Annual Report
To the President and Congress
N A P A P
NATIONAL ACID PRECIPITATION ASSESSMENT PROGRAM
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Interagency Task Force on Acid Precipitation
Joint Chairs Council:
Mr. Lee M. Thomas (Chair)
Dr. Orville G. Bentley
Miss Donna Fitzpatrick
Mr. A. Alan Hill
Mr. T Ary
Dr. William E. Evans
Environmental Protection Agency
Department of Agriculture
Department of Energy
Council on Environmental Quality
Department of the Interior
Department of Commerce
Other Agency Task Force Members:
Dr. Billy J. Bond
Mr. John F. Fitzgerald
Dr. David T. Kingsbury
Dr. Ralph R. Reed
Dr. Shelby Tilford
Tennessee Valley Authority
Department of State
National Science Foundation
Department of Health and Human Services
National Aeronautics and Space Administration
Presidential Appointees:
Ms. Kathleen M. Bennett
Dr. Walter R. Eckelmann
Dr. Ralph M. Perhac
James River Corporation
RCB Company
Electric Power Research Institute
National Laboratory Representatives:
Dr. Jeremy M. Hales
Dr. Bernard Manowitz
Dr. Chester R. Richmond
Dr. Jack D. Shannon
Pacific Northwest National Laboratory
Brookhaven National Laboratory
Oak Ridge National Laboratory
Argonne National Laboratory
NAPAP INTERAGENCY COMMITTEE MEMBERSHIPS
Interagency Science Committee:
Dr. George Y. Jordy DOE
Dr. Lester Machta NOAA
Dr. James F. Meagher TVA
Dr. R. Jack Pickering DOI
Dr. Courtney Riordan EPA
Dr. Eldon Ross USDA
Interagency Policy Committee:
Dr. Joseph R. Barse USDA
Dr. Ralph Brooks TVA
Mr. David L. Dull EPA
Ms. Jacqueline E. Schafer CEQ
Dr. Beverly J. Berger DOI
Mr. J. R. Spradley NOAA
Mr. Edward R. Williams DOE
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1988 ANNUAL REPORT
National Acid Precipitation Assessment Program
Department of Agriculture . Department of Commerce
Council on Environmental Quality . Department of Energy
Environmental Protection Agency » Department of Health and Human Services
Department of the Interior . National Aeronautics and Space Administration
National Oceanic and Atmospheric Administration . National Science Foundation
Department of State . Tennessee Valley Authority
National Acid Precipitation Assessment Program
Office of the Director
722 Jackson Place, N.W.
Washington, DC 20503
January 13, 1989
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NAPAP Task Group Chairmen
Task Group
Emissions and Controls
Atmospheric Chemistry
Atmospheric Transport and
Modeling
Atmospheric Deposition and Air
Quality Monitoring
Terrestrial Effects
Aquatic Effects
Effects on Materials and Cultural
Resources
Name
Ms. Denise Swink
Mr. Bruce Hicks
Dr. Robin Dennis
Mr. F. Paul Kapinos
Dr. Paul H. Dunn
Dr. Daniel McKenzie
Dr. Philip Baedecker
Affiliation
DOE
NOAA
NOAA
DOI
USDA
EPA
DOI
NAPAP Office of the Director
Director:
Scientific Staff:
Technical Staff:
Dr. James R. Mahoney
Dr. Ruth H. Allen
Dr. Patricia M. Irving
Dr. John L Malanchuk
Mr. Ronald J. Nesse
Dr. David S. Renne
Ms. Donna C.Connell
Mr. Robert J. Downing
Mr. Charles N. Herrick
Ms. Judy L Hickey
Ms. Gloria D. Robinson
Ms. Barbara R. Symons
Ms. Denise Vines
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CONTENTS
Introduction
NAPAP Organization 1
NAPAP Assessments 4
1988 Research Highlights and Deliverables
Emissions and Controls
1988 Research Highlights 17
Major Deliverables 19
Atmospheric Chemistry
1988 Research Highlights 23
Major Deliverables 27
Atmospheric Transport and Modeling
1988 Research Highlights 31
Major Deliverables 34
Atmospheric Deposition and Air Quality Monitoring
1988 Research Highlights 35
Major Deliverables 39
Terrestrial Effects
1988 Research Highlights 41
Major Deliverables 47
Aquatic Effects
1988 Research Highlights 55
Major Deliverables 66
Effects on Materials and Cultural Resources
1988 Research Highlights 73
Major Deliverables 76
Publications si
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INTRODUCTION
The Acid Precipitation Act of 1980
(Title VII of the Energy Security Act
of 1980, Public Law 96-294) estab-
lished the Interagency Task Force on
Acid Precipitation to develop and
implement the National Acid
Precipitation Assessment Program
(NAPAP). The purpose of NAPAP is to
increase our understanding of the
causes and effects of acidic deposi-
tion, and to produce scientific infor-
mation to support decisionmaking re-
garding acidic deposition control and
abatement strategies.
The Task Force is required by law to
issue an annual report to the
President and Congress describing the
progress and accomplishments of the
National Acid Precipitation Assessment
Program. This Report, the Program's
seventh, is divided into three major
sections. The first section describes
the Program's organizational
structure, external coordination ac-
tivities, peer reviews, and budgetary
status. It also includes a dis-
cussion of the NAPAP assessment proc-
ess, and provides a synopsis of
NAPAP's plan and schedule for 1989 and
1990 assessment reports. The second
section is a Task Group-by-Task Group
breakdown of the Program's 1988
research and assessment
accomplishments and its plans for
future deliverables. The last section
is a list of NAPAP's 1988 publica-
tions.
NAPAP ORGANIZATION
The Task Force that implements NAPAP
is jointly chaired by the Environ-
mental Protection Agency (EPA); the
Departments of Agriculture (USDA),
Energy (DOE), and the Interior (DOI);
the National Oceanic and Atmospheric
Administration (NOAA); and the Council
on Environmental Quality (CEQ). Other
statutory members include the
Department of Commerce (DOC), the
Department of Health and Human
Services (HHS), the Department of
State (DOS), the National Aeronautics
and Space Administration (NASA), the
National Science Foundation (NSF), and
the Tennessee Valley Authority (TVA).
The Task Force includes four
Presidential appointees as well as
representatives from DOE's Argonne,
Brookhaven, Oak Ridge, and Pacific
Northwest National Laboratories.
Appointed by the Joint Chairs Council
(JCC), the NAPAP Director is respon-
sible for program planning, manage-
ment, and coordination, and for recom-
mending research and assessment ini-
tiatives to the Joint Chairs and the
Task Force. The participating
agencies work with the NAPAP Office of
the Director at several levels. The
Interagency Science Committee (ISC),
comprised of senior scientific mana-
gers from each agency, works with the
Director and his staff to develop,
implement, and evaluate programmatic
research, assessment, and budgetary
requirements. The Interagency Policy
Committee (IPC), comprised of senior
policy officials from the agencies, is
responsible for the review of NAPAP
research and assessment activities to
ensure that they are fully responsive
to policy needs.
.NAPAP's program of research is divided
among seven Task Groups dealing with
the following categories: 1) Emissions
and Controls, 2) Atmospheric Chemis-
try, 3) Atmospheric Transport and
Modeling, 4) Atmospheric Deposition
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and Air Quality Monitoring,
5) Terrestrial Effects, 6) Aquatic
Effects, and 7) Effects on Materials
and Cultural Resources. Senior scien-
tists from the funding agencies are
appointed by the Director and the ISC
to serve as Task Group Leaders. These
individuals are responsible for the
direct oversight of NAPAP research and
assessment activities.
External Coordination and Research
Interaction
A large part of NAPAP's activity is
devoted to coordination among the
various sectors of the acidic deposi-
tion research and assessment com-
munities. NAPAP managers meet regular-
ly with representatives from other
National programs, state government
agencies, the private sector, environ-
mental and resource conservation or-
ganizations, and academia. In addi-
tion, NAPAP draws on state, academic,
and private sector scientists for the
purpose of peer review. NAPAP's 1988
peer review panels included scientists
and technical specialists from
California, Minnesota, Pennsylvania,
the Northeast States
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o projects conducted by the Atmos-
pheric Transport and Modeling
Task Group in May 1988.
In each case, detailed comments from
the reviewers are sent to the appro-
priate agency managers and research-
ers. The Task Force and its member
agencies use the information generated
by the reviews to help guide the
National Program's decisions on re-
search and assessment directions and
project funding. Summary reports from
each of the peer reviews are available
from the NAPAP Office of the Director.
NAPAP FY 1988 Budget
For fiscal 1988, the National Acid
Precipitation Assessment Program's
budget was $82.46 million. Funding
for NAPAP has remained roughly level
over the past three years, after in-
creasing from 1982 through 1986 as the
program implemented its various long-
term research efforts (see Figure
As in years past, the NAPAP budget ap-
portionment has been drawn from six
federal agencies. The Environmental
Protection Agency provided approxi-
mately 62.8 percent of the Program's
funding; the Departments of
Agriculture and Energy were responsi-
ble for 14.2 and 10.5 percent, respec-
tively; and the Department of the
Interior (6.6 percent), the National
Oceanic and Atmospheric Administration
(5.1 percent), and the Tennessee
Valley Authority (1.0 percent) con-
tributed the remainder (Table 1).
As is indicated in Table 1, the total
NAPAP apportionment of $82.46 million
was divided among research categories
as follows: Aquatic Effects, $21.8
million; Terrestrial Effects, $18.5
million; Atmospheric Chemistry, $12.4
million; Atmospheric Transport and
Modeling, $9.9 million; Atmospheric
Deposition and Air Quality Monitoring,
$9.6 million; Emissions and Controls,
$4.7 million; and Effects on Materials
and Cultural Resources, $3.7 million.
FIGURE 1. NAPAP Funding History (in millions)
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TABLE 1. NAPAP 1988 Current Budget ($ K)
USDA
DOI
EPA CSRS ARS FS NOAA DOE NPS USGS FWS BUM TVA TOTAL TG%
I EMISSIONS I CONTROLS
II ATMOSPHERIC CHEMISTRY
III ATMOSPHERIC TRANSPORT
IV ATMOSPHERIC DEPOSITION
& AIR QUALITY MONITORING
V TERRESTRIAL EFFECTS
VI AQUATIC EFFECTS
VIII MATERIAL EFFECTS
Assessment
TOTALS i
Agency Zt
3,985
4,194
8,672
5,919 XI 146
8,198 2,130 284 7,550
18,121 1,005
2,670
2,697 284 8,701
51,759 11,682
62.81 14.21
750
2,806 4,999 400
940 280
430 452 117 1,816 100 40
40 304
250 393 1,044 955 75
825 155
1,850
1,335 3,015 955 100
4,176 8,621 5,405 819
5. It 10.5Z 6.6X l.OZ
4,735
12,399
9,892
9,587
18,506
21,843
3,650
1,850
$82,462
100. OZ
5.7Z
15. OZ
12. OZ
11.61
22. 4Z
26. 5Z
4.4Z
2.2Z
100. OZ
NAPAP ASSESSMENTS
The central focus of NAPAP's 1988 ac-
tivities revolved around the concep-
tion and development of a plan for an
integrated series of assessment re-
ports, to be released in 1989 and
1990. Formalization of the Plan began
in April when the Office of the
Director conducted a week-long work-
shop to discuss the general orienta-
tion and approach that NAPAP will
adopt for assessment development.
This meeting involved over 100 scien-
tists and technical experts from
Federal and State government agencies,
academia, and the private sector.
During the April meeting, attendees
divided into ten working groups based
on the following categories:
Assessment Methodology, Emissions and
Controls, Atmospheric Processes,
Atmospheric Deposition and Air Quality
Monitoring, Terrestrial Effects,
Aquatic Effects, Effects on Materials
and Cultural Resources, Human Health,
Atmospheric Visibility, and Economics.
Each of these groups were requested to
1) define assessment questions,
2) identify pertinent data sources and
methodological approaches, and 3) de-
velop preliminary outlines for reports
detailing the state of acidic deposi-
tion science within each of the areas
of concern. During the months of May
and June, each of the ten groups met
separately with the Office of the
Director to further refine their per-
spectives; and on July 7-8 all ten
groups reconvened to compare their
products and to develop priorities for
an assessment plan.
The draft assessment plan was compiled
in an iterative manner and involved
three review and revision phases dur-
ing July through September. Final
revisions were completed during the
first week of September, and the NAPAP
Joint Chairs Council approved a public
review draft of the Assessment Plan on
October 6, 1988. The resulting docu-
ment, entitled, "Plan and Schedule for
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NAPAP Assessment Reports," was re-
leased for public review on October 12
along with an invitation to attend and
make comments at a public review meet-
ing scheduled for November 17, 1988.
The public meeting was attended by
over 200 individuals. Speakers in-
cluded representatives from the
Canadian Government, environmental
organizations, utility groups, and
various state and provincial govern-
ments. All comments received at the
public meeting, as well as comments
received in writing before December 1,
1988, were recorded and will be con-
sidered in a revision of the Plan that
will be released in January 1989. In
addition, NAPAP will publish a summary
of public comments and indicate how it
responded to these comments in its
revision of the Assessment Plan. The
revised plan may be obtained through
the NAPAP Office of the Director.
