern to the Great Waters. This includes building on recent progress to
        increase communication and program coordination between EPA's Air and Water programs
        (e.g., pulp and paper "cluster" rule). For example, EPA's Office of Water and Office of Air and
        Radiation (OAR) will consider how to involve  the air program in review ofTMDLs that list air
        sources.

        The EPA  will encourage innovation among States to address local air sources of persistent,
        bioaccumulative toxics and promote voluntary pollution prevention actions, where appropriate.
        For instance, EPA will document the results of projects under way nationwide to reduce, collect,
        and recycle mercury-containing products and disseminate the information broadly.

        The EPA will continue to encourage phase-out and safe disposal of banned and restricted Great
        Waters substances (e.g., "clean sweeps "for banned pesticides).  The EPA, working with NOAA
        and other Federal and State partners, will continue to monitor levels in the environment (e.g.,
       fish tissue levels) to verify trends in loadings.

        The EPA expects to complete development of a Mercury Research Strategy in 2000. The
        Strategy will describe the key research questions for mercury that EPA plans to address over the
        coming 5 years and will identify other technical and scientific issues that are important to the
        Agency's efforts in addressing mercury.

        The EPA expects to finalize in 2000 the Dioxin Reassessment following peer review. This report
        will update our scientific understanding of the  health risks resulting from exposure to dioxins.

        The EPA will improve the public's "Right to Know" about certain toxic compounds. The EPA
        will implement the rulemaking which added dioxin and other persistent, bioaccumulative, toxic
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       chemicals to the Toxic Release Inventory and lowered the reporting threshold for these and other
       listed chemicals under the TRI. The EPA also expects to issue to the public by 2001 the first TRI
       reports that include these substances.

       The EPA will continue to lead efforts to research viable controls for sources of pollutants of
       concern. For example, research will continue on mercury from combustion processes, including
       modifying the mixtures and inputs of fuel, and more effective control devices on emitted gases
       and particles.  This research will also evaluate costs and relative effectiveness of control
       options.

       The EPA will continue to provide leadership in reducing transboundary transport of mercury,
       DDT, PCBs, chlordane, and other toxic pollutants of concern by achieving assessment and
       reduction goals contained in international agreements (e.g., Great Lakes Binational Strategy,
       CEC4 North American Regional Action Plans, UN/ECE LRTAP5 Heavy Metals Protocol). The
       EPA will support efforts to share technology, information and expertise with other countries on
       reducing releases to the environment and on cost-effective alternatives. The EPA will also
       continue to provide support to the international negotiations on persistent organic pollutants
       under the United Nations Environmental Programme.

       The EPA will continue to pursue international agreements to reduce transboundary NOy
       including negotiating an ozone annex to the US/Canada Air Quality Agreement.

       The EPA will continue to support joint work with States and industry to fill gaps in source
       categories and further refine emission measurement methods and inventories for Great Waters
       pollutants of concern (e.g., speciated data on pollutants such as metals andPAHsfor the Great
       Lakes RAPIDS inventory and for the National Toxics Inventory) so that they can be used
       effectively in models being developed.
         Commission for Environmental Cooperation

       5 United Nations Economic Commission for Europe Long Range Transboundary Air Pollution Convention

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V.B
CONTRIBUTION OF ATMOSPHERIC DEPOSITION TO
POLLUTANT LOADINGS IN THE GREAT WATERS
       Research, monitoring, and modeling of pollutant inputs to the Great Waters has continued to
provide important information about loadings. Recent results from available data indicate that
atmospheric inputs of some pollutants of concern are decreasing while others remain constant. However,
there is considerable uncertainty in the data because of limited monitoring, technological barriers, and
variable collection and analytical methods, making it difficult to adequately characterize historical as
well as current conditions and to discern pollution trends. In addition, not all Great Waters waterbodies
or all pollutants of concern have been studied.

FINDINGS AND  CONCLUSIONS

•      Based on available data, atmospheric deposition of lead, cadmium, POM/PAHs, PCBs, and
       some pesticides (e.g., DDT, hexachlorocyclohexanes, dieldrin) to the Great Lakes has
       continued to decline in recent years. Similar trends are seen in some other Great Waters.

•      Based on available data, atmospheric deposition of nitrogen compounds has remained
       relatively unchanged in the Great Waters in recent years. This correlates with a relatively
       constant trend in NOX emissions during the same period.  Considerable uncertainty exists,
       however, concerning dry deposition of nitrogen compounds and wet organic nitrogen deposition.

•      Despite recent declines, atmospheric deposition continues to be a significant contributor of
       certain pollutants to some Great Waters. For example, one researcher has reported that
       atmospheric deposition contributes 70 to 90 percent of the direct lead inputs to the Long Island
       Sound. In the Great Lakes, according to another study, the relative contribution of dioxins and
       furans from the atmosphere ranges from 5 to  100 percent. Various studies of nitrogen deposition
       to Atlantic and Gulf Coast bays and estuaries indicate that 2 to 38 percent of total nitrogen inputs
       are attributable to atmospheric deposition.

•      While run-off from fertilizer application, farm animal operations, waste treatment,
       industrial effluents, and crop residues continues to be the largest contributor to total
       nitrogen loadings, atmospheric inputs of nitrogen compounds to the Great Waters are
       much higher than natural rates.  Although atmospheric loading rates of inorganic nitrogen
       appear to have  leveled off, the rates remain many times greater than natural rates and have the
       potential, when combined with other loadings such as runoff, to overwhelm the assimilative
       capacities of surface waters. Research is ongoing into the lesser known but apparently important
       forms of nitrogen deposition (e.g., dry deposition, organic nitrogen). In addition, nitrogen
       saturation of upland forests, grasslands, and agricultural fields may occur in some areas and
       could significantly increase the rate of nitrogen transport from upland watersheds to coastal
       waters in the future, even if atmospheric loading rates remain constant.

•      Although considerable uncertainty remains, EPA's 1997 Mercury Study Report to Congress
       estimates, based on a modeling analysis, that one-third (52 tons) of the anthropogenic
       mercury emitted annually in the U.S. is deposited in the continental U.S., along with an
       estimated 35 tons from the global reservoir (which includes U.S. anthropogenic as well as
       natural and re-emitted mercury emissions). These results to date suggest that the remaining
       two-thirds (~ 107 tons) of annual U.S. anthropogenic emissions are transported beyond U.S.
       borders, where they diffuse into the global reservoir. As U.S. anthropogenic emissions are
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       reduced, the relative contribution from the global pool will be even larger, particularly if similar
       control actions are not undertaken in other countries.  Studies of mercury deposition to certain
       Great Waters indicate that atmospheric deposition contributes between 10 and 85 percent of the
       total mercury loadings to these waterbodies.  Because a deposition monitoring network for
       mercury has only recently been established, there are not yet sufficient data to determine
       monitored trends in mercury deposition levels.

       Certain banned and restricted use pesticides are projected to be the first pollutants of
       concern to be reduced to concentrations below current atmospheric detection limits in the
       Great Lakes atmosphere, indicating that risk management strategies are having the
       intended impact. Based on recent academic research on atmospheric pollutant concentrations in
       the Great Lakes region, DDT and DDE, followed by dieldrin and chlordane, are estimated to fall
       below current detection limits in the atmosphere between 2010 and 2020. Hexachlorocyclo-
       hexane and hexachlorobenzene are projected to fall below current detection limits in the
       atmosphere over the Great Lakes by 2030 and 2060, respectively. These estimates assume
       current rates of long-range transport of these pollutants into the region. Because of their
       persistence, it should be noted that elimination of these pollutants in the atmosphere does not
       mean that concentrations would be eliminated in deposited media (e.g., sediments) by these
       dates.  However, these estimates indicate that reduction strategies in the Great Lakes, along with
       the original bans or restrictions on the use of these substances, are having the intended effect.

       Significant progress has been made involving monitoring and modeling research focused on
       the factors that affect pollutant fate and transport in regional-scale air masses and in
       watersheds.  Since the Second Report to Congress, there have been significant advances in
       monitoring and modeling of pollutant transport and loadings at both regional and national scales.
       Recent accomplishments include data collection and analysis of results from the AEOLOS
       project, establishment of the Mercury Deposition Network (part of the National Atmospheric
       Deposition Program), applications of the HYSPLIT/TRANSCO6 computer program,
       development of the Models-3 community multiscale air quality modeling system, monitoring
       established by the South Florida Mercury Science Program, and progress on the Lake Michigan
       Mass Balance Study. The Integrated Atmospheric Deposition Network, an international effort to
       monitor air toxics deposition, has produced a long-term data set on loadings trends in the Great
       Lakes. As in past years, much of the research on modeling of pollutant loading rates has focused
       on mechanisms of direct pollutant deposition to surface waters (e.g., pollutant exchange
       mechanisms, surface microlayers). However, a growing area of research addresses factors, such
       as the effects of land cover,  weather events, that affect the fate and transport of pollutants in
       watersheds and tributaries.  For example, a variety of factors influence how much deposited
       mercury will be methylated and incorporated into the  food chain, including lake and watershed
       characteristics, water chemistry, and the length of the food chain.

       Long-range transport from other U.S. regions or other countries is estimated to contribute
       significantly to atmospheric loadings of pollutants  of concern to the Great Waters. As
       stated above, EPA estimates that 35 tons of mercury from the global reservoir (derived from both
       foreign and U.S. sources) are deposited annually in the U.S., representing 40 percent of the total
       mercury deposition to the U.S. In a modeling study conducted in the northeastern U.S., sources
       from outside the study region contributed 30 percent of the mercury loadings within the study
       region and the global reservoir contributed approximately 20 percent. Another modeling study
         Hybrid single particle Lagrangian integrated trajectory/transfer coefficient (see page II-31)

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       conducted to assess sources of dioxin to the Great Lakes basin shows that sources as far as
       central Canada may influence deposition of dioxin to the lakes.

RECOMMENDATIONS  FOR CONTINUED  AND  FURTHER ACTION

•      By summer 2000, EPA expects to develop a -workplan to assess  atmospheric deposition on a
       regional basis.  This work plan would include: targeting State-identified impaired waterbodies;
       examining what rules or activities are in place that address impairment caused by atmospheric
       deposition; and, determining what, if any, additional actions are necessary to address
       impairment caused by atmospheric deposition. In addition, EPA expects to revise this work plan
       every two years based on updated scientific information and stakeholder input.