The Assessment Plan
The NAPAP Assessment Plan is intended
to be a major element in the technical
dialogue essential for the preparation
of a useful integrated assessment of
acidic deposition causes, effects, and
control measures. The necessary
dialogue is both internal (within the
Task Force) and external (between
NAPAP and potential users of the
Assessment). Acidic deposition issues
involve significant complexity and
uncertainty. To be of maximum benefit
in resolving such issues, the Assess-
ment must be based on a framework well
understood by all of its preparers and
users.
The expected users of the NAPAP
Assessment include the President,
members of Congress and their staff;
policy, technical, and regulatory
officials within the Executive Branch;
representatives of state and local
government units; representatives of
provincial and federal government
units in Canada; representatives of
environmental, health, and other
public-interest groups; repre-
sentatives of industry, utility, coal,
and economic development organiza-
tions; representatives of labor organ-
izations; representatives of control
technology developers and vendors;
interested scientists and engineers;
and interested representatives of in-
ternational organizations and other
government units.
Approach for the Assessment
NAPAP's assessment will be developed
in two principal parts: 1) a series of
State-of-Science/Technology (SOS/T)
Reports - comprehensive analyses and
discussions of relevant technical in-
formation prepared for specialist
readers, and 2) the Integrated Assess-
ment - a structured compilation of
policy-relevant technical information
presented in a form suitable to assist
policymakers and the public in evalu-
ating the key questions concerning
acidic deposition causes, effects, and
control strategies (see Figure 2).
Plan Update: Details of Future
Scenario Cases
NAPAP's assessment methodology incor-
porates a survey of present conditions
and a comparative approach for evalu-
ating future scenarios. The number of
plausible scenarios that might be
evaluated is prohibitively large to
allow comprehensive treatment. NAPAP
is currently developing specifications
of illustrative scenarios for evalua-
tion in the Integrated Assessment.
The illustrative scenarios will con-
form to the three key guidelines be-
low.
o The scenarios will be based on
plausible combinations of emission
reduction strategies.
o The scenarios will reflect the
range of emission reduction strategies
commonly discussed in the national de-
bate about acidic deposition. NAPAP,
however, will not analyze specific
legislative or other public proposals.
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FIGURE 2. Schematic Illustration of the Relationship Between the State-of-
Science/Technology Reports and the Integrated Assessment
Principal Policy
Driving Issues
Integrated
Assessment
\
State of Science/ Technology
Focusing of Major
Relevant Issues
\
All Issues of
Interest to Users
Support Base
NAPAP data and methods will be avail-
able for specialized analysis by other
investigators.
o The scenarios will be selected to
address a wide range of situations in
order to allow adequate briefing re-
lating to questions such as, "How much
difference (in control costs, effects
patterns, etc.) does it make to adopt
one strategy as opposed to another?"
NAPAP plans to report on the specifi-
cation of illustrative scenarios for
analysis in the Integrated Assessment
in an "Assessment Plan Update" docu-
ment to be published in July 1989.
State-of-Science/Technology Reports
The SOS/T Reports are intended to pro-
vide a comprehensive statement of the
technical information concerning
acidic deposition from all available
sources, i.e., both NAPAP-sponsored
studies and all other relevant studies
reported in the technical literature.
Review drafts of these surveys will be
published in mid- and late 1989 and
will be subjected to several levels of
review: interagency review by the
NAPAP cooperating agencies, peer re-
view by independent scientists, and
open review by all interested persons
at an international scientific meeting
convened specifically to evaluate the
reports. Following this extensive re-
view, the SOS/T Reports will be pub-
lished in final form in 1990, and, in
combination with the updated Assess-
ment Plan, will be used as the basis
for the technical findings, analysis
methods, and projection and comparison
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methodologies that are the key ele-
ments of the Integrated Assessment.
The emphasis on full reporting and
extensive external review of the SOS/T
Reports is intended to ensure that the
Integrated Assessment is based on the
broadest available, fully reviewed
technical information. Also, a lay
summary of each of the SOS/T Reports
will be prepared (with scientific and
public review), to ensure that the
principal information is available to
a wider audience of interested read-
ers. The summaries will also serve as
resources for scholastic and public
educational programs dealing with ac-
idic deposition issues.
Currently, 27 Reports, prepared by
approximately 100 specialist authors,
are planned to provide a survey of all
the pertinent SOS/T areas. The scope
of the documents will include 1) emis-
sions, transport, transformation, air
concentrations, and deposition of
acidic and associated pollutants; 2)
effects of acidic deposition and as-
sociated pollutants in all principal
areas of concern (surface waters, for-
ests, agricultural crops, exposed ma-
terials, human health, and visibility
in the atmosphere); and 3) economic
and technological evaluation of con-
trol and mitigation measures and eco-
nomic evaluation methods relevant to
acidic deposition effects.
Integrated Assessment
The Integrated Assessment is intended
to translate scientific information,
with its associated uncertainties,
into results that can be used to ad-
dress relevant questions for the poli-
cymaking audience. The Integrated
Assessment will aid public officials
and other interested individuals by
focusing the scientific and technical
information on the principal issues of
concern, and by interpreting the imp-
ortance of available technical infor-
mation. The Integrated Assessment
will be structured around five key
questions that address both present
knowledge (Questions I and II) and fu-
ture projections (Questions III, IV,
and V).
Present Knowledge
o Question I: What are the effects
of concern, and what is the relation-
ship between current levels of acidic
deposition/air pollutant concentra-
tions and these effects?
o Question II: What is the relation-
ship between emissions of the precur-
sor pollutants and acidic deposition/
air pollutant concentrations currently
observed in North America?
Future Projections
o Question III: What does available
technical information indicate about
the sensitivity to change for the rel-
ationship between (a) emissions and
future conditions related to economic,
energy, and technological develop-
ments; (b) control costs and changes
in emissions levels; (c) emissions
levels and resulting deposition/air
concentration levels; and (d) air con-
centrations/deposition levels and eff-
ects?
o Question IV: What are the esti-
mates of future conditions (emissions,
deposition, and effects) with and
without additional emissions reduc-
tions strategies?
o Question V: What differences
emerge from comparative evaluations of
future scenarios?
Guiding Principles and Scope for the
Assessment
NAPAP plans to complete its assessment
activities within the ten-year
Congressionally mandated reporting
period, resulting in publication of
its Integrated Assessment in September
1990. NAPAP will receive comments af-
ter publication of the Integrated
Assessment, and will conclude all
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program activity with a document
summarizing and responding to issues
raised in the public response to the
Assessment. Publication of this sup-
plementary document is scheduled for
December 1990.
During the next two years, NAPAP will
conduct several parallel activities:
1) completion and documentation of its
program of sponsored research; 2) pro-
duction and review of the series of
State-of-Science/Technology Reports;
and 3) completion of assessment analy-
ses, involving scientific, technologi-
cal, and economic evaluations.
NAPAP's Integrated Assessment is in-
tended to provide users with compre-
hensive scientific, technological, and
economic information on the causes and
effects of acidic deposition and on
the effectiveness of various illustra-
tive control measures in mitigating
the adverse effects. NAPAP has the
responsibility to provide users with
objective, broadly reviewed data and
analyses, which can serve as a basis
for policy considerations. The
Assessment will not make "public
value" recommendations (such as, "What
are the trade-offs between imposing
stricter emissions controls in the
near future vs. waiting for the imple-
mentation of new, cleaner technologies
over the longer term?"), although it
will provide the technical information
and analyses that assist such public
value decisions. NAPAP's assessment
methodology is intended to facilitate
the development of useful information
for a wide range of state-, regional-,
and national-level policy questions.
NAPAP has adopted several operating
principles for the development of the
Integrated Assessment.
o Based on SOS/T Reports - The SOS/T
Reports are intended to cover the
technical basis for the Assessment.
This ensures that the technical infor-
mation used in the Assessment will be
extensively peer reviewed and avail-
able to all users of the Assessment.
o Based on responses to structured
questions - The Assessment will be
developed in the form of responses to
a specific set of high priority ques-
tions, allowing users of the Assess-
ment to review the questions being
posed and to suggest other formula-
tions if needed.
o Explicit treatment of scientific
confidence level - Unavoidable scien-
tific uncertainty precludes complete
resolution of many key cause-effect
issues. Although NAPAP-sponsored and
other research has greatly improved
understanding of many acidic deposi-
tion issues in recent years, uncert-
ainties will remain in 1990. The
Assessment will explicitly report
NAPAP's best estimate of the level of
confidence associated with various
statements (ranging from
characterizations such as "unsupported
hypothesis" to "generally supported by
data, generally agreed by investiga-
tors"). Reporting of scientific con-
fidence level, after extensive peer
review, will aid policy officials in
assigning weight to various statements
in the Assessment.
o Avoidance of oversimplification -
Because of the complexities involved,
there is a tendency to develop assess-
ments of acidic deposition causes,
effects, and controls in the form of
simplified, parameterized analyses.
NAPAP has adopted an approach that
excludes oversimplified dose-response
relationships and integration methods.
This approach precludes development of
an assessment that can express results
in the form of a few key parameters.
NAPAP's assessment, based on evalua-
tion of changes in control costs and
effects patterns compared to a refer-
ence case, will require more compli-
cated interpretation, but will better
reflect the full body of scientific
and technical knowledge.
o Three-part analysis of benefits -
NAPAP's authorizing statute requires
economic analysis of benefits, as well
as control costs. NAPAP will fully
8
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review economic analysis methods for
valuing environmental benefits in the
appropriate SOS/T reports. In the
Integrated Assessment, however, NAPAP
will not report all benefit valuations
in economic form. Instead, three
general categories of benefits will be
reported: 1) health-related; 2) econ-
omically denominated (i.e., those for
which an agreed economic analysis
methodology is available); and 3) con-
servation-related (including important
resource conservation categories for
which acceptable economic valuation
methods are not generally agreed).
o Assessment based on comparisons to
a future case - Most of the technical
data and projection models available
for use in the NAPAP Assessment (e.g.,
air quality models, aquatic system
response models) are better suited to
comparative evaluation than to absol-
ute value projections. Thus, a com-
parative approach allows significantly
improved confidence in the Assessment
findings, relative to absolute
projections. Moreover, most of the
relevant policy questions also are
comparative. For example, "How would
deposition vary with strategies that
reduce emissions uniformly across the
eastern states vs. in the Ohio
Valley?"
Scope of the State-of-Science/Tech-
nology Reports
The 27 SOS/T reports that are current-
ly planned will summarize and criti-
cally evaluate all the scientific and
technical information available in
each relevant discipline. Titles,
detailed outlines, and authors nomina-
ted for these reports are presented in
Part 2 of the Plan. Guidelines for
authors, including a description of
the review process and international
scientific meeting, are also presented
in the Plan. The following section
provides a brief summary of the
purpose and emphasis for the SOS/T
reports within each discipline.
Major Scientific and Technological
Areas for State-of-Science/Technology
Reports
o Emissions: The first SOS/T report
will describe the sources, magnitudes,
and spatial/temporal patterns of emis-
sions contributing to acidic deposi-
tion and involved in acidic deposition
formation processes.
o Atmospheric Processes: Extensive
efforts have been made, both within
and outside NAPAP, to observe and to
model individual atmospheric processes
that affect acidic deposition. The
second SOS/T report will describe the
physical and chemical processes of the
atmosphere pertinent to the formation
and deposition of acidic species, oxi-
dants, and aerosols, and will present
approaches for modeling these proces-
ses.
The third report will describe how the
information presented in Report 2 is
represented in the current science of
regional deposition and air concentra-
tion modeling. The Report will show
how regional atmospheric models form a
hierarchy with a range of applica-
tions. This report will also discuss
procedures for aggregating episodic
model outputs to produce long-term
average deposition and air quality
information of relevance to the ef-
fects analyses.
The fourth report will provide a com-
prehensive description of the Regional
Acid Deposition Model (RADM). The
purpose of RADM and its attendant ag-
gregation scheme is to provide the
estimates of current and future depo-
sition and air patterns.
The fifth report will present a summ-
ary of evaluation and intercomparison
studies for regional acidic deposition
and air concentration models. A par-
ticular focus of this report will be
the program designed to provide field
data for evaluation of regional mod-
els, such as RADM. Evaluation results
-------
will be presented, including the in-
terim evaluation of RADM and the
sulfur-only Engineering Model.
o Atmospheric Deposition and Air
Quality Monitoring: Reports 6 and 7
will describe and analyze the data
available from wet and dry deposition
and air quality monitoring programs.
Data from programs designed for
research purposes, long-term trends
monitoring, and geographic analysis
will be included, along with advances
in quality assurance and data base
management.
o Source-Receptor Relationships:
Report 8 will consolidate the informa-
tion contained in the emissions, atm-
ospheric processes, and deposition and
air quality monitoring reports to
present our current understanding of
source-receptor linkages. Associa-
tions between historical and current
emissions and observed deposition and
air quality patterns will be described
at three levels: 1) descriptive (such
as through the use of maps and
charts), whereby spatial and temporal
emissions data will be compared
against spatial and temporal deposi-
tion data; 2) statistical (such as
through use of regression and trend
analysis); and 3) model-based (such as
through use of linear and Eulerian
model formulations), whereby deposi-
tion and air concentration patterns
and trends are linked to emissions
patterns and trends through simulation
of atmospheric processes.
o Aquatic Effects: A series of seven
reports (9-15) will present the cur-
rent state of knowledge regarding the
chronic and episodic effects of acidic
deposition on aquatic resources. His-
torical status and methods for fore-
casting future change in status also
will be addressed.
Report 9 will summarize the current
chemical condition of surface waters
in five regions of the United States,
evaluate the spatial distribution of
their chemical characteristics, and
examine the associations of surface
water chemistry with watershed charac-
teristics and wet deposition chemis-
try. Results for the United States
will be compared with those for
Canada, Norway, and other nations
having temperate climates.
Report 10 will focus on what is known
about natural watershed processes,
both aquatic and terrestrial, that
affect chronic acid-base chemistry in
lakes and streams. Processes related
to hydrology and biogeochemistry in
watersheds and in lakes and streams,
and those associated with changes in
land use will be examined. How acidic
deposition interacts with these nat-
ural processes, and the implications
for surface water and soil acidifica-
tion or recovery, will be presented.
Results from case studies of soil and
water acidification, conducted inter-
nationally and in the United States,
will be compared for natural systems
with and without acidic deposition and
for a number of experimentally acidi-
fied systems.
Report 11 will be an overview of the
state of knowledge regarding natural
and anthropogenic factors that influ-
ence the acid-base chemistry of sur-
face waters and how these factors
might influence the occurrence and
detection of historical change.
Methods for investigating historical
change (historical water chemistry
measurements, paleolimnological recon-
structions, comparisons between high
and low deposition areas, and models)
and their associated uncertainties
will be discussed. Results from
several distinct lines of investiga-
tion will be integrated to provide
historical estimates of change for
lakes in the Adirondacks, and possibly
for drainage lakes in the Northeast
and Upper Midwest and seepage lakes in
Florida.
The current understanding of episodic
acidification of surface waters will
be summarized in Report 12. The rela-
tionships of episodes to chronic acid-
10
-------
ification and the hydrologic cycle,
their chemical characteristics and
biological significance, and the proc-
esses that control them will be dis-
cussed. The extent and severity of
episodic acidification will be presen-
ted, with data limitations clearly
identified, for the United States, and
compared when appropriate with
European and Canadian information.
This report concludes with a discus-
sion of modeling approaches for re-
gional estimates of the magnitude,
duration, frequency, and extent of
episodes (and associated uncertaint-
ies).
Report 13 will identify the chemical
parameters that influence the effects
of changes in acid-base chemistry on
biological communities and processes.
Methods for quantitatively evaluating
the relationship between changes in
acid-base chemistry and regional ef-
fects on fish populations will be pre-
sented, along with associated uncer-
tainties. Qualitative discussions
will include the effects of surface
water acidification on aquatic organ-
isms other than fish, e.g., benthic
invertebrates, amphibians, waterfowl,
and mammals.
Methods for forecasting changes in
acid-base chemistry of surface waters
and their associated uncertainties
will be presented in Report 14. Three
general types of models - steady-
state, empirical time-varying, and dy-
namic system models - will be evaluat-
ed. Prior model applications in the
United States, other North American
regions, and Europe will be summariz-
ed. Each model will be discussed with
regard to its structure, assumptions
and limitations, sensitivity and be-
havioral analyses, and verification/
validation studies. Error analyses,
linkages to deposition estimates and
inputs to biological models, and pro-
cedures for extrapolation to obtain
regional estimates will be discussed.
The last report on aquatic effects
(Report 15) will be an evaluation of
the mitigative (surface water acid
neutralization) approaches to restore
and protect surface waters from acidi-
fication. This report will include a
description of previously applied mit-
igative strategies and the effects of
these mitigation techniques on ecosys-
tem structure and function.
o Terrestrial Effects: Three SOS/T
reports will evaluate terrestrial ef-
fects. Two reports (16, 17) will dis-
cuss the forest and agricultural crop
resources in the United States. They
will examine factors that influence
forest and crop health and productiv-
ity, forming the basis for interpret-
ing the influences from air pollutants
that will be presented in the third
report for this area. Aspects of ex-
tending interpretation of experimental
results to estimate pollutant impacts
on growth, production, and management
will also be discussed. The third
report (18) will discuss the theoreti-
cal basis for air pollution effects on
plants, experimental results, and our
level of understanding regarding the
mechanisms of plant response to pol-
lutant exposure.
o Materials Effects: The current
state of knowledge regarding the in-
cremental effects of acidic deposition
on the degradation of metals, carbon-
ate stone, paint, and other finishing
systems will be reviewed in Report 19.
Patterns of urban deposition to struc-
tures will be discussed in Report 20.
Methodologies for preparing inventor-
ies of cultural and construction ma-
terials exposed to acidic deposition
for the assessment of materials damage
will be discussed in Report 21, along
with a review of the available data
bases.
o Human Health Effects: Scientific
issues related to both direct and in-
direct health effects of air pollut-
ants associated with acidic deposition
precursors will be discussed in separ-
ate SOS/T reports. Report 22 on dir-
ect health effects will examine the
effects of particulate matter, sulfur
11
-------
dioxide, acidic aerosols, ozone, and
nitrogen dioxide. It will include a
presentation of ambient exposures and
deposition of the pollutants in the
lungs, but the focus will be on health
effects and concentrations/times of
exposures that will cause these
effects. Factors that affect suscep-
tibility to these pollutants, such as
exercise and pre-existing disease,
also will be covered.
Report 23 on the indirect health ef-
fects of acidic deposition will dis-
cuss how acidic deposition can influ-
ence exposure of humans to pollutants
through mechanisms such as acidity-
dependent leaching of pollutants in
some drinking water systems and food-
chain accumulation of pollutants.
Susceptibility factors will also be
discussed. Given the nature of the
data base, this report will focus on
lead, mercury, and asbestos; however,
other relevant metals such as cadmium,
arsenic, aluminum, copper, and zinc
will also be reviewed.
o Visibility Effects: This report,
number 24, will present a thorough
review of aerosol impacts on atmos-
pheric visibility. The document will
describe pertinent theory, results of
controlled experiments, and analysis
of ambient observations. To the deg-
ree possible, the chain of relations-
hips between emissions sources, pol-
lutant concentrations, and perceived
visibility will be discussed.
o Control Measures: Report 25 will
discuss the performance, costs, and
applicability of available and emerg-
ing technologies and other techniques
for emissions reduction. Report 26
will describe models for projecting
future emissions and estimating con-
trol costs and will present results of
selected sensitivity runs of those
models.
o Economic Evaluations: Report 27
will be divided into two sections.
The first section will provide a
general review of the methods used to
estimate the economic values associat-
ed with environmental changes. The
second section will focus on models,
methods, and issues specific to valu-
ing acidic deposition effects.
Scope of the Integrated Assessment
The Integrated Assessment will struc-
ture the scientific information from
the SOS/T Reports to focus on the
principal policy-driving issues.
These issues will be raised in a ser-
ies of questions organized into five
principal categories that will be ad-
dressed in the Assessment. The
approach, assumptions, information
sources, and uncertainties associated
with answering these questions are
described in Part 3 of the Plan. The
guidelines for contributors to the
Integrated Assessment, including a
description of the review process and
the protocol for evaluating the con-
fidence level of the answers, are also
provided in the Plan. The Integrated
Assessment will be developed by the
same technical specialists who have
been involved in the production of the
Plan and by the authors of the SOS/T
Reports. The purpose, approach, and
major focus for each of the five prin-
cipal questions to be addressed in the
Assessment are described below.
Question I: What are the effects of
concern and what is the relationship
between acidic deposition/air pollu-
tant concentrations and these effects?
The basis for concern about acidic
deposition is its possible effects.
Thus, the Integrated Assessment will
begin with a summary of the effects
that have been hypothesized and an
evaluation of the role of acidic depo-
sition and associated pollutants in
causing the effects currently observ-
ed. The evaluation will be conducted
in a sequence of steps, beginning with
a description of the current status
and rate of change for aquatic resour-
ces, forest health, crop production,
materials resources, human health, and
12
-------
visibility. The approach, assump-
tions, and information sources that
will be used to provide this informa-
tion for each effects category are
given in Part 3 of the Plan. The pre-
dicted level of confidence in the
information is also provided. The
important hypotheses that relate the
effects of concern to acidic deposi-
tion and associated pollutants are
then listed along with an estimated
confidence level for the information
available to test each hypothesis.
The approach, assumptions, and infor-
mation available to test each hypothe-
sis are grouped into categories of
evidence from exposure-response stud-
ies and evidence from correlative stu-
dies (such as epidemiological
studies). These two categories of
evidence are then integrated and
assessed, along with information on
the role of other stress factors, to
determine the cause(s) of the effects
of concern. A well-established cause-
and-effect relationship can be devel-
oped only when there is a strong pat-
tern of consistency and responsive-
ness, and a proven mechanism between
observed effects and the suspected
causal factor. The answers to this
question are meant to document system-
atically the determination of causal-
ity for the effects of concern.
Question II: What is the relationship
between acidic deposition, air qual-
ity, and emissions?
Question II is meant to explain depo-
sition and air concentration patterns
and the linkage between emissions
sources and deposition. The first
part of Question II will relate to the
current status of deposition and air
quality relevant to the effects dis-
cussed in Question I, and will rely on
current measurements of deposition and
air pollutant concentrations and on
surrogates for measurement data to
provide a historical perspective of
long-term trends. Because historical
deposition data are lacking, long-term
emissions and visibility trends may be
used to infer historical deposition
trends. The second part of Question
II will relate to source-receptor
linkages, based on knowledge derived
from observations and models. The
third part of Question II will provide
information on changes in deposition
and air quality that may result from
changes in emissions.
Question III: What is the sensitivity
to change?
The ability to estimate future impacts
is an important aspect of environmen-
tal assessment. In order to evaluate
the potential for future changes, a
general methodology must be available
for examining a wide range of relevant
factors. For acidic deposition, this
methodology involves the use of models
and other methods to describe func-
tional relationships. Three major
categories of models to be used in the
Assessment are 1) emissions projec-
tion, 2) source-receptor, and 3) dose-
response. These models range from
very simple empirical relationships to
integrated series of functions.
The answers to Question III will
describe the sensitivity in model out-
put to incremental changes over a wide
range of input factors. This analysis
will also evaluate the relative impor-
tance of key input parameters. This
question is intended to provide the
transition between the current state
of knowledge, as summarized in Ques-
tions I and II, and future projec-
tions, as summarized in Questions IV
and V.
The sensitivity of effects to changes
in emissions will be evaluated for
four areas: 1) emissions, using dif-
ferent assumptions for future condi-
tions; 2) control costs, with emis-
sions changes for a selected set of
emission-reduction strategies; 3)
deposition/air quality, with incremen-
tal emissions changes; and 4) effects,
with incremental deposition/air qual-
ity changes. For the purposes of this
question, effects sensitivity will not
13
-------
be linked directly to the sensitivity
analyses for emissions and deposi-
tion/air concentrations. This linkage
will be developed in the answers to
Questions IV and V.
Question IV: What are the estimates of
future conditions?
A two-part answer to this question
will be provided: 1) estimates of fu-
ture conditions without changes in
current policy and legislation direct-
ed at acidic deposition control, and
2) estimates of future conditions with
illustrative emissions reduction stra-
tegies for S02I NOX, and VOCs.
Looking at the future allows us to
estimate, under various sets of
assumptions, what emissions levels,
source-receptor relationships, and ef-
fects might be. An evaluation of
changes in effects expected to result
from a wide range of scenarios will
allow focus on the more effective sets
of options. This evaluation will also
include calculations of costs for each
control option. The models used in
the sensitivity analyses for Question
III will be linked together to project
future changes in effects for Question
IV. While the output of these linked
models may not have a high level of
confidence in absolute terms, compara-
tive analyses based on changes from
reference cases will generally allow
higher confidence levels.
The inherently uncertain nature of
future conditions will cause the
answers developed for Question IV of
the Assessment to have a lower level
of confidence than those developed for
Questions I and II, which rely direct-
ly on current measurements. The un-
certainties about future conditions
are different from those encountered
in Questions I and II; in most cases
they can only be resolved over time,
rather than by more research. Because
of these uncertainties, many assump-
tions affecting future scenarios that
will be used to answer Question IV
will be based on conditions that
remain constant over time (e.g., land-
use patterns, natural emissions, tree
populations in forests). For compara-
tive purposes, though, the answers to
Question IV should allow a reasonable
level of confidence in evaluating fu-
ture conditions.
Question V: What differences emerge
from comparative evaluations of future
scenarios?