•      The EPA will work with national deposition monitoring programs, States, National Estuary
       Programs, NOAA, and other research institutions to establish monitoring sites in coastal areas
       where they do not already exist, as appropriate. The EPA will encourage expansion of the
       National Atmospheric Deposition Program's Mercury Deposition Network, the continuation of
       other toxics deposition monitoring networks, such as the Integrated Atmospheric Deposition
       Network, and the development of a national air toxics monitoring network to support assessment
       of the contribution of long-range transport to deposition of Great Waters pollutants of concern
       in the U.S. and to evaluate the impact of urban sources.

•      The EPA will encourage the use of standard monitoring methods to enable comparison of data
       and trends analysis.  Where methods for measuring atmospheric deposition for pollutants of
       concern do not exist, EPA, working with NOAA and other Federal colleagues and key
       institutions such as the National Atmospheric Deposition Program, will continue to lead and
       support efforts to develop technology and establish standard methods (e.g., POM and PAH,
       mercury species, dissolved organic nitrogen, and dry deposition of pollutants).

•      The EPA will continue to work with NOAA and other scientific partners to develop, refine, and
       validate modeling tools that help us to better understand the pathways of the pollutants of
       concern —from emissions to transport to deposition to fate to environmental and human health
       effects.

•      The EPA will work with NOAA and other agencies to better quantify the indirect loadings of
       atmospheric deposition to the Great Waters through the development of tools that can quantify
       watershed transport of pollutants of concern.

•      The EPA will continue to support international efforts to quantify the transboundary
       contributions of pollutants of concern, such as the Commission for Environmental Cooperation
       efforts to assess continental pollutant pathways and the Binational Strategy challenge to assess
       global sources of pollutants to the Great Lakes.
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V.C  ENVIRONMENTAL AND PUBLIC  HEALTH EFFECTS

       Because the Second Report to Congress discussed potential adverse human health and
environmental effects from exposure to the Great Waters pollutants of concern in considerable detail, this
report focused on observed changes in exposure levels and trends in observed effects, to the extent that
data were available.  Scientific research has continued to improve our understanding of the toxic effects
of the pollutants of concern, including endocrine disruption. Concentrations of some of the pollutants of
concern in the environment have decreased in recent years, while others have remained constant or are
variable. At some locations, mercury concentrations are at levels sufficient to produce adverse health
effects for certain groups consuming large amounts of contaminated fish (e.g., young children, pregnant
women and their developing fetuses, women of child-bearing age, and populations that subsist on fish),
as well as ecological risks.

FINDINGS AND CONCLUSIONS

       Available monitoring data indicate that concentrations of dioxin/furans and PCBs, in the
       sediment, water, and biota of several of the Great Waters appear to be declining, while
       concentrations of lead, cadmium, mercury, and POM/PAH are too variable for a trend to
       be discerned.  For example, concentrations of PCBs in biota have continued to decline in the
       Great Lakes, with PCB concentrations in St. Lawrence River fish decreasing by a factor of 30
       since 1975. Trends in concentrations of lead, cadmium, mercury, and POM/PAH were more
       variable or could not be discerned from the available data. Although recent research did not
       address contamination levels of all pollutants of concern, no identified studies indicated
       increasing levels of pollutants of concern in the Great Waters.

•      Available monitoring data indicate that various pollutant concentrations in sediments,
       water, and/or biota of the Great Waters have been detected at levels resulting in exposures
       that are high enough to cause adverse environmental effects. As was reported in the Second
       Report to Congress, a number of regional- and national-scale assessment and monitoring
       programs (e.g., the National Sediment Quality Survey, Benthic Surveillance Project) suggest that
       the ecological health of many Great Waters are impaired by pollution that is partially attributable
       to atmospheric deposition.  Further evidence of ecological impairment includes research results
       indicating that up to 30 percent of the loons in the northeastern U.S. have mercury levels
       sufficiently high to cause adverse effects.

•      Excess nitrogen loadings can cause algal blooms (including harmful algal blooms), shifts in
       aquatic vegetation, fish declines and  kills, and shellfish bed losses. The NOAA Estuarine
       Eutrophication Surveys indicate that the adverse effects of excess nitrogen loadings  are currently
       evident to some degree in approximately 89 percent of the U.S. coastal Great Waters. Numerous
       studies on individual  estuaries have estimated that 20 to 40 percent of total loading of nitrogen
       compounds can come from atmospheric deposition, with the rest of the loading originating from
       water discharges or land-use activities.

•      Fish consumption is the primary pathway of human exposure to mercury, is an important
       pathway for dioxin and PCBs, and may be an important pathway for various other Great
       Waters toxic pollutants.  While such exposures may not be of concern for most  of the
       general population,  for certain pollutants and contamination situations, certain groups
       such as young children, developing fetuses, subsistence fish-eating populations, and others
       who consume large amounts of contaminated fish, may be at risk. For mercury  specifically,
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        exposures do not appear to pose a health risk to people consuming average amounts offish, but
        sensitive sub-populations (e.g., young children, and pregnant women and their developing
        fetuses) with higher than typical fish consumption are at risk.  Also at risk are subsistence fish-
        eating populations who consume large amounts offish. The extent of risk for these groups
        depends on the amount offish consumed and the mercury concentrations present in the fish.

 •       The role of transformation processes on certain pollutants once they are emitted is an
        important phenomenon which can increase their toxicity and persistence in the
        environment. For instance, mercury emitted by industrial or combustion processes becomes
        much more toxic and biologically available after it is deposited in the  environment and
        transformed to methylmercury. Another example is the transformation of alpha- and gamma-
        hexachlorocyclohexane to beta-hexachlorocyclohexane (HCH).  More research on these
        transformation processes is needed to better understand their role and to develop appropriate
        responses.

 •       Evidence for adverse effects from endocrine disrupting chemicals continues to be found.
        Recent research provides additional evidence of the adverse effects of endocrine disrupters on
        both wildlife  and humans, and at least two Great Waters pollutants of concern (i.e., PCBs and
        dioxins) are known to possess endocrine disrupting capabilities. The EPA has worked with
        various governmental and non-governmental interests to develop a screening and testing
        approach for systematically identifying endocrine disrupters and quantifying their effects.

 RECOMMENDATIONS FOR CONTINUED AND  FURTHER ACTION

 •       The EPA will continue to support the development and validation of modeling tools which
        address the transport and fate of pollutants in ecosystems and characterize risk, such as the
        Total Risk Integrated Methodology. The EPA will also continue to support the improvements in
        inventories, monitoring data, and human and environmental effects information necessary to
        effectively apply these tools.

 •       In conjunction with its related efforts on persistent, bioaccumulative, toxic pollutants (e.g., the
        Great Lakes Binational Strategy and the Persistent, Bioaccumulative Toxics Initiative), EPA will
        identify and evaluate additional pollutants which may be  of concern to the Great Waters.

 •       The EPA expects to explore one or more community-based pilot projects to develop and examine
        methodologies for characterizing local risks and to work  with stakeholders on risk reduction
        strategies. In conducting such pilot studies, the EPA will consider cumulative risks presented by
        exposures to air toxics emissions in the aggregate, including exposures through noninhalation
       pathways, such as consumption of contaminated fish from waterbodies affected by deposition of
        air toxics.

 •       The EPA will continue to support work to quantify the ecological effects of atmospheric
        deposition.  For instance, EPA will support research to answer critical questions related to the
        assessment of pollutant exposures for varying life stages and for species at various levels of the
       food chain.

 •       The EPA expects to complete, by December 2000, the new Water Quality Criterion Methodology
       for Human Health to better reflect pollutants that bioaccumulate and the Nation's changing fish
        consumption patterns.
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        The EPA will work with NOAA, US Fish and Wildlife Service, other Federal agencies, States,
        and tribes to expand the geographic coverage and consistency ofwaterbody monitoring to
        enable more accurate characterizations of the extent of contamination and ecosystem effects due
        to atmospheric deposition of Great Waters pollutants of concern.  In addition, EPA will increase
        efforts to implement nationally-consistent methods and protocols for assessing contaminants in
       fish and wildlife and establishing consumption advisories.

        The EPA, working with States, tribes, and other relevant partners, will continue to support
        efforts to improve awareness and understanding offish consumption advisories among
       populations most at risk to exposure to the Great Water pollutants of concern.

        The EPA will provide leadership for efforts to examine the mechanisms of action and resulting
        effects (e.g., reproductive failure, death, species diversity, ecological sustainability) of exposures
        to realistic concentrations of common contaminants, alone and in combination. The EPA will
        also lead the development of predictive models to assess likely effects of single and multiple
        stressors and alternative environmental conditions on individual aquatic plants and animals,
       populations, communities, and ecosystems.

        The EPA will continue to pursue as apriority its research plan for endocrine disrupters,
        covering ten broad categories of research needs:  basic research,  biomarkers, database
        development, exposure determination, exposure follow-up, mixtures, multidisciplinary studies,
        risk assessment methods, hazard identification, and sentinel species.

        The EPA will accelerate work to better quantify the water quality  benefits of air pollution
        controls in order to provide decisionmakers with critical information on environmental
       strategies to reduce the extent of contamination by Great Waters pollutants  of concern.  By 2001,
       EPA expects to conclude a pilot study of the economic benefits of reducing nitrogen deposition in
        a particular estuary, developing methodologies that could be applied to other waterbodies.
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V.D  EXCEEDANCES OF WATER QUALITY OR DRINKING WATER
       STANDARDS

       Atmospheric deposition and other inputs of pollutants of concern to the Great Waters can result
in exceedances of drinking water standards and surface water quality guidance and criteria, posing
threats to human health and the environment. Recent data indicate that water quality standards in place
for drinking water supplies in the Great Waters are not being exceeded for the pollutants of concern;
however, surface water quality guidance and criteria are being exceeded in some of the Great Waters.

FINDINGS AND CONCLUSIONS

•      The pollutants of concern cause no exceedances of water quality standards in place for
       drinking water supplies in the Great Waters. Pollutant levels in both the Great Lakes and
       Lake Champlain are below primary drinking water standards and other thresholds of water
       quality. Data indicate that most of the Great Lakes nearshore waters can be used as a source of
       drinking water with normal treatment.  Similarly, Lake Champlain was not associated with any
       violations of standards in place for drinking water supplies due to Great Waters pollutants of
       concern from 1986 to  1995.  Further reductions in pollutant concentrations may reduce the cost
       of drinking water treatment in some areas.