The objective of Question V is to com-
pare and contrast the results of
various future scenarios with and
without additional future acidic depo-
sition control and mitigation mea-
sures. This comparison will be per-
formed through an evaluation of a set
of policy-relevant issues regarding
the need for additional controls, the
costs and effectiveness of .various
levels of control and mitigation, the
timing of implementing such measures,
and the environmental changes that are
expected to result. This information
will help define further analyses of
key issues. As previously discussed,
NAPAP will not develop recommendations
regarding optimal control strategies,
nor will the analysis be aggregated
into a comprehensive benefit-cost
framework.
Examples of these issues include the
following:
o What future trends of emissions and
effects, compared to current cond-
itions, are possible if current Clean
Air Act authorities are not changed?
o Given the geographic regions of
concern for all effects areas, is it
most effective to implement a control
scenario uniformly for all 31 eastern
states or are other scenarios more
effective?
o Is current damage sufficiently low
and the rate of natural resource
change sufficiently slow to warrant
delaying implementation to await com-
mercialization of new, lower-emitting
or possibly more cost-effective tech-
14
-------
nology rather than relying on existing
retrofit technology?
A more comprehensive list of issues
selected for analysis will be reported
in the July 1989 Plan Update.
The answers to these questions will be
based on quantitative answers from
Question IV, as well as information
from the SOS/T Reports and other In-
tegrated Assessment questions. In
many cases, the answers to Question IV
will not provide complete information
on the results of the strategies.
However, comparisons among strategies
will incorporate all available
information about effects, including
levels of uncertainty, as well as
using deposition and control cost
information.
Information on the effect changes will
be categorized according to health
effects, conservation effects, and
economic effects. Health effect chan-
ges are considered separately because
of their general importance and their
prominence within regulatory statutes.
Conservation effects are related to
maintaining or preserving the natural
or cultural environment. Economic
effects include those that can be ex-
pressed in economic terms, by general-
ly agreed methodologies.
15
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EMISSIONS AND CONTROLS
1988 Research Highlights
Current Emissions Trends
A preliminary report of current emis-
sions trends through 1987 indicated
that sulfur dioxide, nitrogen oxide,
and VOC emissions did not change sub-
stantially from 1986. The report pro-
vides an additional year of current
trends data with which to gauge the
status of current Clean Air Act emis-
sion reductions and provides a basis
for the comparison of emissions and
economic activity. Recent emissions
data will also be utilized in the
evaluation of emissions projections
models and regional acid deposition
models.
Transportation Emissions Modeling
Emissions from light duty vehicles
constitute a major area source in the
NAPAP data base. A recent study as-
sessed the uncertainties associated
with emissions estimates derived from
the MOBILE 3 model. The model outputs
were found to be quite sensitive to
input parameters such as average speed
by road type and temperature.
Model Set Integration Review and
Workshop
A third party review and subsequent
workshop were conducted on the model
set integration and the Commercial/
Residential Sector Emission Projection
Model (CRESS). The panel of indepen-
dent reviewers emphasized the need for
consistent integration and recommended
some specific improvements. This will
provide NAPAP with a consistent set of
emissions models to project future
emissions and to evaluate the effec-
tiveness and cost of illustrative con-
trol scenarios.
AUSM Review
An independent review of the Advanced
Utility Simulation Model (AUSM) was
carried out by the Massachusetts In-
stitute of Technology. The review
results are being used to strengthen
the AUSM's methodology. In particu-
lar, inputs from the review have re-
sulted in revisions to the AUSM that
enhance its analytical capability as a
tool to evaluate future generating
technologies.
Transportation Emissions Projections
Model
A third party review and subsequent
workshop were conducted on the Trans-
portation Emissions Projection Model
(TEEMS). Input from the workshop and
review will be used to improve the
TEEMS model. The transportation sec-
tor is the largest emitter of nitrogen
oxides and a large source of volatile
organic compounds. Improvements in
this model will help to provide a more
accurate portrayal of future nitrogen
oxide and volatile organic compound
emissions.
Advanced Utility Simulation Model
In special studies of the Advanced
Utility Simulation Model (AUSM), the
model's forecasts are being compared
to historical emissions data from
1980-1985 and to future emissions pro-
jected by the Coal Electric Use Model
(CEUM), operated by ICF, Inc. The
17
-------
characterization of the extent to
which the model can reproduce histori-
cal emissions data and compares favor-
ably with other models will contribute
to an evaluation of the preformance of
the model.
Utility Reference File
Emissions, facility, and generation
data for all electric utilities in the
United States were compiled in the
National Utility Reference File (NURF)
from data submitted to EPA and DOE.
NURF data are used as input to NAPAP's
Advanced Utility Simulation Model.
Sulfur Dioxide, Nitrogen Oxide, and
Volatile Organic Compounds Projection
Models
Two industrial S02/NOX and a national
VOC emission and cost projection model
were completed and tested. The Indus-
trial Combustion Emissions (ICE) Model
(version 6.0), the Process Model Pro-
jection Technique (PROMPT, version
3.0), and the Volatile Organic Com-
pound (VOC) Model (version 1.8) were
released for agency use. Each of the
models uses a 1980 baseline year, and
future versions will employ a 1985
baseline year. Magnetic tapes or
floppy disks and published reports
were released to the National Techni-
cal Information Service for public
distribution.
1985 NAPAP Emissions Inventory
United States' anthropogenic point and
area source SOX, NOX, and VOC emissions
were complied into the 1985 NAPAP
Emissions Inventory. The 1985 emis-
sions inventory is highly resolved in
space, time, and chemical species.
These intensive requirements were de-
signed to meet the needs of atmospher-
ic modelers. The emissions inventory
will be essential in NAPAP assessment
activities, as well as atmospheric
chemistry studies using RADM and other
mode 1s.
18
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MAJOR DELIVERABLES
DELIVERABLE
DATE
SIGNIFICANCE
1989 Emissions of SOX, NOX(
and VOC (Flash Report):
These emissions data will
provide decisionmakers and
researchers with the latest
trend information in man-
made emissions.
Utility File Updates (Codes
and Report): Updates are
made of the EPA/NAPAP
Reference File to in-
corporate the yearly
utility inputs from sources
such as the DOE/EIA 767,
759, and 423 files; the
North American Electric
Reliability Council (NERC)
files; and the DOE Generat-
ing Unit Reference Files
(GURF) and Flue Gas Desul-
furization Information Sys-
tem Files (FGDIS).
Yearly up- Coupled with deposition and am-
dates bient trends data since 1975,
through these data provide information
March 1990 for developing or evaluating
transformation and transport
hypotheses. Emissions trends
data are also helpful to
decisionmakers who wish to gauge
the impact of current Clean Air
Act legislation and energy and
economic shifts. The March 1990
update will provide the latest
available emissions trends in-
formation to support the NAPAP
State of Science/Technology
Reports and Integrated Assess-
ment.
Early 1989 The 1989 update will be utilized
to update the 1985 data base in
the Advanced Utility Simulation
Model.
19
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DELIVERABLE
DATE
SIGNIFICANCE
1985 Detailed Inventory
(Code and Reports):
Provides estimates of 1985
emissions of some 59 man-
made species of interest
with regard to acidic
deposition formation and
neutralization. The
inventory will be based on
20 by 20 km grid cells with
temporal profiles on an
hourly basis for weekdays,
Saturdays and Sundays, for
each season, and contains a
high degree of source iden-
tification.
Integrated Projection Model
Set: This interconnected
set of sector models and
energy/economic drivers
will be used to project
future emissions of S02,
NOX, and VOC as a function
of assumptions regarding
future economic, energy,
technology, operational,
and control scenarios; and
for estimating the primary
and secondary costs of
illustrative control
scenarios in the NAPAP
Integrated Assessment.
Early 1989
Early 1989
(updates in
early 1990)
The 1985 detailed inventory will
characterize emissions sources
in the United States and Canada,
and will provide input for driv-
ing the RADM atmospheric trans-
port and transformation model.
The 1985 data will support the
Emissions State of Science/Tech-
nology Report and the integrated
assessment activities involving
RADM.
The Integrated Projection Model
Set will play a major role in
answering key questions in the
NAPAP Integrated Assessment with
respect to potential future
emissions patterns and how and
at what costs these patterns
might be altered.
20
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DELIVERABLES
DATE
SIGNIFICANCE
Site-Specific Utility Early 1990
S02/NOX Control Report: This
report will describe the
methods and costs
associated with the
retrofit reduction of S02
emissions from typical
utility units. A detailed
evaluation of 15 plants
will form the basis for a
more generalized evaluation
of the remaining top 200
emitters of S02.
Emerging Technology (Cost, Early 1990
Performance, and Emissions
Report): This report will
analyze the present and fu-
ture state of industrial
sectors and emerging energy
technologies, and describe
factors which will
determine technological
penetration and the
resultant emission
patterns.
This report will provide an im-
proved source of information on
the cost of accomplishing emis-
sion reductions from the utility
sector, because it will be based
on site-specific information as
opposed to "generic" cost infor-
mation. Information, including
retrofit difficulty estimates,
gathered in the development of
the report will be used in the
Advanced Utility Simulation
Model, and will also be utilized
in analyses to be contained in
the scenario comparisons of the
NAPAP Integrated Assessment.
The report will provide impor-
tant information for integrated
assessment activities with
regard to what future emissions
patterns may result because of
the penetration of new energy
technologies in new plant or
repowering/reboiler modes. The
report will be used in analyses
to be contained in the future
conditions and scenario com-
parison parts of the Integrated
Assessment.
21
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ATMOSPHERIC CHEMISTRY
1988 RESEARCH HIGHLIGHTS
Natural Emissions
o NOX emission rates from soils have
been refined.
The emission of nitrogen oxides from
soils is a source of atmospheric NOXI
but the magnitude of this source is
difficult to assess. A major goal of
recent field studies has been to re-
duce the uncertainty associated with
NOX emission measurements, and to im-
prove methods for estimating emission
rates from areas of the size of RADM
grid cells.
During the last year, NO and N02 emis-
sion rates have been measured at sev-
eral sites including an ungrazed
grassland site in Colorado, an uncul-
tivated, ungrazed forest clearing in
the eastern United States, and an
agricultural area in the eastern U.S.
Results of these studies and of con-
trolled tests on synthetic soil samp-
les have been used to relate emission
rates to soil nitrate concentrations,
soil temperature, soil type, moisture,
and pH. Emission rates appear to be
independent of ammonium levels, for
the soils that have been studied; the
emission algorithm that has been de-
veloped depends only on soil tempera-
ture and nitrate level, for reasonable
levels of soil moisture. The results
confirm that soil emissions account
for an average of about 5 percentof
all NOX emissions in the eastern U.S.
Ongoing work is focused on the need to
refine this estimate and to provide
uncertainty bounds for it.
o Systems for measuring ammonia (NH3)
in air have been improved.
Ammonia is the the only basic gas in
the troposphere with concentrations
that are readily measurable, yet can
act as an acidifying agent in soils as
a result of its incorporation in biota
and the release of nitrogen in soil.
Ammonia is known to be derived from
the decay of plant and animal matter,
at average rates that are presently
poorly specified. An assessment of
acid deposition requires an under-
standing of the scope of this problem.
Definitive measurements of ambient
concentrations of ammonia in key re-
gions would permit such an estimate.
Since gas phase ammonia is particular-
ly difficult to measure reliably, work
has started by emphasizing instrument
development, assessment of field reli-
ability, and pilot field measurements.
An automated metal oxide annular de-
nuder system has been developed for
gas phase ambient ammonia measure-
ments; this design represents an ad-
vance in ammonia sampling technology.
The system is based on the adsorption
of ammonia on molybdenum oxide, fol-
lowed by its release (upon heating) as
nitric oxide which can then be meas-
ured using chemiluminescence detec-
tors. Field tests have been conducted
at Niwot Ridge and the Pawnee
Grassland research sites in Colorado.
Gas Phase Chemistry
o Field tests of alternative meas-
urement techniques have continued.
As a continuation of the effort re-
ported last year, two additional field
campaigns were devoted specifically to
comparing the performances of four of
the most popular techniques currently
23
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being used to measure N02 concentrat-
ions, with the intent to demonstrate
the advantages and disadvantages of
each. The most common technique re-
lies on the detection of NO produced
by catalytic reduction of N02; these
methods were found to be susceptible
to interference by other compounds
which are also affected by the cata-
lyst. Methods based on the measure-
ment of luminescence produced by reac-
tion of N02 with organic dyes (usually
luminol) offer a small and convenient
package, but can also suffer from in-
terferences. A more specific but more
complicated method is based on the
conversion of N02 to NO by ultraviolet
light followed by the detection of the
NO by chemiluminescence. The most
advanced method is based on the use of
tunable diode lasers; this was found
to be both sensitive and precise, but
too elaborate for routine use. In
general, the results of the compari-
sons permit more confident selection
of measurement methods for field pro-
grams.
o A major field investigation of in-
teractions of NOX, volatile organic
compounds, and oxidants was conducted.