•      Primarily because of contamination with metals and nutrients from a variety of sources,
       some of which are atmospheric, approximately 40 percent of the Nation's surveyed rivers,
       lakes, and estuaries have been found to have contaminant levels exceeding water quality
       criteria and, therefore, discourage basic uses, such as fishing and swimming. In lakes and
       rivers, nutrients and metals are the most widespread pollutants, and agriculture is the most
       common source; however, atmospheric deposition has also been identified as a source.  In
       estuaries, nutrients are the most widespread pollutants with industrial point dischargers, urban
       runoff, and storm sewers identified as the most common pollutant sources. Atmospheric
       deposition has also been identified as a significant source of nitrogen loadings, directly to the
       water surface and indirectly via runoff, to most coastal waters where measurements have been
       made.

•      While the Great Lakes generally are safe for swimming and other recreation, virtually all
       of the surveyed shoreline area shows unfavorable conditions for supporting aquatic life and
       is impacted by toxic organic chemicals that appear in fish tissue samples at much higher
       concentrations than in water samples. This is partially due to persistent toxic pollutant
       burdens, such as PCBs and PAHs, in the food web.  Several of the Great Lakes States identified
       aur pollution among other sources as contributing to impaired water quality.

RECOMMENDATIONS FOR CONTINUED AND FURTHER ACTION

•      The EPA expects to complete the development of national water quality criteria for nutrients for
       lakes, reservoirs,  rivers, streams, estuaries, and coastal waters.  This includes developing
       waterbody-specific guidance manuals  to help State and tribal agencies: (1) classify and assess
       their waters in terms of nutrient condition; (2) develop region-specific water quality standards;
       and (3) plan management responses to nutrient pollution. Where sufficient data are available,
       EPA also expects to develop specific target ranges for total nutrient loads that States can use in
       the development of their standards.
Page V-14
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                                                                                     Chapter V
                                                  Findings, Conclusions, and Recommendations
       The EPA expects to complete a pilot project to demonstrate total maximum daily load allocations
       for two waterbodies receiving mercury from atmospheric deposition. This pilot project will
       evaluate the integration of air and water program technical tools and authorities, and will
       examine emission reduction options. The EPA will also work with States that have identified
       waterbodies whose impairment may be the result of atmospheric deposition to develop tools to
       assist in establishing TMDLs that account for air sources. For example, based on the outcome
       of the pilot project, EPA will explore the possibility of providing States with modeled regional
       baseline and projected deposition estimates for several Great Waters pollutants of concern.

       The EPA, in partnership with the Chesapeake Bay watershed States, will account for nitrogen
       deposition as apart of an effort to improve water quality in the Bay and its tributaries.  The
       Chesapeake Bay partners have committed to working to integrate a cooperative, statutory
       program so that these waters could be removed from the list of impaired waters by 2010.

       The EPA, working with the Great Lakes States, will ensure implementation of the Great Lakes
       Water Quality Guidance.

       The EPA will continue to work with its Federal agency partners such as  NOAA, and with States,
       tribes, and local agencies to improve understanding of the relationship and relative contribution
       of atmospheric deposition and water pollution. The EPA expects to develop guidance to assist
       National Estuary Programs, States, tribes and local organizations, among others, to evaluate the
       role of air deposition in assessing water quality.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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Chapter V
Findings, Conclusions, and Recommendations
V.E   SUMMARY AND KEY RECOMMENDATIONS

        The EPA expects that the many ongoing and scheduled future regulatory and voluntary programs
and activities, many of which are described in this report, will further reduce the impact of air deposition
of pollutants of concern on the Great Waters. These include, but are not limited to:

•       Establishing remaining MACT and section 112(c)(6) standards for sources emitting Great Waters
        pollutants of concern;

•       Implementing EPA's strategy for the Residual Risk program, which assesses the risk remaining
        from MACT source categories (including those emitting Great Waters pollutants of concern),
        and issuing additional standards, as appropriate, within the required 8 years of the MACT
        standard being promulgated for the source category;

•       Implementing programs to control NOX, such as regional strategies to reduce NOX emissions (e.g.,
        the NOX SIP call and the rulemaking by EPA in response to States' petitions under CAA section
        126), Tier II/Gasoline sulfur rules for cars, and emission standards and guidelines for municipal
        waste combustors, as well as encouraging voluntary approaches to reduce these emissions;

•       With NOAA and other Federal agency partners, completing the strategy described in the Clean
        Water Action Plan issued in 1998,  which addresses remaining obstacles to establishing "fishable
        and swimmable waters for all Americans"; and,

•       Completing and implementing national multimedia action plans for persistent, bioaccumulative
        toxics (PBT) under the Agency's PBT Initiative.

        Development and implementation of these and other programs and initiatives  described in this
report should not require revisions to requirements, standards, and limitations pursuant to the CAA and
other Federal laws. Consequently, EPA expects that these programs should help to assure protection of
human health and the environment from atmospheric deposition to the Great Waters.  However, in order
to ensure continued progress in reducing sources and loadings of atmospheric deposition to the Great
Waters, and to further reduce the environmental and public health effects, EPA will:

•       Continue to support the maintenance and expansion of efforts to monitor Great Waters pollutants
        of concern in order to evaluate the  relative contributions of local, regional, and long-range
        transport to deposition in the U.S.,  as well as natural versus human-made sources;

•       Continue to develop and implement regulations and pollution prevention programs regionally
        and nationally, including multimedia programs, in order to reduce the release  and impact of
        sources of Great Waters pollutants of concern within the U.S.;

•       For Great Waters pollutants not emitted by U.S. sources, work within international frameworks
        to reduce sources of these pollutants;

•       Support model development and research that establish and, if possible, quantify the linkages
        from emissions to atmospheric deposition to waterbody loadings to adverse public health and the
        environmental effects of Great Waters pollutants of concern in order to enable effective risk
        management decisions;
PageV-16
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                                                                                     Chapter V
                                                  Findings, Conclusions, and Recommendations
•      Encourage and support the establishment of common baselines and measures of progress in order
       to better assess trends and health of Great Waters and other waterbodies affected by atmospheric
       deposition; and,

       Work to increase public awareness of risks of exposure to Great Waters pollutants of concern.

       The EPA is committed to continuing to address air deposition of pollutants into the Nation's
waters as a priority matter. To that end, and to assure continued coordination of the many related tasks
involved and outlined in this report, EPA will develop a detailed biennial work plan for implementation
actions beginning this year and updated every two years.  As EPA develops and implements plans,
programs and initiatives with NOAA and its other Federal, State, tribal, industry and community
partners, we expect to make significant, measurable progress toward our goal of assuring the protection
of human health and the environment from adverse effects attributable to atmospheric deposition of
pollution to the Great Waters.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
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 U.S. EPA 1998s. United States - Canada Air Quality Agreement: 1998 Progress Report.  EPA430-R-98-
 016.

 U.S. EPA.  1998t. www.epa.gov/children. October 21, 1998.

 U.S. EPA.  1998u. www.epa.gov/indian. October 22, 1998.

 U.S. EPA.  1998v. www.epa.gov/OWOW/tmdl/tmdlcstt. September 10, 1998.

 U.S. EPA 1997a. Benefits of Reducing Deposition of Atmospheric Nitrogen in Estuarine and Coastal
 Waters.

 U.S. EPA.  1997b. Deposition of Air Pollutants to the Great Waters: Second Report to Congress. Office
 of Air Quality Planning and Standards.  EPA-453/R-97-011.  June 1997.

 U.S. EPA.  1997c.  EPA Strategic Plan. U.S. Environmental Protection Agency, Office of the Chief
 Financial Officer, Washington, DC.  EPA/190-R-97-002. September 1997.

 U.S. EPA. 1997d.  Fact Sheet: The Voluntary Advanced Technology Incentives Program. EPA-821-F-
 97-012.  November 1997.

 U.S. EPA. 1997e.  Mercury Study Report to Congress (Volumes I - VIII).  Office  of Air Quality
 Planning and Standards and Office of Research and Development. EPA-452/R-97-005. December.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000          Page R-15

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References

U.S. EPA. 1997f. National Air Pollutant Emission Trends, 1900-1996. Office of Air Quality Planning
and Standards. EPA-454/R-97-011.

U.S. EPA. 1997g. National Air Quality and Emissions Trends Report, 1996. Office of Air Quality
Planning and Standards.

U.S. EPA. 1997h. Nitrogen Oxides: Impacts on Public Health and the Environment. Office of Air and
Radiation. EPA 452/R-97-002

U.S. EPA. 1997i. The Incidence and Severity of Sediment Contamination in Surface Waters of the
United States, Volume 1: National Sediment Quality Survey.  U.S. Environmental Protection Agency,
Office of Science and Technology. EPA 823-R-97-006.  September 1997.

U.S. EPA. 1997J. The Incidence and Severity of Sediment Contamination in Surface Waters of the
United States, Volume 2: Data Summaries for Areas of Probable Concern. U.S. Environmental
Protection Agency, Office of Science and Technology. EPA 823-R-97-007.  September 1997.

U.S. EPA. 1997k. The Incidence and Severity of Sediment Contamination in Surface Waters of the
United States, Volume 3: National Sediment Contaminant Point Source Inventory. U.S. Environmental
Protection Agency, Office of Science and Technology. EPA 823-R-97-008.  September 1997.

U.S. EPA. 1996a. Environmental health threats to children. EPA 175-F-96-001.  Obtained from
http://www.epa.gov/epadocs/child.htm

U.S. EPA. 1996b. TMDL Development Cost Estimates: Case Studies of 14 TMDLs.  Office of Water.
EPA-R-96-001.

U.S. EPA. 1995. Environmental Justice 1994 Annual Report: Focusing on Environmental Protection for
All People. Office of Environmental Justice. April 1995. EPA/200-R-9J-003.

U.S. EPA. 1994. Deposition of Air Pollutants to the Great Waters: First Report to Congress. Office of
Air Quality Planning and Standards. May 1994. EPA-453/R-93-055.

U.S. EPA and Environment Canada.  1998.  Draft Great Lakes Binational Toxics Strategy: Activities by
Partners. November 16,1998 draft.

Valiela, L, G. Collins, J. Kremer, K. Lajtha, M. Geist, B. Seely, J. Brawley, and C.H. Sham.  1997.
Nitrogen loading from coastal watersheds to receiving estuaries: New method and application.
Ecological Applications. 7(2):358-380.

Valiela, I, G. Collins, J. Kremer, K. Lajtha, M. Geist, B. Seely, J. Brawley, and C.H. Cham.  1996.
Nitrogen loading from coastal watershed to receiving waters: Review of methods and calculations of
loading to  Waquoit Bay. Ecol. Appl. 7: 358-380.

Valigura, R., M. Kerchner, M. Conley, J. Thomas, Michele Monti, and Bruce Hicks. 1997. Airsheds and
Watersheds II: A Shared Resources Workshop. Chesapeake Bay Program Air Subcommittee.
Annapolis, MD.
Page R-16
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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	References

VCGI. 1996.  Catalog of Digital Spatial Data for the Lake Champlain Basin. Vermont Center for
Geographic Information, Inc.  Lake Champlain Basin Program, Technical Report No. 18. September
1996.

Vitousek, P.M., J.D. Aber, R.W. Howarth, G.E. Likens, P.A. Matson, D.W. Schindler, W.H. Schlesinger,
and D.G. Tilman.  1997. Human alteration of the global nitrogen cycle:  Sources and consequences.
Ecological Applications. 7(3):737-750.

Wade, T.L., L. Chambers, P.R. Gardinali, J.L. Sericano, T.J. Jackson, R.J. Tarpley, and R. Suydam.
1997a. Toxaphene, PCB, DDT and chlordane analyses of Beluga whale blubber. Chemosphere.  34(5-
7):1351-1357.

Wade, T.L., T.J. Jackson, P.R. Gardinali, and L. Chambers.  1997b.  PCDD/PCDF sediment
concentration distribution:  Casco Bay, Maine, USA. Chemosphere.  34(5-7): 1359-1367.

Ward, M. H.,  S.D. Mark, K. P. Cantor, D.D. Weisenburger, A. Correa-Villasenor, and S. H. Zahm.  1996.
Drinking water nitrate and the risk of Non-Hodgkin's Lymphoma. Epidemiology. 7:465-471. As cited
inU.S.EPA1997f.

Watras, C. and J. Huckabee (eds).  1994. Mercury Pollution: Integration and Synthesis. Lewis
Publishers: Boca Raton.

Zarbock, P.E., A. Janicki, D. Wade, D. Higmuch, and H. Wilson. 1994.  Estimates of total nitrogen, total
phosphorous,  and total suspended solids loadings to Tampa Bay, Florida. Coastal Environment, Inc., for
the Tampa Bay Estuary Program.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page R-17

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                          INDEX OF WATERBODIES
WATERBODIES

Chesapeake Bay
        i, iii, 1-3,1-5,1-12,1-13, II-l, H-13, H-14,11-16,11-19,11-21,11-26,11-27,11-28,11-29,11-30,11-34,
        11-38,11-39,11-40,11-44,11-49,11-50,11-52,11-53,11-54,11-56,11-58,11-60,11-62,11-65,11-66,11-72,
        11-73,11-75, III-l, 111-34,111-38,111-39,111-40,111-41,111-52,111-65, IV-7, IV-11, IV-13, IV-14, IV-
        15, IV-16, IV-17, IV-18, IV-19, IV-24, V-15

Everglades
        m-5, m-53, m-54, m-ss, iv-12, iv-13

Great Lakes
        i, ii, iii, iv, 1-1,1-2,1-3,1-5,1-12,1-13, II-8, II-9,11-11,11-12,11-17, H-18,11-19,11-20,11-21,11-22,
        11-23,11-28, n-30, H-31,11-32,11-33,11-34,11-35,11-36,11-37,11-49,11-50,11-57,11-58,11-59,11-60,
        11-61,11-63,11-64,11-65,11-66,11-67,11-68,11-69,11-70,11-71,11-73,11-75, III-l, 111-31,111-34, III-
        35,111-36, HI-37, HI-49,111-60,111-66,111-67,111-68,111-69, IV-4, IV-6, IV-7, IV-9, IV-10, IV-13,
        IV-15, IV-18, IV-24, V-4, V-7, V-8, V-9, V-10, V-ll, V-12, V-14, V-15

        Lake Michigan
               1-12,11-12,11-13,11-14,11-17,11-21,11-32,11-33,11-36,11-37,11-59,11-60,11-61,11-63,11-64,
               11-65,11-66,11-67,11-69,111-34,111-35,111-36,111-37,111-64, IV-13, IV-14, IV-15, IV-16,
               IV-19, IV-22, V-4, V-9

        Lake Erie
               11-12,11-21,11-33,11-58,11-60,11-61,11-63,11-64,11-65,11-67, HI-36,111-37

        Lake Superior
               11-21, n-32,11-33,11-36,11-56,11-58,11-59,11-60,11-63,11-64,11-65,11-66,11-67,11-69, III-
               30,111-36,111-37,111-59, IV-16, IV-17

        Lake Huron
               11-31,11-33, H-36,11-59,11-60,11-63,11-64,11-66,11-67,11-69,111-36, IH-37, IV-21

        Lake Ontario
               11-12,11-19,11-33,11-32,11-56,11-60,11-61,11-63,11-64,11-65,11-66,11-67,111-36,11-37,
               IV-19, IV-21, IV-22

Gulf of Mexico
        1-5,1-13,11-34, H-55,11-56,11-57,11-71, III-l, IH-41, IH-42, IH-48, IV-9, IV-16, IV-17, IV-18

Lake Champlain
        i, 1-3,1-5,1-12, II-l, 11-11,11-14,11-15,11-49,11-50,11-57,11-69,11-73,11-75, III-l, HI-37,111-38, V-
        14

Mississippi River/Delta
        II-8,11-51,11-54,11-56,111-41,111-42, IV-17
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000        Page Index-1

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Index of Water Bodies
Neuse River
       n-54, ni-43

Peconic Bay
       n-53, m-42

St. Lawrence River
       11-17, E-28,11-60, HI-36, V-l 1

NATIONAL ESTUARY PROGRAM WATERBODIES

Albemarle-Pamlico Estuary
       1-3, n-52, n-53, n-56, m-6, m-30, m-42, m-si

Casco Bay
       1-3, m-42, IH-43

Charlotte Harbor
       m-42, m-43

Coastal Bend Bay (and Estuary)
       m-42, m-43

Delaware Inland Bays
       n-53, m-42, m-43, m-44

Delaware Estuary (or Bay)
       H-16,11-17,11-19, H-30, E-34,11-52,11-53, D-72

Galveston Bay
       1-3,11-34, H-72

Long Island Sound
       ii, 11-13,11-14, E-19, H-27,11-52,11-53,11-54,11-56,11-72, m-42, m-44, V-8

Massachusetts Bay
       H-27, H-37, H-38,11-53, m-42, m-44, IV-9

Narragansett Bay
       n-52, n-53, n-72, m-44

New York Bight
       1-3, H-52, H-53

New York/New Jersey Harbor
       n-56, m-42, m-44,111-45

San Francisco Bay (or Estuary)
       1-3, n-i, n-76, m-42, m-45
Page Index-2       Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                Index of Water Bodies
Santa Monica Bay
      1-3,111-42,111-45

Sarasota Estuary (or Bay)
      11-49,11-53, III-42,111-46

Tampa Bay
      1-3,11-49,11-53,11-56,11-70,11-72, HI-42,111-46,111-47, IH-48

NATIONAL ESTUARINE  RESEARCH RESERVE SYSTEM
WATERBODIES

Chesapeake Bay (MD and VA)
      (See above under "Waterbodies")

Delaware Inland Bays
      (See above under "Waterbodies")

Delaware Estuary (or Bay)
      (See above under "Waterbodies")

Hudson River
      HI-45

Narragansett Bay
      (See above under "Waterbodies")

Waquoit Bay
      11-51,11-52,11-53, H-55,11-56
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000       Page Index-3

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                                  APPENDIX A
                    Major Sources  of Information:
                   Publications  and  Internet Sites
PUBLICATIONS

Baker, J.E. (ed.). 1997. Atmospheric Deposition of Contaminants to the Great Lakes and Coastal
Waters.  SETAC Press.

Chesapeake Bay Program. 1999, in press. Chesapeake Bay Basin Toxics Loading and Release
Inventory.

Eisenreich, S.J., and W.M.J. Strachan.  1992. Estimating atmospheric deposition of toxic substances to
the Great Lakes - An update. Report on a workshop held at the Canada Centre for Inland Waters;
January 31-February 2, 1992; Burlington, Ontario. Sponsored by the Great Lakes Protection Fund and
Environment Canada.

Eskin, R.A., K.H. Rowland, and D.Y. Alegre. 1996.  Contaminants in Chesapeake Bay Sediments 1984-
1991. Printed by U.S. EPA for the Chesapeake Bay Program. May 1996.

Hartig, J.H., M.A. Zarull, T.B. Reynoldson, G. Mikol, V.A. Harris, R.G. Randall, and V.W. Cairns.
1997. Quantifying targets for rehabilitating degraded areas of the Great Lakes. Environ. Management
21(5):713-723.

Hoff, R.M., Strachan, W.M.J., Sweet, C.W., Chan, C.H., Shackleton, M., Bidleman, T.F., Brice, K.A.,
Burniston, D.A., Cussion, S., Gatz, D.F., Harlin, K., and W.H. Schroeder. 1996.  Atmospheric deposition
of toxic chemicals to the Great Lakes: A review of data through 1994. Atmos. Environ.  30(20):3505-
3527.

Lake Champlain Basin Program. 1998. Long-Term Water Quality and Biological Monitoring Project for
Lake Champlain, Cumulative Report for Project Years 1992-1996. Prepared by the Vermont Department
of Environmental Conservation and the New York State Department of Environmental Conservation for
the Lake Champlain Basin Program. Technical Report No. 26. March 1998.

Mackay, D. and E. Bentzen. 1997. The role of the atmosphere in Great Lakes contamination.  Atmos.
Environ. 31 (23):4045-4047.

San Francisco Estuary Institute.  1997.  1996 Annual Report: San Francisco Estuary Regional Monitoring
Program for Trace Substances.  December.

Schroeder,  W.H., and J. Munthe. 1998. Atmospheric mercury - An overview. Atmos. Environ.
32(5):809-822.

Sweet, C.W., E. Prestbo, B. Brunette. 1999. Atmospheric wet deposition of mercury in North America.
Proceedings of the 92nd Annual Meeting of the Air and Waste Management Association.  June 21-23,
1999, St. Louis, MO.
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page A-l

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Appendix A
Major Sources of Information: Publications and Internet Sites
U.SVCanada IADN Scientific Steering Committee. 1998. Technical Summary of Progress Under the
Integrated Atmospheric Depositions Program 1990-1996.