An intensive study was conducted dur-
ing the summer of 1988, at the Scotia
Range site in central Pennsylvania,
operated by Pennsylvania State Univer-
sity. Measurements were made of of a
wide range of oxidants and nitrogen
compounds, including organic nitrates.
Measurements were also made of the
emission of isoprene from the forest.
An imbalance between the total of the
reactive nitrogen oxides (NOX) and the
sum of the individual components (NO +
NOZ + PAN + HN03) was observed over a
wide range of conditions. The sum of
the individual measured components was
less than the total reactive N0y,
sometimes approaching 20 percent,
greater than had been encountered pre-
viously. The implications of this
imbalance are to be explored further
during 1989, especially in regard to
the uncertainty of predictions of
models.
o Reaction rates of volatile organic
compounds with NOX were measured.
The rate constant for the reaction of
N03 with hydrocarbons derived from fo-
rests (isoprene, and alpha-pinene) and
with acetaldehyde were measured as a
function of temperature in a series of
laboratory studies. Isoprene and al-
pha-pinene are emitted by trees and
are thought to be the most important
natural nonmethane hydrocarbon emis-
sions; they influence the formation of
oxidants and hence affect the produc-
tion of acids. Acetaldehyde is one of
the principal products of the oxida-
tion of anthropogenic hydrocarbons and
is an important compound in the clear-
air reactions that oxidize sulfur di-
oxide and NOX to form acids.
o A new model has been developed to
describe the interaction between pho-
tochemical reactions and vertical
transport in the lower atmosphere.
The impact of natural volatile organic
compounds (VOC) on the oxidation of
NOX and S02 and on the formation of 03
in rural air has been studied using a
one-dimensional photochemical model
with more detailed vertical transport
than in previous simulations. Such
detailed vertical resolution may be
important because the high reactivity
of natural VOC causes their concentra-
tions to decrease rapidly with height;
in comparison, in rural situations
anthropogenic VOC are relatively well-
mixed in the lower atmosphere. The
model shows that the effects of natur-
al VOC on the concentrations of oxi-
dants in the lower atmosphere can
be substantial. Potential consequences
extend to the gas-phase oxidation of
NOX and S02 and the aqueous-phase oxi-
dation of S02; the H202 produced by the
gas-phase reactions provides much of
the fuel for the aqueous-phase oxida-
tion, and hence natural VOC's influ-
ence both gas-phase and aqueous-phase
chemistry.
24
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Preliminary conclusions drawn from
this model, in combination with know-
ledge of aqueous-phase chemistry, are
as follows:
(1) Natural VOC increase the rate of
formation of peroxides and ozone in
rural air.
(2) The aqueous-phase oxidation of
S02 is enhanced by natural VOC.
(3) In relatively clean air, gas-
phase oxidation rates of NOX and S02
are also affected. This effect is
less evident in air with elevated NOX
levels.
These results on the importance of
natural VOC's in producing oxidants in
rural areas differ somewhat from other
model results. Research is underway
to investigate the basis for these
differences.
Precipitation Scavenging
o The 3CPO/PRECP VI field study was
conducted.
A field study of scavenging by midwes-
tern convective storms was completed
during June, 1988. The goal was to
provide the strongest possible data
base for evaluation of the convective-
storm scavenging portion of the
Scavenging Module of the Regional Acid
Deposition Model (RADM). Data are
currently under analysis, and will be
applied along with PRECP V data for
module evaluation during the coming
year.
o Analysis of the PRECP I and PRECP
II data was completed.
PRECP I's data analysis has been con-
cluded; a final series of computer
simulations is now being performed at
the Universities of Kentucky and Iowa.
Diagnostic model runs for the PRECP II
study are nearing completion and will
be published in the open literature
during 1989. Efforts on PRECP II will
conclude with this step. In addition,
data from PRECP III and PRECP IV have
been compiled for use in model evalua-
tion.
o Advanced cloud-physics models have
been developed.
On the basis of the field studies con-
ducted thus far (identified above),
several advanced cloud-physics para-
meterizations have been developed for
use in conjunction with the scavenging
modules of RADM. In essence, the ad-
vanced models will be used to test the
adequacy of the simpler parameteriza-
tions used in RADM, and will provide
an objective evaluation of the uncer-
tainties involved.
o The collection of gas-phase reac-
tants by ice particles and by water
droplets was studied and reported.
Many chemical conversions in the atmo-
sphere take place on surfaces or in
liquid drops; it has been estimated
that half of the S02 emitted by indus-
try is oxidized to suIfuric acid in
liquid drops by peroxides. A labora-
tory study was conducted to measure
the ability of liquid droplets and ice
particles to absorb various trace
gases. The collection of S02, H202,
03, N03, and N02 by ice particles, and
the subsequent reactions, were meas-
ured and have been reported. Nitric
acid exhibits the highest affinity for
ice surfaces, with a retention of
greater than 95 percent in all cases.
Hydrogen peroxide shows a variable
affinity, indicating a retention rang-
ing between 50 percent and 80 percent,
and the remaining gases are less than
1 percent retained. There is a strong
reaction between hydrogen peroxide and
ozone on ice surfaces; this has strong
implications for future modeling ef-
forts involving in-cloud S02 oxida-
tion.
25
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Dry Deposition Processes
o The CORE/satellite dry deposition
research network was extended.
The extension of research data on dry
deposition rates, at selected "CORE"
sites, to satellite stations where
simpler measurements are made contin-
ued; a new satellite site in central
New York is now being set up.
o Dry deposition data obtained rou-
tinely were compared against results
using research methods.
"Benchmarking" efforts continued in
1988, with field studies at Oak Ridge,
Tennessee, and State College,
Pennsylvania. Results indicate that
the routine "inferential" method con-
sistently overestimated the deposition
rate of 03 by 20-40 percent; the cause
appears to lie in an inadequate par-
ameterization of cuticular uptake.
The inferential model of dry deposi-
tion was revised by updating the des-
criptions of stomatal and cuticular
resistance in the program.
o Dry deposition was compared to wet
deposition.
Estimates of the dry deposition rates
of relevant components (S02, S04, N03,
HN03, and the base cations reported in
wet deposition programs) were calcu-
lated for all 12 satellite research
sites up to September 1987. These data
were combined with wet deposition data
at or near the satellite locations to
determine the relative contributions
from dry or wet deposition for each
chemical species. For most locations,
dry deposition of sulfur accounted for
about half of the total deposition
while the dry deposition of nitrogen
compounds accounted for slightly more.
The contribution by dry deposition to
the total deposition of base cations
(present as small particles) was sub-
stantially smaller with values ranging
from 0.05 to 0.2. The role of large
particles is presently being assessed,
for both base cations and nitrate.
o Probability distributions of air
concentrations were computed.
Weekly average air concentration data
derived using the NOAA satellite-site
filterpack network were in general
found to be log-normal. This result
will permit interpolation among the
limited array of dry deposition re-
search stations now in operation.
o Dry deposition to a forest floor
was measured.
In an experiment in April 1988, the
uptake of S02 and 03 by the floor of a
mixed-species forest near Oak Ridge,
Tennessee, was measured. Preliminary
results indicate that deposition ve-
locities to the forest floor are on
the order of 0.1 cm/s for both S02 and
03, substantially lower than values
appropriate for the forest as a whole.
A major goal is to examine the role of
soil moisture on the uptake of 03 and
S02.
o The role of surface moisture was
explored in field studies.
Experiments continue to reveal that
dry deposition is closely linked to
surface moisture. A major limitation
of current models of dry deposition
lies in their crude consideration of
surface moisture; when plants are
short of water, transpiration is lim-
ited and dry deposition rates are low-
er than if water is plentiful. When
foliage is wet, very high rates of
exchange of sulfur dioxide (in partic-
ular) are known to occur. Detection of
surface water and inclusion of mois-
ture in the description of the dry
deposition process is an important
factor. The wetness sensor deployed
in the satellite network has been
tested in a comparison study involving
several alternatives. The results
indicated that the sensors should be
placed as close to the top of the can-
opy as possible, since strong gradi-
ents in humidity exist at night.
26
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o Initial evaluations of the effects
of surface heterogeneity on dry depo-
sition have been conducted.
The spatial variability of dry deposi-
tion was examined for an 80 km x 80 km
area in central Pennsylvania. This
was accomplished by estimating and
comparing dry deposition to individual
1 km x 1 km squares within the larger
area. In this initial study, uniform
meteorological conditions were assumed
across the entire area. However, the
nature of the surface, which controls
the rate of pollutant uptakes, was al-
lowed to vary and was characterized
using satellite imagery. For both S02
and 03, the spatially averaged deposi-
tion was estimated to be about twice
that which would be computed if the
surface were assumed to be covered by
maize only, and about 20 percent lower
than if it were grass.
o Throughfall methods were tested
using sulfur isotopes.
During 1988, experiments were conduc-
ted using 35S tracers with mature trees
to determine that foliar leaching of
sulfate is generally insignificant
relative to the total flux of sulfate
in forest throughfall. This has impor-
tant implications for NAPAP model
evaluations of sulfate deposition,
suggesting that fluxes in throughfall
primarily reflect total wet plus dry
deposition of sulfate. Studies at a
new site in the Smoky Mountains indi-
cate that cloudwater fluxes may also
be measured in this manner.
MAJOR DELIVERABLES
DELIVERABLE
DATE
SIGNIFICANCE
Report on the annular
denuder method for meas-
uring ammonia.
Report on field measure-
ments of natural nitrogen
compounds.
Inventory of natural
aerosol fluxes, elemental
analysis.solubility and
mean time
Refined inventory of ni-
trogen emissions from
soils in the continental
U.S.
Early 1989 Estimates of ammonia emissions
from natural sources require ac-
curate measurement of ammonia in
air.
Mid-1989 NO emissions from soil add to
emissions from anthropogenic
sources. This report will
document emission rates from
soils across the eastern U.S.
Early 1990 Soil-derived particles tend to
neutralize rain acidity. Assess-
ment of the consequences of
reducing emissions require ac-
curate estimates of background
neutralizing capacity.
Early 1990 The NAPAP assessment reports re-
quire an inventory of natural
sources of NOX, since these add
to industrial emissions.
27
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DELIVERABLE
DATE
SIGNIFICANCE
Report on natural hydrocar- Early 1990
bon emission inventory for
the continental U.S.
Report on background NH3
levels representative of
major biomes in the U.S.
Mid-1990
Report on comparisons of Early 1989
methods for measuring N02.
The NAPAP assessment requires
background VOC data. VOC's in-
teract with other chemicals in
the air, and influence the
production rates of acids.
The NAPAP assessment requires
background ammonia data, because
ammonia can neutralize
atmospheric acids in the air and
still act as an acidifying agent
in the soil.
High-quality field
measurements are required to
test model predictions and guide
module development, yet some
methods are not reliable.
Report on the key photoc- Mid-1989
hemical and transport pro-
cesses that control the
budget of atmospheric oxi-
dants.
A model of natural back- Late 1989
ground ozone distribution
and natural oxidation capa-
cities
Report comparing H202 and Late 1989
organic peroxide
concentrations in Colorada
and Pennsylvania.
Report on chamber Simula- Late 1989
tion of single day H202
chemistry - simple hydro-
carbons/NO, mixtures.
The report will help assess
uncertainties in modeling the
oxidation of sulfur and nitrogen
oxides in the lower atmosphere.
Modeling the consequences of re-
ductions in emissions requires
that the background situation be
well understood as well as that
in polluted air.
The report will quantify differ-
ences between the oxidizing
capacities of polluted and clean
air.
Data from smog chambers will
provide a basis to refine model
formulations and assess modeling
uncertainties.
Report on regional budgets
of odd-hydrogen species,
H202 and 03
Early 1990 Background concentrations are
needed to provide a baseline for
RADM predictions.
28
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DELIVERABLE
DATE
SIGNIFICANCE
Report on comparisons of Late 1990
methods for measuring
VOC's.
Report on chamber Simula- Late 1990
tion of single day H202
chemistry -comples hydro-
carbon/NOx mixtures.
Completion of subgrid eval- Mid-1989
uation of reaction kinetics
and scavenging modules.
Installation and Mid-1989
application of source
attribution and emission-
change software in regional
acid deposition model(s).
Completion of processing of Late 1989
PRECP III-PRECP VI data
bases for model evaluation
purposes.
Report on sticking coeffi- Late 1989
cients for water surfaces,
related to atmospheric oxi-
dant concentration.
Completion of statistical Early 1990
analysis of precipitation
chemistry spatial/temporal
variability.
Summary of wet and dry Early 1989
deposition data by location
and by season.
High-quality data are required
for model testing and for module
development, yet some methods
are not reliable. It is sus-
pected that VOC's may presently
be underestimated.
The report is needed to provide
an independent basis for testing
model formulations.
These results will be of direct
importance for interpreting the
validity of the regional
model(s).
This methodology will be
employed as a model-based tool
for direct application to the
1990 assessment.
These data provide a basis for
direct comparison of RADM pre-
dictions against field observa-
tions.
Much of the oxidation of NOX and
S02 occurs in droplets. The
rate of oxidation depends on the
rate of transfer from the air
into the droplet of gas-phase
reactants.