U.S. EPA. 1999. Residual Risk Report to Congress.  Office of Air Quality Planning and Standards.
EPA-453/R-99-001. March 1999.

U.S. EPA. 1998.  Condition of the Mid-Atlantic Estuaries. Office of Research and Development. EPA
600-R-98-147.

U.S. EPA. 1998.  National Air Quality and Emissions Trends Report, 1997. Office of Air Quality
Planning and Standards. EPA454/R-98-016. December 1998.

U.S. EPA. 1998. National Listing of Fish and Wildlife Advisories (NLFWA) Database-1997.  Office
ofWater. EPA-823-C-98-001.

U.S. EPA. 1998.  Study of Hazardous Air Pollutant Emissions from Electric Utility Steam Generating
Units - Final Report to Congress. February 1998. EPA 453/R-98-004a.

U.S. EPA. 1998.  The Regional NOX SIP Call and Reduced Atmospheric Deposition of Nitrogen:
Benefits to Selected Estuaries.  U.S. EPA. Washington, DC.

U.S. EPA. 1998. United States-Canada Air Quality Agreement: 1998 Progress Report. EPA430-R-98-
016.

U.S. EPA. 1997. Benefits of Reducing Deposition of Atmospheric Nitrogen in Estuarine and Coastal
Waters.

U.S. EPA. 1997. Deposition of Air Pollutants to the Great Waters: Second Report to Congress. Office
of Air Quality Planning and Standards. EPA-453/R-97-011. June 1997.

U.S. EPA. 1997. Mercury Study Report to Congress (Volumes I -  VIII). Office of Air Quality Planning
and Standards and Office of Research and Development. EPA-452/R-97-005. December 1997.

U.S. EPA. 1997. National Air Pollutant Emission Trends, 1900 - 1996. Office of Air Quality Planning
and Standards. EPA-454/R-97-011.

U.S. EPA. 1997. National Air Quality and Emissions Trends Report,  1996. Office of Air Quality
Planning and Standards.

U.S. EPA. 1997.  Nitrogen Oxides: Impacts on Public Health and the Environment. Office of Air and
Radiation. EPA 452/R-97-002.

U.S. EPA. 1994. Deposition of Air Pollutants to the Great Waters: First Report to Congress. Office of
Air Quality Planning and Standards. EPA-453/R-93-055. May 1994.

Valigura, R., M. Kerchner, M. Conley, J. Thomas, Michele Monti,  and Bruce Hicks. 1997. Airsheds and
Watersheds II: A Shared Resources Workshop.  Chesapeake Bay Program Air Subcommittee.
Annapolis, MD.
Page A-2
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                                  Appendix A
                                   Major Sources of Information: Publications and Internet Sites
 INTERNET SITES

 Chesapeake Bay Program
        http://www.chesapeakebay.net

 Commission for Environmental Cooperation
        http://www.cec.org

 Environment Canada Great Lakes Regional Programs
        http://www.cciw.ca/glimr/program.html

 Great Lakes Information Network
        http://www.great-lakes.net

 Great Lakes National Program Office
        http://www.epa.gov/ghipo

 Gulf of Mexico Program Office
        http://pelican.gmpo.gov

 Integrated Atmospheric Deposition Network - Environment Canada
        http://airquality.tor.ec.gc.ca/IADN

 Integrated Atmospheric Deposition Network - U.S. EPA
        http://www.epa.gov/grtlakes/air

 International Joint Commission
        http://www.ijc.org

 Lake Champlain Basin Program
        http://www.anr.state.vt.us/champ

 Lake Michigan Mass Balance Study (LMMBS)
        http://www.epa.gov/glnpo/hnmb

 Michigan State Mercury Pollution Prevention
        http://www.deq.state.mi.us/ead/p2sect/mercury

 National Atmospheric Deposition Program/AIRMoN
        http://nadp.sws.uiuc.edu/airmon

 National Atmospheric Deposition Program/National Trends Network (NADP/NTN)
        http://nadp.sws.uiuc.edu

National Atmospheric Deposition Program/Mercury Deposition Network (NADP/MDN)
        http://nadp.sws.uiuc.edu/mdn

National Estuarine Research Reserve System (NERRS)
        http://inlet.geol.sc.edu/nerrsintro.html
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page A-3

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Appendix A
Major Sources of Information: Publications and Internet Sites
National Estuary Program (NEP)
       http://www.epa.gov/nep

NOAA Air Resources Laboratory, AIRMoN-Dry
       http://www.arl.noaa.gov/research/projects/airrnon_dry.html

North American Agreement on Environmental Cooperation (NAAEC)
       http://www.naaec.gc.ca/english/index.html

Persistent Bioaccumulative Toxics (PBT) Initiative
       http://www.epa.gov/pbt

U.S. Environmental Protection Agency (EPA)
       http://www.epa.gov
 Page A-4
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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                                                                                      Appendix B
  Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
                                                            than 1 Percent of Total U.S. Emissions
                                      APPENDIX B
       Detailed  Breakdown  of Air  Emissions Inventory
  by Pollutant for  Source  Categories  Emitting Less than
                    1 Percent  of Total U.S.  Emissions
        This appendix lists the source categories that contribute less than 1 percent to total U.S.
emissions for mercury and compounds, lead and compounds, cadmium and compounds, dioxins and
furans, polycyclic aromatic hydrocarbons (PAHs), and polychlorinated biphenyls (PCBs). This
information is from EPA's Mercury Study Report to Congress (U.S. EPA 1997e) for mercury and
compounds and from EPA's 1993 National Toxics Inventory (NTI) for the remaining compounds (U.S.
EPA 1999a). This list is referenced in Tables II-l, II-4, II-5, II-l 1,11-14, and 11-22, in which the source
categories contributing greater than 1 percent to total U.S. emissions are listed along with the percent
contribution to total U.S. emissions.
                                MERCURY AND COMPOUNDS
Batteries
Byproduct Coke
Carbon Black
Crematories
Electrical Apparatus
Flourescent Lamp Recycling
Geothermal Power
Instruments Manufacturing
Lime Manufacturing
Mercury Compounds
Abrasive Products
Adhesives and Sealants
Aerospace Industry (Surface Coating)
Agricultural Production
Agricultural Chemicals and Pesticides
Air and Gas Compressors
Air, Water, & Solid Waste Management
Aircraft Engines and Engine Parts Manufacturing
Aircraft Manufacturing
Aircraft Parts and Equipment Manufacturing
Aircraft And Parts
Airports, Flying Fields, & Services
Aluminum Extruded Products
Aluminum Foundries
Aluminum Foundries (Castings)
Aluminum Sheet, Plate, and Foil manufacturing
Aluminum Die-Castings
Ammunition, Except for Small Arms
Amusement Parks
Amusement And Recreation, Nee
Animal Cremation
Asphalt Paving Production
Asphalt Paving Mixtures And Blocks
Asphalt Production
Asphalt Roofing Production
                                                     Pigments, Oil, etc.
                                                     Primary Copper
                                                     Primary Lead
                                                     Primary Mercury Production
                                                     Refineries
                                                     Secondary Mercury Production
                                                     Sewage Sludge Incinerators
                                                     Turf Products
                                                     Wood-fired Boilers
                                   LEAD AND COMPOUNDS
                                                     Automotive stampings
                                                     Automotive Dealers, Nee
                                                     Aviation Gasoline Distribution: Stage I & II
                                                     Beet Sugar
                                                     Black Liquor Combustion
                                                     Blast Furnaces and Steel Mills
                                                     Boat Building and Repairing
                                                     Bolts, Nuts, Rivets and Washers Manufacturing
                                                     Bookbinding And Related Work
                                                     Botanical And Zoological Gardens
                                                     Brass, Bronze, Copper, Copper Base Alloy Foundries
                                                     Bread, Cake, And Related Products
                                                     Brick and Structural Clay Tile
                                                     Business services, nee (1987)
                                                     Canned specialties
                                                     Canned Fruits and Vegetables
                                                     Carbon and Graphite Products
                                                     Carbon Black Manufacture
                                                     Carburetors, Pistons, Rings and Valves Manufacturing
                                                     Cathode Ray Television Picture Tubes Manufacturing
                                                     Cement, Hydraulic (not subject to Portland Cement Regulation)
                                                     Ceramic Wall and Floor Tile Manufacturing
                                                     Chemical Manufacturing: Explosives & Blasting Agents
Deposition of Air Pollutants to the Great Waters - 3  Report to Congress 2000
                                                                                         Page B-l