This analysis will have direct
importance for the application
of historical and special-pur-
pose precipitation-chemistry
data for refined RADM model
evaluation.
These data are required as input
to effects computations and for
testing models such as RADM.
29
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DELIVERABLE
DATE
SIGNIFICANCE
Benchmark inferred dry Mid-1989
deposition data against
more direct measurements at
CORE and selected other
sites.
Report on spatial and temp- Early 1990
oral distributions of
dry/wet ratios.
These data are needed to verify
deposition deposition estimates
from routine methods. Such
tests are conducted every year.
Assessment of total deposition
to effects areas can be based on
assumed dry/wet ratios. The as-
sumptions need to be tested.
Report on the application Early 1990
of throughfall methods to
measure cloud droplet and
dry deposition.
Benchmark inferred dry dep- Mid-1990
osition data against more
direct measurements at core
and selected other sites.
Assess the uncertainty in Late 1990
sub- regional estimates of
dry deposition from meas-
urement sites and modeling.
This report will present data on
the total deposition of sulfate
in wet deposition, droplet in-
terception, and dry particle
deposition at high altitude
locations.
Confidence in dry deposition es-
timates based on indirect rou-
tine methods is based on compar-
isons against independent meas-
urements at shared sites.
Comparisons are made every year.
It is needed to assess the error
involved in using point meas-
urements to represent areas and
vice versa. The RADM produces
spatial average estimates,
whereas measurement programs
yield local quantifications.
30
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ATMOSPHERIC TRANSPORT AND MODELING
1988 Research Highlights
Model Development
The version of the Regional Acid
Deposition Model to be used in NAPAP's
1990 Assessment, RADM II, was comple-
ted at SUNY-Albany. This version con-
tains important advances over earlier
versions of the RADM: (1) an improved
advection scheme which significantly
reduces diffusion introduced arti-
fically through the mathematical sol-
ver; (2) an updated dry deposition
module; (3) improvements to the aque-
ous chemistry and wet scavenging mod-
ule which resulted from testing
against the scavenging module deliver-
ed from Pacific Northwest Laboratory
to SUNY and; (4) a significantly en-
hanced gas-phase chemistry module.
RADM II is undergoing final testing
and will be transferred to EPA for use
by NAPAP in January 1989.
A "tagged species" Engineering Model,
based on the full RADM, was developed
by EPA in cooperation with SUNY-
Albany, and implemented on a VAX com-
puter system. The tagging of certain
emitted sulfur species allows for
source attribution to be studied.
Under conditions when oxidants are
limited in the atmosphere, which can
result in non-linear source-receptor
relationships, the linear-chemistry
modeling assumption that the effects
of different sources of emissions can
be treated independently and then
superposed is not valid. Consequent-
ly, the contribution of emissions from
specified sources need to be determin-
ed "in situ" with the other emission
sources. The Engineering Model
version of RADM, operating on an
Eulerian framework, is ideally suited
to meet this analysis need.
Model Evaluation
The Central United States RADM Test
and Assessment Intensives (CURTAIN)
are a series of aircraft measurements
designed to obtain data along the in-
flow boundary of the RADM modeling
domain used in applications. These
data can also be used to establish
seasonal trends in critical chemical
and physical varibles to guide the
setting of chemical concentrations at
the RADM boundaries. Further, the
data can be used to provide critical
chemical measurements for use in the
RADM so that observed concentration
patterns can be compared with RADM
predictions. Flights were made in
each of four seasons along a path near
the Mississippi River between Iowa and
the Gulf of Mexico. The data show
significantly higher hydrogen peroxide
concentrations in summer than in win-
ter. Consistent with 1987 results,
spring and summer ozone concentrations
were higher than the fall and winter.
Both hydrogen peroxide and ozone are
important oxidants that transform sul-
fur dioxide into sulfuric acid. No
significant altitude dependence was
observed for hydrogen peroxide. The
seasonal patterns were duplicated by a
photochemical model, indicating that
the increase in solar radiation and
absolute water vapor from winter to
summer contributed to the increase in
oxidant level. Conversely, hydro-
carbon concentrations were minimized
during the summer. Sulfur dioxide
concentrations peaked in both winter
and summer at low altitude, but at
high altitude little seasonal trend
was evident. Based on the observed
31
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ratios between hydrogen peroxide and
sulfur dioxide, the in-cloud conver-
sion of sulfur dioxide to sulfate in
this region is not expected to be oxi-
dant limited during the summer. There
may be oxidant limitations during
other seasons.
The ACID-MODES surface monitoring net-
work was installed and made operation-
al in June 1988. ACID-MODES is a pro-
ject in support of a two-year regional
acidic deposition model evaluation
program. This EPA-sponsored surface
network is coordinated with three
other networks under the sponsorship
of the Electric Power Research
Institute, the Atmospheric Environment
Service of Canada, and the Ontario
Ministry of the Environment. These
four networks comprise more than 100
sites distributed across eastern North
America for use in the operational
evaluation of the models. As a part
of the model evaluation field study
program, intensive sampling from addi-
tional research-grade surface sites
and from aircraft was conducted during
the period of August 15 through
October 7. This intensive program is
designed to provide data for the diag-
nostic evaluation of regional acidic
deposition models. Although no re-
sults of the intensive data collection
program are available as of yet, the
aircraft program was successful in
completing all planned flight missions
for obtaining data for use in specific
diagnostic model tests.
Model Application
Measurements of dry deposition data
throughout the eastern United States
are limited, yet can be an important
factor in perfoming assessments of the
acidification of aquatic resources.
As a means of interpolating limited
measurements and estimating dry depo-
sition levels for the eastern United
States, the Regional Lagrangian Model
of Air Pollution (RELMAP) was tested
against observational data from twelve
monitoring sites in the northeastern
Unites States and southeastern Canada.
The results of this test suggest that
RELMAP underpredicted dry deposition
near sources and overpredicted dry
deposition at longer distances from
sources, and as a consequence, did not
replicate the strong dry deposition
spatial variations indicated by the
available data. Modifications to the
RELMAP were made. In addition, the
first generation version of RADM (RADM
I) was applied to the study. The
results indicate that the revised
RELMAP and the RADM I both provide
reasonably good replications of the
observed dry deposition fields. This
indicates that the revised RELMAP and
the RADM I might be used as a means of
interpolating actual dry deposition
measurements, once model calculations
have been "anchored" to actual obser-
vations. This technique of using mod-
els to interpolate limited data sets
could be an important methodology for
providing the information needed for
effects assessments.
Special Studies: Characteristics of
Regional Transport
The Across North America Tracer
Experiment (ANATEX) was a field study
conducted in early 1987 to provide
experimental data on the meteorologi-
cal influence on the transport and
dispersion of pollutants over scales
of hundreds to thousands of kilo-
meters. By releasing tracer material
at two different ground level loca-
tions in the central United States and
tracking the material as it spreads
eastward, data which demonstrate the
ability of long-range transport models
to represent the regional transport of
pollutants released at ground level
can be obtained. Further, the data
can be used to characterize meteoro-
logical influences on regional
transport.
Although the analyses are somewhat
limited since tracer observations are
based on 24-hour averages, preliminary
results show that the behavior of the
32
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tracer material after release is in
part a function of the release rela-
tive to large scale weather patterns.
For example, several cases indicate
that the material remained within the
airmass into which it was released,
particularly behind a frontal system,
for extended periods. The position of
the material remained stationary rela-
tive to troughs and ridges, and hori-
zontal transport was accomplished by
movement of these troughs and ridges
relative to the ground. This illus-
trates the classic case of fronts
acting as barriers to the pollutant.
However, there were also cases where
material was released in the vicinity
of a front, and found behind the front
in subsequent sampling periods, or was
dissipated by the passage of the
front, presumably due to strong verti-
cal mixing and wind shear aloft.
These preliminary observations suggest
that pollutants released at ground
level may not always behave in a clas-
sic sense near frontal systems. This
may be of considerable importance for
the development and evaluation of
long-range transport models, which
incorporate a variety of assumptions
regarding the flow of pollutants in
the vicinity of air mass boundaries.
Special Studies:
Field Study
Washington Mesoscale
The Washinton D.C. Mesoscale Field
Study, like its predecessor the Phila-
delphia Study, was designed to provide
observational information on the rela-
tive importance of industrial and
transportation emissions within the
"urban plume" on the wet deposition of
pollutants on the mesoscale. The
intention is to provide insight on the
amount of urban emissions available
for long-range transport, which is
directly relevant for the evaluation
of models such as the RADM. Results
from four storm measurement periods in
the Washington study confirmed find-
ings from the Philadelphia study: When
wind directions remain relatively uni-
form throughout the storm event, clear
upwind-downwind differences in rain
chemistry are observed. Downwind ni-
trate wet deposition increases
considerably above background. The
study further indicates that mesoscale
circulations embedded within the
storms can have a significant influ-
ence on deposition patterns.
33
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MAJOR DELIVERABLES
DELIVERABLE
DATE
SIGNIFICANCE
A report on an analysis of
emissions change and source
attribution using the RADM
II and the Engineering
Model.
A report on an analysis of
nonlinearity based on the
applications of RADM and
the Engineering Model.
Late 1989
Late 1989
A report covering 1987
ANATEX results.
Mid-1989
A report on the preliminary
evaluation of RADM II
against the first six
months of field study data.
A report on CURTAIN program
boundary condition
measurements for use by
RADM.
Early 1990
Late 1989
The report will provide an
assessment of source attribution
using the new models,
incorporating the effects of
nonlinearity.
This report will provide an
assessment of the importance of
nonlinearity in the acidic
deposition system, involving
transport and transformation. It
will also provide a reference
against which to judge earlier
estimates of the effect of
emissions changes in a given
source region on deposition to
receptor areas.
This report will provide a data
base for testing the estimates
from mathematical models of
inert gas transport under more
complex meteorological
conditions.
The report will provide a first
evaluation of the RADM II. It
will also provide an assessment
of the degree of confidence
associated with the use of RADM
for NAPAP's assessment
activities.
The report will provide an
important data base for reducing
uncertainties in setting
boundary conditions for the RADM
model.
34
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ATMOSPHERIC DEPOSITION AND AIR QUALITY MONITORING
1988 RESEARCH HIGHLIGHTS
o The annual data summary of precip-
itation chemistry in the United States
for 1987 was published by the NADP/NTN
Coordinator's Office at Colorado State
University. The annual mean pH data
for 1987 are shown in Figure IV-1.
Network data suggest no striking chan-
ges in the pH of precipitation during
the past several years since NAPAP has
been producing these maps. Several
organizations, including the U.S. Geo-
logical Survey (USGS) and the U.S.
Environmental Protection Agency (EPA),
are involved in analyzing and summar-
izing data from the NADP/NTN in prepa-
ration for the NAPAP assessment.
o A LOWESS (locally weighed scatter-
plot smoothing) analysis of the
NADP/NTN blind-audit data was per-
formed by the USGS for all data from
1980 to 1987. This evaluation indi-
cates that during the 7-year period,
contamination of the samples by
sampling-materials has decreased for
calcium, magnesium, chloride, and sul-
fate. The annual average contamina-
tion in samples of calcium, magnesium,
chloride, and sulfate is, respective-
ly, 0.05 mg/L, 0.02 mg/L, 0.04 mg/L,
FIGURE IV-1. pH of Wet Deposition in 1987. (Precipitation-weighted Annual
Average) Based on NADP/NTN Data. Isolines omitted in West due to
sparceness of data points.
35
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FIGURE IV-2. NDDN Monitoring Sites. Continental United States. (Through
Fiscal Year 1988)
and 0.09 mg/L. Sodium contamination
of the samples by the same sources
generally decreased until 1986 and
increased during 1987. Hydrogen-ion
neutralization appears to have de-
creased until about 1986 and has been
steady since that time. This recogni-
tion of sample contamination is impor-
tant because it permits more accurate
data evaluation and deposition
computation.
o A 52-station National Dry Deposi-
tion Network (NDDN) has been designed
(Fig. IV-2) and is in the process of
deployment. Basically a long-term
trends network, the first thirty-five
sites have been placed in operation in
the eastern United States in support
of an international model evaluation
program sponsored by the EPA, Electric
Power Research Institute, Atmospheric
Environment Service of Canada, and the
Ontario Ministry of the Environment.
Field, laboratory, and data management
procedures have been developed to per-
mit rapid delivery of validated data.
As the first broad-scale dry deposi-
tion network established in the U.S.,
data from the NDDN will be used to
determine the contribution of dry
deposition to total deposition in the
East.
The current database is limited to 35
sites, some of which have less than 1-
year's data; however, important pat-
terns have begun to emerge. First,
the seasonal variability of S04"2 is
high relative to that to HN03 and N03".