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Appendix B
Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
than 1 Percent of Total U.S. Emissions
                                  LEAD AND COMPOUNDS (CONTINUED)
Chemical Preparations
Chemical Manufacturing: Cyclic Crude and Intermediate
Production
Chemicals and Allied Products Manufacturing
Chromium Plating: Chromic Anodizing Plating
Coated Fabrics, not Rubberized, Manufacturing
Coke Ovens: By-product Recovery Plants
Cold Finishing of Steel Shapes
Commercial Printing, Lithographic
Commercial Printing, nee
Commercial Physical Research
Commercial/Institutional Boilers:  Coal Combustion, all types
Commercial/Institutional Heating: Anthracite Coal Combustion
Commercial/Institutional Heating: Bituminous and Lignite Coal
Combustion
Commercial/Institutional Heating: Distillate Oil Combustion
Commercial/Institutional Heating: Natural Gas Combustion
Commercial/Institutional Heating: Residual Oil Combustion
Commercial/Institutional Heating: Wood/Wood Residue
Combustion
Communications Equipment, nee
Computer Peripheral Equipment, nee
Construction Machinery Manufacturing
Construction (SICs 15-17)
Construction Sand And Gravel
Conveyors and Conveying Equipment Manufacturing
Copper Rolling and Drawing
Copper Foundries
Cordage and Twine
Correctional  Institutions
Costume Jewelry
Cotton
Cottonseed Oil Mills
Courts
Crop Preparation Services For Market
Crude petroleum and natural gas
Crude Petroleum Pipelines
Crushed And Broken Limestone
Crushed And Broken Stone, Nee
Crushed And Broken Granite
Current-carrying Wiring Devices
Custom Compound Purchased Resins Manufacturing
Dehydrated fruits, vegetables, and soups
Depository Institutions
Dog and Cat Food
Drum and Barrel Reclamation
Durable Goods, Nee
Electric and other services combined
Electric Lamps
Electric services
Electrical Equipment and Supplies, nee
Electrical Industrial Apparatus, nee
Electrical Apparatus and Equipment
Electromedical Equipment Manufacturing
Electrometallurgical Products
Electron Tubes Manufacturing
Electronic Components, nee
Electronic Computers
Electronic Computing Equipment
Electronic Connectors
Electronic Capacitors Manufacturing
Electronic Resistors
Elevators and Moving Stairways Manufacturing
Engine Electric Equipment
                                       Engineering Services
                                       Environmental Controls Manufacturing
                                       Fabricated Metal Products, nee
                                       Fabricated Plate Work (Boiler Shops)
                                       Fabricated Rubber Products, nee
                                       Fabricated Structural Metal Manufacturing
                                       Fabricated Structural Metal Products
                                       Farm Machinery and Equipment Manufacturing
                                       Ferroalloy Ores, Except Vanadium
                                       Fertilizers, Mixing only
                                       Flat Glass
                                       Fluid power Valves and Hose Fittings Manufacturing
                                       Fluid Meters and Counting Devices
                                       Food and Agricultural Products: Cotton Ginning
                                       Food Preparations Production
                                       Food Products Machinery Manufacturing
                                       Frozen fruits, fruit juices and vegetables
                                       Funeral Service And Crematories
                                       Furniture and Fixtures Manufacturing
                                       Gas And Other Services Combined
                                       Gaskets, Packing and Sealing Devices Manufacturing
                                       Gasoline Distribution Stage II
                                       Gasoline Distribution Stage I
                                       General Industrial Machinery Manufacturing
                                       General Automotive Repair Shops
                                       General Medical & Surgical Hospitals
                                       Glass Containers
                                       Gold Ores
                                       Grain And Field Beans
                                       Gray and Ductile Iron Foundries
                                       Greeting Cards
                                       Grocery Stores
                                       Guided Missiles and  Space Vehicles Manufacturing
                                       Halogenated Solvent Cleaners
                                       Hand and Edge Tools Manufacturing
                                       Hardware Manufacturing
                                       Heating Equipment, Except Electric
                                       Heavy Construction, Nee
                                       Hospitals
                                       Hotels And Motels
                                       Household Cooking Equipment
                                       Household Audio and Video Equipment
                                       Hunting, Trapping, Game Propagation
                                       Industrial Boilers:  Residual Oil Combustion
                                       Industrial Boilers: Bituminous and Lignite Coal Combustion
                                       Industrial Boilers:  Coal, all types
                                       Industrial Boilers:  Distillate Oil Combustion
                                       Industrial Boilers: Natural Gas Combustion
                                       Industrial Boilers: Anthracite Coal Combustion
                                       Industrial Boilers:  Waste Oil Combustion
                                       Industrial Boilers:  Wood/Wood Residue Combustion
                                       Industrial Gases Manufacturing
                                       Industrial Inorganic Chemical Manufacturing
                                       Industrial machinery and equipment
                                       Industrial Organic Chemicals Manufacturing
                                       Industrial Sand
                                       Industrial Supplies
                                       Industrial Trucks and Tractors Manufacturing
                                       Industrial/Utility Dist. Oil/Diesel Turbines
                                       Inorganic Pigments Manufacturing
                                       Instruments to Measure Electricity
                                       Integrated Iron and Steel Mills
Page B-2
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

-------
                                                                                                           Appendix B
  Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
                                                                          than 1 Percent of Total U.S. Emissions
                                  LEAD AND COMPOUNDS (CONTINUED)
Intercity & Rural Bus Transportation
Internal Combustion Engine Manufacturing
Iron and Steel Foundries: Steel Foundries
Iron and Steel Foundries: Steel Investment Foundries
Iron and Steel Forging
Laminated Plastics Plate and Sheet
Lead Pencils, Art Goods Manufacturing
Life Insurance
Lighting Equipment
Lightweight Aggregate Kilns
Lime
Lubricating Oils and Greases
Malleable Iron Foundries
Malt Beverages
Manufacturing Industries Manufacturing
Marine Cargo Handling
Measuring and Controlling Devices, nee
Meat Packing Plants
Membership Sports & Recreation Clubs
Metal cans (3411)
Metal coating and allied services (3479)
Metal Coil (Surface Coating)
Metal Barrels, Drums, and Pails Manufacturing
Metal Foil and Leaf
Metal Forgings and Stampings
Metal Heat Treating Manufacturing
Metal Sanitary Ware Manufacturing
Metal Stampings Manufacturing
Metal Valves
Mineral Wool Manufacturing (includes Wool Fiberglass)
Mineral Wool
Minerals, Ground or Treated Production
Mining Machinery Manufacturing
Miscellaneous Plastics Products
Miscellaneous Fabricated Wire Products
Miscellaneous Metal Work
Miscellaneous Nonmetallic Minerals
Miscellaneous Fabricated Metal Products
Miscellaneous Plastics Products, nee
Mobile Sources: Railroads
Mobile Sources: Non-Road Vehicles and Equipment -
Commercial Marine Vessels
MON - Continuous Processes
Motion Picture & Video Production
Motor Vehicle Equipment
Motor Vehicle Parts and Accessories Manufacturing
Motor Vehicles and Car Bodies Manufacturing
Motor and Generators Manufacturing
Musical Instruments
National Security
Natural Gas Liquids
Newspapers
Non-road Mobile Vehicles
Noncommercial research organizations (1987)
Noncurrent-Carrying Wiring Devices
Nonferrous Foundries, nee
Nonferrous Rolling and Drawing
Nonferrous Wire Drawing and Insulating
Nonferrous Forgings
Nonferrous Die-castings, Except Aluminum
Nonmetallic Mineral Products Manufacturing
Nursing And Personal Care, Nee
Office Machines
Office Furniture, Except Wood Manufacturing
Oil And Gas Field Services, Nee
Oil and Gas Field Machinery Manufacturing
On-Site Waste Incineration
Open Burning: Forest and Wildfires
Open Burning:  Scrap Tires
Ophthalmic Goods
Optical Instruments and Lenses
Ordnance and Accessories Manufacturing
Organic Fibers, Non-cellulosic Manufacturing
Ornamental Nursery Products
Other Structural Clay Products
Paint Application:  Medium Shops
Paint Application:  Large Shops
Paints and Allied Products Manufacturing
Paper Coated and Laminated, Packaging, nee
Paperboard Mills
Paved Road Dust
Petroleum Refining
Petroleum Refining
Petroleum Refining: Catalytic Cracking Units
Petroleum Refining: Other Petroleum Products
Petroleum Bulk Stations and Terminals
Pharmaceutical Preparations Manufacturing
Phosphatic Fertilizers
Plastics Materials and Resins Manufacturing
Plastics Products Manufacturing
Plastics Foam Products Manufacturing
Plumbing Fixture Fittings and Trim
Porcelain Electrical Supplies
Portland Cement Manufacture: All Fuels
Potash, Soda, And Borate Minerals
Potato Chips and Similar Snacks
Pottery Products, nee
Power Transmission Equipment
Prefabricated Metal Buildings
Prepared Feeds Manufacturing
Primary Aluminum Production
Primary Batteries, Dry and Wet, Manufacturing
Primary Copper
Primary Metal Products Manufacturing
Primary Smelting and Refining of Zinc
Printing Ink
Printing Trades Machinery Manufacturing
Products of Purchased Glass
Pulp mills (2611)
Pulp and Paper: Kraft Recovery Furnaces
Pumps and Pumping Equipment Manufacturing
Radio and Television Communications Equipment (3662)
Radio and Television Communications Equipment (3663)
Railroad Equipment Manufacturing
Railroads, Line-haul Operating
Ready-mixed Concrete
Refrigeration and Heating Equipment Manufacturing
Refuse Systems
Relays and Industrial Controls
Repair services, nee
Residential Bituminous and Lignite Coal Combustion
Residential Care
Residential Distillate Oil Combustion
Residential Anthracite Coal Combustion
Residential Wood/Wood Residue  Combustion
Rice Milling
Rubber and Plastic Hose and Belting Manufacturing
Sawmills and Planing Mills, general
Deposition of Air Pollutants to the Great Waters - 3   Report to Congress 2000
                                             Page B-3

-------
Appendix B
Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
than 1 Percent of Total U.S. Emissions
                                  LEAD AND COMPOUNDS (CONTINUED)
 Schools & Educational Services, Nee
 Scrap And Waste Materials
 Screw Machine Products, Bolts, etc.
 Screw Machine Products Manufacturing
 Search and Navigation Equipment
 Secondary Aluminum Smelting
 Semiconductors and Related Devices
 Scmivitreous Table & Kitchenware
 Service Industry Machinery
 Sewage Sludge Incineration
 Sewerage Systems
 Sheet Metal Work
 Ship Building & Repair
 Ship Building And Repairing
 Signs and Advertising Displays
 Silverware and Plated Ware
 Skilled Nursing Care Facilities
 Small Arms Ammunition
 Small Arms
 Soap and Other Detergents Manufacturing
 Soil Dust
 Space Research and Technology
 Space Vehicle Parts and Equipment, nee
 Space Propulsion Units and Parts Manufacturing
 Special Dies, Tools, Jigs and Fixtures
 Special Industry Machinery, nee
 Special Trade Contractors, nee
 Specialty Hospitals Exc. Psychiatric
 Speed Changers, Drives, and Gears
 Sporting and Athletic Goods Manufacturing
 Stainless Steel Manufacture - EAF
 Stationary 1C Engines - Diesel
 Stationary 1C Engines - Natural Gas
 Steam And Air-conditioning Supply
 Steel Pipe and Tubes Manufacturing
                                        Structural Clay Products, nee
                                        Structure Fires
                                        Surface Active Agents Manufacturing
                                        Surface Coating Operations
                                        Surgical and Medical Instruments Manufacturing
                                        Taconite Iron Ore Processing
                                        Telephone and Telegraph Apparatus
                                        Textile Machinery
                                        Tire Cord and Fabric
                                        Tire Manufacturing
                                        Tires and Inner Tubes
                                        Top & body repair and paint shops (1987)
                                        Transformers, Except Electronic
                                        Travel Trailers and Campers Manufacturing
                                        Truck Trailers
                                        Truck and Bus Bodies
                                        Trucking, Except Local
                                        Turbines and Turbine Generator Sets
                                        Turbines - Natural Gas
                                        U.S. Postal Service
                                        Unpaved Road Dust
                                        Unsupported Plastics Profile Shapes
                                        Unsupported Plastics Film & Sheet
                                        Utility Boilers:  Coke
                                        Utility Boilers:  Natural Gas Combustion
                                        Utility Boilers:  Oil Combustion, all types
                                        Valves and Pipe Fittings Manufacturing
                                        Vehicular Lighting Equipment
                                        Vitreous Plumbing Fixtures
                                        Vitreous China Table and Kitchenware
                                        Waste Disposal: Open Burning (all categories)
                                        Water supply
                                        Wood Products
                                        Wool Fiberglass Manufacturing
                                        X-ray Apparatus and Tubes
                                         CADMIUM AND COMPOUNDS
Adhesives and Sealants
Aerospace Industry (Surface Coating)
Agricultural Production
Air, Water, & Solid Waste Management
Aircraft Manufacturing
Aircraft Parts and Equipment Manufacturing
Aircraft And Parts
Airports, Flying Fields, & Services
Aluminum Extruded Products
Aluminum Foundries
Aluminum Foundries (Castings)
Aluminum Die-Castings
Ammunition, Except for Small Arms
Amusement Parks
Animal Cremation
Asphalt Production
Asphalt Roofing Production
Asphalt Paving Mixtures And Blocks
Automotive stampings
Ball and Roller Bearings Manufacturing
Beet Sugar
Black Liquor Combustion
Blast Furnaces and Steel Mills
Boat Building and Repairing
Bolts, Nuts, Rivets and Washers Manufacturing
Brick and Structural Clay Tile
                                        Cadmium Stabilizers for Plastics
                                        Canned specialties
                                        Canned Fruits and Vegetables
                                        Carbon Black Manufacture
                                        Cement, Hydraulic (not subject to Portland Cement Regulation)
                                        Chemical Preparations
                                        Chemical Manufacturing:  Cyclic Crude and Intermediate
                                        Production
                                        Chromium Plating: Chromic Anodizing Plating
                                        Chromium Metal Plating
                                        Coated Fabrics, not Rubberized, Manufacturing
                                        Commercial Physical Research
                                        Commercial Printing, Letterpress, and Screen
                                        Commercial Printing, Lithographic
                                        Commercial Printing, nee
                                        Commercial/Institutional Boilers: Coal Combustion, all types
                                        Commercial/Institutional Heating: Anthracite Coal Combustion
                                        Commercial/Institutional Heating: Bituminous and Lignite Coal
                                        Combustion
                                        Commercial/Institutional Heating: Distillate Oil Combustion
                                        Commercial/Institutional Heating: Natural Gas Combustion
                                        Commercial/Institutional Heating: Residual Oil Combustion
                                        Commercial/Institutional Heating: Wood/Wood Residue
                                         Combustion
Page B-4
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

-------
                                                                                                           Appendix B
  Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
                                                                          than 1 Percent of Total U.S. Emissions
                              CADMIUM AND COMPOUNDS (CONTINUED)
Confectionery
Construction Machinery Manufacturing
Construction Sand And Gravel
Construction (SICs 15-17)
Copper Rolling and Drawing
Correctional Institutions
Cotton
Cottonseed Oil Mills
Courts
Crop Services
Crop Preparation Services For Market
Crude petroleum and natural gas
Crude Petroleum Pipelines
Crushed And Broken Limestone
Crushed And Broken Stone, Nee
Crushed And Broken Granite
Custom Compound Purchased Resins Manufacturing
Dehydrated fruits, vegetables, and soups
Depository Institutions
Durable Goods, Nee
Electric and other services combined
Electric services
Electron Tubes Manufacturing
Electronic Computers
Electronic Connectors
Electronic Components, nee
Engine Electric Equipment
Engineering Services
Environmental Controls Manufacturing
Fabricated Structural Metal Manufacturing
Fabricated Metal Products, nee
Ferroalloy Ores, Except Vanadium
Flat Glass
Flour and other grain mill products
Fluid power Valves and Hose Fittings Manufacturing
Food and Agricultural Products:  Cotton Ginning
Frozen fruits, fruit juices and vegetables
Funeral Service And Crematories
Gas And Other Services Combined
General Medical & Surgical Hospitals
Glass Containers
Gold Ores
Gray and Ductile Iron  Foundries
Grocery Stores
Guided Missiles and Space Vehicles Manufacturing
Halogenated Solvent Cleaners
Hardware Manufacturing
Heating Equipment, Except Electric
Heavy Construction, Nee
Hospitals
Hotels And Motels
Household Cooking Equipment
Human Cremation
Hydrochloric Acid Production
Industrial Boilers:  Bituminous and Lignite Coal Combustion
Industrial Boilers:  Anthracite Coal Combustion
Industrial Boilers:  Coal, all types
Industrial Boilers:  Distillate Oil Combustion
Industrial Boilers:  Natural Gas Combustion
Industrial Boilers:  Residual Oil Combustion
Industrial Boilers:  Waste Oil Combustion
Industrial Boilers:  Wood/Wood Residue Combustion
Industrial machinery and equipment
Industrial Machinery,  nee
Industrial Organic Chemicals Manufacturing
Industrial Sand
Industrial/Utility Dist. Oil/Diesel Turbines
Inorganic Pigments Manufacturing (Cadmium only)
Instruments to Measure Electricity
Intercity & Rural Bus Transportation
Internal Combustion Engine Manufacturing
Iron and Steel Foundries: Steel Foundries
Iron and Steel Forging
Lead Pencils, Art Goods Manufacturing
Life Insurance
Lighting Equipment
Lightweight Aggregate Kilns
Lime
Lubricating Oils and Greases
Malt Beverages
Manufacturing Industries Manufacturing
Marine Cargo Handling
Metal coating and allied services (3479)
Metal Heat Treating Manufacturing
Metal Sanitary Ware Manufacturing
Metal cans (3411)
Mineral Wool
Mineral Wool Manufacturing (includes Wool Fiberglass)
Minerals, Ground or Treated Production
Miscellaneous Nonmetallic Minerals
Miscellaneous Metal Work
Mobile Sources: On- Road Vehicles
Mobile Sources: Non-Road Vehicles and Equipment -
Commercial Marine Vessels
MON - Continuous Processes
Motion Picture & Video Production
Motor and Generators Manufacturing
Motor Vehicle Parts and Accessories Manufacturing
National Security
Natural Gas Liquids
Non-road Mobile Vehicles
Non-stainless Steel Manufacture - EAF
Noncommercial research organizations (1987)
Nonferrous Wire Drawing and Insulating
Nonferrous Rolling and Drawing
Nonferrous Foundries, nee
Nonmetallic Mineral Products Manufacturing
Nursing And Personal Care, Nee
Oil And Gas Field Services, Nee
On-Site Waste Incineration
Ordnance and Accessories Manufacturing
Ornamental Nursery Products
Other Cadmium Compound Production
Other Structural Clay Products
Paints and Allied Products Manufacturing
Paved Road Dust
Petroleum Refining
Petroleum Bulk Stations and Terminals
Petroleum Refining
Petroleum Refining: Other Petroleum Products
Pharmaceutical Preparations Manufacturing
Plastics Materials and Resins Manufacturing
Plastics Products Manufacturing
Plastics Foam Products Manufacturing
Portland Cement Manufacture:  All Fuels
Prepackaged Software
Prepared Feeds Manufacturing
Pressed and Blown Glass and Glassware Manufacturing
 Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
                                              Page B-5

-------
 Appendix B
 Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
 than 1 Percent of Total U.S. Emissions	

                               CADMIUM AND COMPOUNDS (CONTINUED)
 Primary Copper
 Primary Batteries, Dry and Wet, Manufacturing
 Primary Metal Products Manufacturing
 Puip mills (2611)
 Pulp and Paper:  Kraft Recovery Furnaces
 Radio and Television Communications Equipment (3663)
 Railroads, Line-haul Operating
 Raw cane sugar
 Ready-mixed Concrete
 Refrigeration and Heating Equipment Manufacturing
 Refuse Systems
 Repair services, nee
 Residential Bituminous and Lignite Coal Combustion
 Residential Care
 Residential Distillate Oil Combustion
 Residential lighting fixtures
 Residential Anthracite Coal Combustion
 Residential Wood/Wood Residue Combustion
 Rice Milling
 Sawmills and Planing Mills, general
 Schools & Educational Services, Nee
 Scrap And Waste Materials
 Screw Machine Products, Bolts, etc.
 Search and Navigation Equipment
 Secondary Aluminum Smelting
 Secondary Nonferrous Metals Production
 Secondary Zinc Production
 Semiconductors and Related Devices
 Service Industry Machinery
 Sewerage Systems
 Sheet Metal Work
                                        Ship Building And Repairing
                                        Skilled Nursing Care Facilities
                                        Soap and Other Detergents Manufacturing
                                        Soil Dust
                                        Space Research and Technology
                                        Space Propulsion Units and Parts Manufacturing
                                        Specialty Hospitals Exc. Psychiatric
                                        Stainless Steel Manufacture - EAF
                                        Stationary 1C Engines - Diesel
                                        Stationary 1C Engines - Natural Gas
                                        Steam And Air-conditioning Supply
                                        Storage Batteries Manufacturing
                                        Structural Clay Products, nee
                                        Telephone and Telegraph Apparatus
                                        Tire Manufacturing
                                        Tires and Inner Tubes
                                        Top & body repair and paint shops (1987)
                                        Travel Trailers and Campers Manufacturing
                                        Trucking, Except Local
                                        Turbines and Turbine Generator Sets
                                        Turbines - Natural Gas
                                        Unpaved Road Dust
                                        Unsupported Plastics Film & Sheet
                                        Utility Boilers: Coal Combustion, all types
                                        Utility Boilers: Coke
                                        Utility Boilers: Natural Gas Combustion
                                        Utility Boilers: Oil Combustion, all types
                                        Valves and Pipe Fittings Manufacturing
                                        Water supply
                                        Wood Products
                     DIOXINS AND FURANS (MEASURED AS 2,3,7,8-TCDD TEQ)
Carbon Reactivation Furnaces
Commercial/Institutional Heating: Anthracite Coal Combustion
Commercial/Institutional Heating: Bituminous and Lignite Coal
Combustion
Commercial/Institutional Heating: Wood/Wood Residue
Combustion
Drum and Barrel Reclamation
Hazardous Waste Incineration
Industrial Boilers: Anthracite Coal Combustion
Industrial Boilers: Bituminous and Lignite Coal Combustion
                                       Lightweight Aggregate Kilns
                                       Portland Cement Manufacture: Hazardous Waste-fired
                                       Pulp and Paper: Kraft Recovery Furnaces
                                       Residential Bituminous and Lignite Coal Combustion
                                       Residential Anthracite Coal Combustion
                                       Scrap Tire Combustion
                                       Secondary Copper Smelting
                                       Secondary Lead Smelting
                                       Sewage Sludge Incineration
                                       Utility Boilers: Coke
             POLYCYCLIC AROMATIC HYDROCARBONS (MEASURED AS 16-PAH)
Abrasive Products
Adhesives and Sealants
Agricultural Chemicals and Pesticides
Aircraft Parts and Equipment Manufacturing
Aircraft Manufacturing
Aluminum Extruded Products
Aluminum Foundries
Aluminum Sheet, Plate, and Foil manufacturing
Animal Cremation
Asphalt Felts And Coatings
Asphalt Paving Production
Blast Furnaces and Steel Mills
Carbamatc Insecticides Production
Carbon and Graphite Products
Cement, Hydraulic (not subject to Portland Cement Regulation)
                                       Chemical Manufacturing: Naphthalene
                                       Chemical Manufacturing: Alkalies and Chlorine
                                       Chemical Manufacturing: Cyclic Crude and Intermediate
                                       Production
                                       Chemical Manufacturing: Naphthalene Sulfonates
                                       Chemical Preparations
                                       Cigarette Smoke
                                       Clay Refractories
                                       Coke Ovens: By-product Recovery Plants
                                       Cold Finishing of Steel Shapes
                                       Commercial/Institutional Heating: POTW Digester Gas
                                       Combustion
                                       Commercial Physical Research
                                       Commercial Printing, Gravure
                                       Commercial Printing, Letterpress, and Screen
Page B-6
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