Average S04"2 concentrations decrease
by a factor of 2 from summer to
winter, while S02 concentrations in-
crease by a factor of 2, except in the
midwest. HN03 is reasonably constant
from season to season, while N03"
exhibits what appears to be site-spec-
ific variability. Second, annual av-
erage rural ozone concentrations for
1987 show little variability across
the network (range is from 30 to 34
ppb). On a monthly basis, however,
significant seasonal variability is
apparent. In general, the southwest-
ern Virginia site and the site south-
west of Chicago, Illinois, exhibit the
36
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highest and lowest monthly ozone val-
ues, respectively. Diurnal variabil-
ity, or the lack thereof, appears to
explain much of the difference between
these two extremes.
o The Global Trends Network (GTN) was
established in 1980 to measure pre-
cipitation chemistry in areas far from
manmade sources. Between May 1980 and
August 1985, 190 precipitation events
were sampled on Amsterdam Island, a
GTN site located in the central Indian
Ocean, and samples were subsequently
analyzed for major chemical constitu-
ents, losbaric back trajectories were
calculated for each event and a clus-
ter analysis technique was used to
identify patterns in the multivariate
data sets for both chemistry and
transport. The cluster analysis tech-
nique represents a relatively objec-
tive alternative to the more subjec-
tive method of classifying trajector-
ies according to compass sector, or
stratifying chemical concentrations
into evenly spaced ranges. In this
analysis two chemical clusters were
identified; one representing 141 sam-
ples and the other having 21 samples.
Storms in the smaller chemical cluster
occurred mainly in the spring and were
associated with significantly greater
deposition of H+, NH4+, N03", and non-
sea-salt (nss) S04"2. Samples in the
larger subset were very clean. Four
distinct transport clusters revealed
no significant differences for either
concentrations or per-event deposi-
tions of any of the major chemical
constituents suggesting that transport
is not an important factor in control-
ling the chemical composition of pre-
cipitation on the island. Although a
continental influence on some air mas-
ses was suggested from both back tra-
jectories and data for 222Rn and C02, a
signal in terms of major ions in
associated precipitation events was
not discernible from the marine back-
ground after the mean 3.5 day trans-
port over the ocean. A significant
seasonal signal in nss S04 , NH/ and H*
is consistent with the hypothesis of
stronger source strengths of marine
emissions and enhanced photochemistry
during warmer months.
o A major intercomparison program
has been undertaken at the
Pennsylvania State University Atmos-
pheric Chemistry Research Site.
Installation of an instrumentation
trailer and new precipitation and air
sampling equipment proceeded through-
out the spring of 1988. Complete op-
erations began in June and are
scheduled to last approximately 2
years. The purpose of the project is
to intercompare collectors and proto-
cols for sampling and analysis used by
all of the major measurements programs
involved in NAPAP. In addition to
program intercomparisons, most of the
programs have set up duplicate samp-
ling equipment in order to obtain data
from which measurement precisions can
be estimated. This large intercompar-
ison project follows and extends an
earlier project, which began in
October 1988 and is coordinated by the
USGS, to compare the sampling methodo-
logies of CAPMoN and NADP/NTN. Pre-
liminary results of this initial study
reveal minor differences in some para-
meters, specifically N03" and NH4*, but
overall agreement is within about 10
percent. Extensive analysis of the
complete data sets from all of the
programs involved, to be conducted
toward the end of the 2-year measure-
ment phase, should provide a quantita-
tive means of assessing the quality of
the data on which validation of the
acidic deposition models will depend.
o Daily precipitation samples are
collected at nine sites of the Multi-
state Atmospheric Power Production and
Pollution Study (MAP3S) network in the
eastern United States. An analysis of
the distribution of event deposition
at these sites has shown that while a
significant fraction of the deposition
of the major ionic species is contri-
buted by relatively few events, the
MAP3S network sites are not as strong-
ly "episodic" as are sites in remote
areas. The deposition distributions
for the major species are quite uni-
37
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form spatially: the highest 20 percent
of deposition events contribute about
55 percent of the annual deposition of
sulfate, whereas the highest 20 per-
cent of the precipitation events con-
tribute only 40 percent of the annual
precipitation amount. This indicates
that high deposition episodes are in
part caused by relatively high ionic
concentrations and are not exclusively
due to high precipitation amounts.
Therefore, the study of ecosystem
responses to acidic wet deposition
must consider the effects of high con-
centration events as well as episodic
deposition amounts.
o MAP3S data have been analyzed for
evidence of temporal trends. At some
sites the data record now extends
beyond ten years. Statistically sig-
nificant (p=0.05) linear trends were
found in the annual precipitation-
weighted mean ionic concentrations for
only a few species at a few sites.
Concentrations of H+ decreased with
time at both Ithaca, New York and Ox-
ford, Ohio, but only at Oxford did the
concentration of S04"z also decrease
significantly. Except for NH4+, which
has increased with time at Ithaca, no
other significant trends over the
MAP3S data period from 1977 to 1986
were found for any of the other major
ions at any other sites.
o An analysis of pre- and post-event,
gas-phase concentrations of ammonia at
Pennsylvania State University found
that below-cloud scavenging contribu-
ted less than 50 percent of the ammon-
ium found in rainwater at this MAP3S
site. In spite of the high solubility
of ammonia in water, the limited rate
of diffusion of ammonia to raindrops
prevents the drops from achieving
equilibrium with gas-phase ammonia
during their transit from cloud base
to the surface. Therefore, the major-
ity of the ammonium ion found in rain-
water must be incorporated via in-
cloud processes.
38
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MAJOR DELIVERABLES
DELIVERABLE
DATE
SIGNIFICANCE
1988 precipitation Mid-1988
chemistry data for all
NADP/NTN stations.
A report on the temporal Late 1989
and spatial trends analyses
of wet deposition data.
An issue paper addressing Mid-1989
spatial interpolation
techniques for wet
deposition.
A data report and analysis Mid-1989
from the National Dry
Deposition Network, 1984-
1988.
A summary report on 1987 Late 1989
MAP3S network data.
A summary report on MAP3S Late 1989
network research
activities.
These data will be available for
interpretation by NAPAP scient-
ists and used for NAPAP assess-
ment activities.
This report will provide an
interpretation of spatial and
temporal changes in wet
deposition over the last 10
years.
This paper weighing the pros and
cons of a variety of
interpolation techniques will be
presented and recommendations
made on how best to present data
for NAPAP Assessment.
This report will describe and
analyze the first four years of
data from the National Dry
Deposition Network.
This report will provide an
update on precipitation
chemistry statistics and trends
through 1987.
This report will provide an
overview of all of the research
accomplishments produced by the
MAP3S community since the start
of the network in 1976.
39
-------
DELIVERABLE
DATE
SIGNIFICANCE
Several journal articles Mid-1989
will be published on the
higher moments of the
distributions of event
precipitation chemistry.
A journal article on the Early 1989
use of multiple regression
techniques to classify
western NADP/NTN sites in
terms of the relative
importance of S04 and N03 as
acidifying influences on
precipitation.
These articles will provide
information on the shape of the
frequency distributions of ionic
concentrations in precipitation
that can be compared to results
from computer simulations of
acidic deposition processes.
This publication will identify
local and regional sources of
air pollution which dominate
acidic deposition at specific
monitoring sites.
40
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TERRESTRIAL EFFECTS
1988 RESEARCH HIGHLIGHTS -
CROPS
Soybean Response to Acidic Rain
Controlled experiments utilizing simu-
lated acidic rain indicate that ambi-
ent and even greater-than-ambient lev-
els of rain acidity have no direct
effects on the growth and productivity
of the cultivars examined. Studies of
two soybean cultivars (Williams and
Cutler 71) demonstrated no significant
differences in growth or seed yield in
treatments groups receiving simulated
rain at pH levels of 3.0, 3.5, 4.0,
and 5.0.
These experimental results are consis-
tent with other studies and do not
appear to support earlier reports that
acidic rain may reduce soybean yield
although further studies of cultivar
differences may be necessary to fully
evaluate this conclusion.
Response of Corn to Acidic Rain and
Drought
Preliminary results from a third year
of study to examine the possible in-
teraction of rain acidity and drought
stress on corn are supportive of the
second year's results which indicated
no significant interaction. This out-
come suggests that an apparent inter-
action between the two stresses ob-
served for one of two corn cultivars
during the first year of study cannot
be easily explained or readily repeat-
ed. Studies at another research in-
stitute suggest a possible mechanism
for such an interaction but corrobo-
rating studies have failed to provide
additional support.
These results tend to minimize early
speculation that an acidic rain event
during pollination and after prolonged
drought stress may be an important
mechanism by which corn yield is re-
duced during periods of drought
stress.
Acidic Rain and Ozone Effects on the
Rhizosphere
Studies using sorghum x sudangrass
hybrid seedlings in a soil-sand mix
were completed to examine the effects
of ozone and acidic rain on rhizo-
sphere microorganisms. Opposing ef-
fects of the two types of pollutants
(generally inhibitory at the highest
03 level and stimulatory at the high-
est rain acidity level) contributed to
a significant 03 x acidity interaction
with respect to shoot growth.
Ozone and acidic rain also generally
caused different changes in the rhizo-
sphere, but an interaction was ob-
served for only one of eight assays.
Conclusions regarding pollutant ef-
fects on rhizosphere ecology must be
considered in the context of specific
pollutants and microorganisms.
Acidic Fog Effects in California
Strawberry plants exposed to several
repeated simulated fog events at pH
levels of 1.6 had reduced yield com-
pared to plants exposed to higher fog
pH.values; however, pH levels of 2.0
did not result in yield impacts after
ten weeks of treatment although visi-
ble injury was evident. Injury of the
calyx at pH 2.8 and lower suggests
that crop marketability may be affect-
ed at these lower pH levels.
41
-------
These studies indicate that further
research and monitoring activities are
needed to examine the magnitude and
extent of low acidity fog events in
the south coast of California and
their possible effects on crop yield
and quality.
Acidic Deposition Effects on a Forage
Plant/Soil System
The response of a forage ecosystem to
different deposition acidity levels
over the short term was examined to
determine possible impacts on an agri-
cultural system regarded to be poten-
tially sensitive to acidic deposition.
In experiments using simulated rain
for two acidic, low CEC unfertilized
soils, orchardgrass seedling viability
and dry weights were significantly
enhanced by the two most acidic treat-
ments (pH 3.1 and 2.5) compared to pH
3.7 and 4.3. The composition of the
soil solution was also affected by the
acidity of the rain treatments; nutri-
ent levels, acidity, and ionic
strength increased while the Ca/Al
activity ratio decreased with increas-
ing rainfall acidity.
Agricultural soils lacking natural
buffering ability and receiving rela-
tively low intensity management may be
particularly sensitive to acidic depo-
sition, yet these studies with an or-
chardgrass forage system indicate that
simulated rain at high acidity levels
can have a positive effect on seed
germination and growth even though
soil solution chemistry is changed.
Effects on Soil Through Foliar
Applications of Acids
Foliar application of sulfuric acid
(pH 3.2) to recently germinated alfal-
fa, corn, fescue, and soybean had lit-
tle influence on the acidity of the
soil adjacent to the roots of these
plants when compared to plants treated
with a control solution (pH 5.6), ex-
cept for corn where soil pH adjacent
to the root was reduced by 0.1 unit.
Regardless of treatment, there was a
trend for pH differences in the vicin-
ity of roots to increase as bulk soil
pH increased from 4.0 to 6.2.
There is little evidence that applica-
tion of acidic solutions to foliar
surfaces changes the acidity level of
root exudates to the degree that soil
pH is affected, except possibly for
corn growing in nearly neutral soil.
Interactive Effects of Ozone and
Sulfur Dioxide
Exposure to very high concentrations
of sulfur dioxide (as high as 0.4 ppm
for 4 hrs per day, 5 days per week for
4 weeks) did not produce any visible
injury symptoms in three watermelon
cultivars in greenhouse experiments.
However, foliar injury resulting from
0.1 ppm ozone for the same exposure
times was significantly increased when
combined with simultaneous sulfur di-
oxide exposures that had no effect
when they occurred in the absence of
ozone.
Further research at lower pollutant
concentrations is indicated to deter-
mine if ambient levels of sulfur di-
oxide and ozone interact synergisti-
cally to affect watermelon growth and
yield as is reported for the higher
concentrations used in this study.
Ambient Ozone Affects Melons in
Indiana
Additional observations of field-grown
melons in Indiana indicate that appar-
ent foliar injury from ambient levels
of ozone was more prevalent in water-
melon than in muskmelon and that early
maturing varieties were more suscep-
tible to injury than late-maturing
varieties, perhaps because higher lev-
els of ozone occurred during suscepti-
ble growth periods of the early-matur-
ing varieties. Both muskmelons and
watermelons had lower yields in plants
42
-------
exposed to non-filtered air compared
to plants grown in open-top chambers
with filtered air that removed ambient
ozone.
Differential ozone sensitivity in mel-
on cultivars may be related to differ-
ences in maturity times and periods of
high ambient ozone concentrations dur-
ing susceptible life stages. Ambient
ozone apparently reduces the yield of
some melons in southwestern Indiana.
Use of EDU to Examine Ozone Effects
In field experiments using the antiox-
idant EDU to protect plants from am-
bient levels of ozone, five white po-
tato cultivars were differentially
susceptible to ambient ozone with re-
spect to foliar injury and yield re-
duction. Significant effects on yield
were observed in two of three culti-
vars in New Jersey in 1980 when foliar
injury was 75 percent or greater and
cumulative ozone dose was 110 ppm hr.