-------
                                                                                                          Appendix B
  Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
                                                                         than 1 Percent of Total U.S. Emissions
   POLYCYCLIC AROMATIC HYDROCARBONS (MEASURED AS 16-PAH) (CONTINUED)
Commercial/Institutional Heating: Anthracite Coal Combustion
Commercial/Institutional Heating: Bituminous and Lignite Coal
Combustion
Commercial/Institutional Heating: Distillate Oil Combustion
Commercial/Institutional Heating: Natural Gas Combustion
Commercial/Institutional Heating: Residual Oil Combustion
Commercial/Institutional Heating: Wood/Wood Residue
Combustion
Construction Machinery Manufacturing
Drum and Barrel Reclamation
Fabric Dress and Work Gloves
Fabricated Plate Work (Boiler Shops)
Fabricated Metal Products, nee
Fabricated Rubber Products, nee
Fabricated Structural Metal Manufacturing
Ferroalloy Manufacture
Fiber Cans, Drums, and Similar Products
Gray and Ductile Iron Foundries
Gum and Wood Chemical Manufacturing
Hard Surface Floor Coverings Manufacturing
Household Cooking Equipment
Household Appliances Manufacturing
Human Cremation
Hydrochloric Acid Production
Industrial Boilers: Waste Oil Combustion
Industrial Boilers: Anthracite Coal Combustion
Industrial Boilers: Bituminous and Lignite Coal Combustion
Industrial Boilers: Distillate Oil Combustion
Industrial Boilers: Natural Gas Combustion
Industrial Boilers: Residual Oil Combustion
Industrial Boilers: Wood/Wood Residue Combustion
Industrial Gases Manufacturing
Industrial Inorganic Chemical Manufacturing
Integrated Iron and Steel Mills
Internal Combustion Engine Manufacturing
Landfills: Gas Flares
Lubricating Oils and Greases
Manufacturing Industries Manufacturing
Meat Packing Plants
Medical Waste Incineration
Medicinals and Botanicals Manufacturing
Metal Barrels, Drums, and Pails Manufacturing
Metal Coil (Surface Coating)
Metal Doors, Sash, and Trim
Metal Household Furniture
Miscellaneous Plastics Products
Miscellaneous Chemical Products (2890)
Mobile  Sources: Non-Road Vehicles and Equipment - Aircraft
Mobile  Sources: Non-Road Vehicles and Equipment -
Commercial Marine Vessels
Mobile  Sources: Non-Road Vehicles and Equipment - Other
Mobile  Sources: On- Road Vehicles
Motor Vehicle Equipment
Motor Vehicles and Car Bodies Manufacturing
Municipal Waste Combustion
Naphthalene: Miscellaneous Uses
Needles, Pins, Hooks and Eyes and Similar Notions
Non-stainless Steel Manufacture - EAF
Nonferrous Wire Drawing and Insulating
Nonmetallic Mineral Products Manufacturing
Office Furniture, Except Wood Manufacturing
Oil and Gas Field Machinery Manufacturing
Other Structural Clay Products
Paints and Allied Products Manufacturing
Paper Coated and Laminated, Packaging, nee
Paper Mills
Partitions and Fixtures, Except Wood
Petroleum Bulk Stations and Terminals
Petroleum Refining
Pharmaceutical Preparations Manufacturing
Phthalic Anhydride Production
Plastics Materials and Resins Manufacturing
Plastics Foam Products Manufacturing
Polishes and Sanitation Goods Manufacturing
Potato Chips and Similar Snacks
Primary Nonferrous Metals Production
Public Building and Related Furniture
Publicly Owned Treatment Works (POTWs)
Refrigeration and Heating Equipment Manufacturing
Residential Anthracite Coal Combustion
Residential Bituminous  and Lignite Coal Combustion
Residential Distillate Oil Combustion
Residential Natural Gas Combustion
Residential Wood/Wood Residue Combustion
Scrap Tire Combustion
Secondary Lead Smelting
Sewage Sludge Incineration
Sheet Metal Work
Ship Building & Repair
Soap and Other Detergents Manufacturing
Sporting and Athletic Goods Manufacturing
Stainless Steel Manufacture - EAF
Stationary 1C Engines -  Diesel
Stationary 1C Engines -  Natural Gas
Surface Active Agents Manufacturing
Tire Manufacturing
Transformers, Except Electronic
Truck and Bus Bodies
Turbines - Natural Gas
Utility Boilers: Coke
Utility Boilers: Coal Combustion, all types
Utility Boilers: Natural Gas Combustion
Utility Boilers: Oil  Combustion, all types
Wood Household Furniture Manufacturing
Wood Treatment/Wood Preserving
Yarn Spinning Mills
 Deposition of Air Pollutants to the Great Waters - 3   Report to Congress 2000
                                              Page B-7

-------
 Appendix B
 Detailed Breakdown of Air Emissions Inventory by Pollutant for Source Categories Emitting Less
 than 1 Percent of Total U.S. Emissions	

                                POLYCHLORINATED BIPHENYLS
 Adhcsives and Sealants
 Air, Water, & Solid Waste Management
 Animal Cremation
 Commercial Printing, Lithographic
 Electric services
 Industrial Boilers: Wood/Wood Residue Combustion
                                  Landfills: Gas Flares
                                  Minerals, Ground or Treated Production
                                  Petroleum Refining
                                  Secondary Nonferrous Metals Production
                                   Services, Nee
Page B-8
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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a Major tributary rivers to the Che
"Multiple pollutants (unspecified]
c Specific embayments of Puget
tetrachloroethylene, arsenic, mel
d Other unspecified pesticides.
Note: Shading is used in rows to
Source: U.S. EPA 1998m (Advis.

-------
                     APPENDIX D
     Names of Numbered Sites from Figure 11-17:
    Locations of Watersheds Designated as Areas of
                   Probable Concern
Map#
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25
26
27
28
Watershed Name
Charles
Cape Cod
Narragansett
Hackensack-Passaic
Sandy Hook-Staten Island
Raritan
Southern Long Island
Middle Delaware-Musconetcong
Lower Delaware
Schuylkill
Mullica-Toms
Gunpowder-Patapsco
Conococheague-Opequon
Lower Pee Dee
Seneca
Middle Savannah
Lower St. Johns
Middle Chattahoochee-Lake Harding
Choctawhatchee Bay
Perdido Bay
Mobile Bay
Door-Kewaunee
Menominee
Lower Fox
Little Calumet-Galien
Pike-Root
Milwaukee
St. Joseph
Map#
49
50
51
52
53
54
55
56
57
58
59
60
61
62
63
64
65
66
67
68
69
70
71
72
73
74
75
76
Watershed Name
Watts Bar Lake
Lower Clinch
Middle Tennessee-Chickamauga
Hiwassee
Guntersville Lake
Pickwick Lake
Lower Tennessee-Beech
Kentucky Lake
Twin Cities
Rush-Vermillion
Buffalo-Whitewater
Castle Rock
Copperas-Duck
Kishwaukee
Chicago
Des Plaines
Upper Fox
Lower Illinois-Senachwine Lake
Cahokia-Joachim
Big Muddy
Upper Kaskaskia
Middle Kaskaskia
Lower Mississippi-Memphis
Deer-Steele
Lower Ouachita
Lower Calcasieu
Lower Mississippi-New Orleans
Lower Kansas
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000
Page D-l

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Appendix D
Names of Numbered Sites from Figure 11-16:
Locations of Watershed Designated as Areas of Probable Concern
Map#
29
30
31
32
33
34
35
36
37
38
39
40
41
42
43
44
45
46
47
48
Watershed Name
Manistee
Lake St. Glair
Detroit
Ottawa-Stony
Raisin
Cedar-Portage
Huron-Vermillion
Black-Rocky
Ashtabula-Chagrin
Chautauqua-Conneaut
Buffalo-Eighteenmile
Niagara
Oak Orchard-Twelvemile
Upper St. Lawrence
Upper Ohio
Shenango
Tuscarawas
Vermilion
Middle Wabash-Busseron
Holston
Map#
77
78
79
80
81
82
83
84
85
86
87
88
89
90
91
92
93
94
95
96
Watershed Name
Spring
Lower Neosho
Buffalo-San Jacinto
Coeur D'Alene Lake
Lower Yakima
Lower Willamette
Strait of Georgia
Duwamish
Puyallup
Puget Sound
Tulare-Buena Vista Lakes
Coyote
San Francisco Bay
Santa Monica Bay
Los Angeles
San Pedro Channel Islands
Seal Beach
Newport Bay
Aliso-San Onofre
San Diego
Source: U.S. EPA 1997i
Page D-2
Deposition of Air Pollutants to the Great Waters - 3rd Report to Congress 2000

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