A similar approach to examine soybean
cultivars during 1982 through 1985 did
not indicate significant effects from
ambient levels of ozone as high as 101
ppm hr.
Further studies of EDU effects on soy-
beans are needed to determine effec-
tive doses and to reconcile apparent
differences in these results with
those of several other studies that
have predicted negative impacts on
yields of soybeans at ozone concentra-
tions similar to those causing no ef-
fect in these EDU studies.
Ozone Effects on Photosynthetic
Processes
In experiments using isolated soybean
cells, ozone reduced post-treatment
photosynthesis when ozone was adminis-
tered in the light or in the dark.
The results indicate that ozone can
affect photosynthesis independently of
affecting stomatal activity and that
the damage can occur when the cell is
not actively photosynthesizing. This
provides significant new information
on possible mechanisms of ozone
damage.
Indirect Effects of Ozone on Soil
Organisms
Experiments to determine the effects
of ozone on beneficial root-infecting
microorganisms indicated that ozone
exposure induces an alteration of the
carbon relations among subterranean
clover and its two microbial sym-
bionts, rhizobia and an endomycor-
rhizal fungus. Ozone suppressed the
proportion of plant nitrogen that had
been fixed from the air.
The results indicate that the direct
effects of ozone on carbon allocation
in plants may have indirect effects on
associated soil organisms which result
in further changes to the ecosystem.
More research is necessary on this
important aspect of potential air pol-
lution damage to terrestrial ecosys-
tems.
Survival of Ozone-Resistant Plants
Within a Population
Clones of ladino clover that survived
two years of exposure to high doses of
ozone in the field were generally much
more resistant to subsequent short-
term ozone exposure than those surviv-
ing two years of exposure to low ozone
levels.
Thus, individual plants within a per-
ennial crop population that survive
exposure to high levels of ozone may
be genetically predisposed to resist
the damage caused by ozone and are
therefore less sensitive to subsequent
ozone episodes than a population of
unexposed plants. This suggests that
under polluted conditions ozone-resis-
tant individuals within a population
have an advantage and that over time
43
-------
this may result in lower ozone sensi-
tivity in naturally reproducing popu-
lations.
1988 RESEARCH HIGHLIGHTS -
FORESTS
Varietal Differences in Response to
Ozone
Results of initial experiments with
two varieties of snapbean indicated
physiological and developmental char-
acteristics that might account for
observed differences in their growth
response to ozone. The sensitive va-
riety may absorb ozone at a much high-
er rate and also appears to allocate a
greater proportion of its total photo-
synthate to reproductive growth, per-
haps leading to a reduced ability to
compensate for pollution-induced leaf
tissue injury than more resistant va-
rieties.
These studies provide additional in-
formation that sensitivity to ozone is
genetically determined and is related
to metabolic rates and strategies of
carbon allocation.
Ozone-Drought Interaction
Experiments performed with soybeans at
two different laboratories did not
detect a significant interactive ef-
fect on yield between drought and
ozone stress, although both ozone and
drought reduced yields. In one of the
experiments root growth was stimulated
by drought stress but reduced by ele-
vated ozone, whereas, in we 11-watered
plots ozone had little effect on root
growth.
A number of experiments have indicated
an interactive effect of ozone and
drought stress on crop plants.
Definitive conclusions cannot yet be
reached, however, because, as these
studies indicate, the results have not
been totally consistent. More infor-
mation on the influence of the timing
and magnitude and the two stresses may
resolve the inconsistencies.
SOUTHERN COMMERCIAL FORESTS
Dose-Response Studies
Open-top chamber studies of loblolly
pine seedlings found no apparent ef-
fects of simulated acid precipitation
through the first year of treatment.
However, a small but significant
growth increase was seen after 18
months at the pH 3.5 treatment. This
stimulation in growth may be a fertil-
ization effect from added nitrogen in
the simulated acid precipitation.
Soil Characteristics
Based on a critical analysis of infor-
mation on soils, it is expected that
up to 30 percent of southern forest
soils will show major changes in soil
chemistry within the next 50 years.
Many southern soils are not expected
to retain deposited sulfur in the fu-
ture. However, virtually all deposi-
ted nitrogen will be retained by the
forest ecosystem. These projections
will be vital inputs to NAPAP terres-
trial assessment activities. This
analysis was based on: (1) a synthesis
of available literature on the biogeo-
chemical impacts of sulfate and
nitrate, (2) an examination of empiri-
cal evidence relating to the effects
of sulfate and nitrogen on southern
forest ecosystems, and (3) simulation
models exploring soil sensitivity to
sulfate deposition.
EASTERN HARDWOOD FORESTS
Minnesota-to-Michigan Deposition
Gradients
A study of the relationships between
various aspects of forest condition
and atmospheric deposition concluded
that there is a terrestrial sulfur
44
-------
gradient which increases from north-
eastern Minnesota to southeastern
Michigan and corresponds to a gradient
of atmospheric wet sulfate deposition.
This conclusion was based on chemical
analysis of forest floor and mineral
soil samples from 169 forested plots.
Sulfate deposition estimates for each
plot were derived from NADP monitoring
stations and weather stations. For
sampling and sataistical purposes, the
anthropogenic deposition gradient was
divided into five zones from west to
east corresponding approximately to
the 1, 2, 4, and 8 kg/ha/yr total sul-
fate isolines of the acid sulfate de-
position gradient. Estimated total
average sulfate deposition levels
ranged from 7.5 to 18.2 kg/ha/yr for
plots in zone one (west) through zone
five (east) and were significantly
different (p=<0.01).
The study did not indicate a
corresponding gradient in sulfur con-
centration in tree woody tissue based
on chemical analysis of increment
cores. The strongest relationships
between diameter growth and sulfate
deposition estimates were for jack
pine, red pine, and sugar maple. The
relationship was negative for the
pines and positive for sugar maple.
Maple Decline
A joint United States and Canadian
research program on the causes of
sugar maple decline is underway.
Field plots have been established in
both commercial sugar bushes and
natural stands of sugar maple in On-
tario, Quebec, New Brunswick, Maine,
Michigan, New Hampshire, New York,
Vermont, Massachusetts, and Wisconsin.
Initial tree vigor ratings were made
using a field manual prepared by the
study team. Subsequent ratings in
1989 and 1990 will establish the rate
of change in tree condition in rela-
tion to: (1) high vs. low pollutant
(sulfate and nitrate) deposition
zones, (2) commercial sugar bush vs.
natural stands, and (3) initial vigor
rating. Also underway is a feasibil-
ity study for sampling root feeding
insects which have been implicated in
maple decline.
Hardwood Decline
A case history study of hardwood de-
cline in the eastern United States has
been completed. This literature re-
view found that many hardwood species
have experienced declines and mortal-
ity events during the last few de-
cades. This may be due to intensified
reporting and to the maturation of the
forest. Most of the mortality events
have been attributed to various abi-
otic and biotic stress factors such as
weather, management practices, and
damage by insects and diseases. Firm
evidence of atmospheric pollutant dam-
age is present from point-source pol-
lution such as smelters and from ozone
damage on white pine. No consistent
evidence was found in these reported
studies for an association between
patterns of hardwood mortality and
regional atmospheric pollution.
Sensitivity Testing
A seedling exposure study to screen 12
important eastern hardwood species for
relative sensitivity to acid rain,
sulfur dioxide, and ozone, singly and
in combination, has been completed.
Ozone was by far the most toxic of the
three compounds, as measured by foliar
symptoms to seedlings. The more sen-
sitive species in terms of foliar in-
jury or growth response include white
ash, yellow birch, sweetgum, red ma-
ple, yellow poplar, and sugar maple.
White oak, shagbark hickory, and Amer-
ican beech were more tolerant. In-
crease in rain acidity from pH 4.2 to
3.0 caused white ash to decrease
height growth by 6 percent and leaf
dry weight, leaf area and new growth
dry weight by 20 percent. This same
45
-------
change in rain pH caused an increase
in yellow birch leaf area by 4 percent
and height by 8 percent. The chloro-
tic leaf stippling, characteristic of
ozone symptoms on leaves, was not af-
fected by acid rain treatments. The
sulfur dioxide response of these hard-
wood species seedlings was unclear.
Ongoing work will evaluate atmospheric
deposition effects on root and top
growth of hardwood seedlings, includ-
ing drought interaction. Atmospheric
deposition effects on photosynthesis,
water relations, and carbohydrate re-
serves will also be examined.
WESTERN CONIFEROUS FORESTS
Cloud Chemistry
A study of cloud chemistry and S04 and
N03 deposition in the Rocky Mountains
of Colorado found that, during the
summer months, deposition from clouds
was of the same magnitude as that from
precipitation, and greater than that
from dry deposition. A few cloud
events sampled during the study period
showed pH values similar to those for
the northeastern United States. How-
ever, on average, the cloud samples
from the Rockies were ten times less
acidic than cloud sample values repor-
ted for the Northeast. The study
demonstrated that accurate estimates
of acidic deposition to high elevation
forests in the West cannot be achieved
without determining the contribution
from cloud deposition.
Acid Hist and Foliar Leaching
For solution-cultured Douglas-fir see-
dlings with intermediate nutrient
availability (0.1 x full strength nu-
trient solution), foliar leaching was
higher for pH 3.1 acid mist exposures
than for pH 5.6. However, the amount
of nutrients removed was small re-
lative to daily root uptake rates.
None of the seedlings exposed to 24
low-pH fog events showed measurable
deficiency symptoms or reductions in
either biomas production or foliar
nutrient concentration.
Ponderosa Pine Growth Trends
A study of ponderosa pine increment
cores from 56 mixed conifer stands
throughout the Sierra Nevada found no
evidence of recent, large-scale
regional growth reduction. Regional-
ly, precipitation is the main variable
influncing growth rates. Some sites
in the southern Sierra Nevada showed
recent reduced growth rates correlated
with foliar ozone damage.
EASTERN SPRUCE-FIR FORESTS
High Elevation -- North
A 100 percent mapping of dead spruce
and fir for all the high elevation
forests in the northeast has been com-
pleted. Results indicate that, at
elevations over 800 meters (2,600
feet) in the Adirondacks, Green, and
White Mountains, red spruce mortality
in the past 25 years has greatly
reduced the number of trees. There is
a decreasing gradient in damage from
west-to-east with several mountains in
the Adirondacks having 50 percent or
more standing dead trees. Percent
standing dead red spruce in the Green
Mountains is less than that in the
Adirondacks and less still in the
White Mountains. Mortality has occur-
red in stands of differing age and
disturbance history and there is high
variability in mortality from mountain
to mountain within each geographic
area. Current regeneration of spruce
in the Northeast appears to be within
normal stocking levels.
A region-wide abrupt reduction of
growth began in the early 1960s in
stands of differing age and distur-
bance history. This reduction in
growth seems to be associated with a
change in the historical climate/
growth relationship. An exception to
this region-wide phenomenon is Mount
46
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Moosilauke, where the growth decline
does not appear to be synchronous be-
cause starting dates vary from 1954 to
1980.
historical climate/growth relation-
ship. Regeneration is found at all
elevations, with abundance proportion-
al to overstory species composition.
High-Elevation -- South
Twenty-four percent of high elevation
spruce-fir forests in the southern
Appalachian Mountains have greater
than 70 percent standing dead timber.
This is accounted for, in part, by
balsam woolly adelgid-caused mortality
in Fraser fir. The percent standing
dead for red spruce alone ranges from
5 to 13 percent with no relationship
between elevation and mortality.
Crown condition (foliar thinning) and
growth reductions have been found to
be the only important indicators of
poor red spruce health in the southern
Appalachians. At high elevations
there is evidence of an unusual reduc-
tion in radial increment that has been
associated with a breakdown of the
Winter Injury
It has been hypothesized that a fer-
tilization effect due to increased
nitrogen deposition might play a role
in high elevation spruce decline by
reducing frost hardiness and thus
resulting in increased winter injury.
However, experimental work has shown
that nitrogen fertilization does not
reduce frost hardiness in red spruce.
Under experimental conditions, one
study did reveal that exposure to
ozone resulted in delayed development
of frost hardiness in red spruce see-
dlings, while a separate study found
delayed frost hardiness following ex-
posure to simulated acidic cloud
water.
MAJOR DELIVERABLES - CROPS AND FORESTS
DELIVERABLE
DATE
SIGNIFICANCE
Evaluation of the effects
of ambient levels of ozone
for various crop species in
several locations in the
U.S. through studies using
the antioxidant, EDU, which
may protect plants from
ozone injury when used as a
foliar spray or soil
drench.
Late 1989
The use of an antioxidant may
provide an alternative methodol
ogy to open top chambers for in
vestigating the effects of ambi
ent ozone on crop production.
When EDU and open-top chambers
are used in combination, possi-
ble "chamber effects" and/or
"EDU" effects can be examined.
47
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DELIVERABLE
DATE
SIGNIFICANCE
Publication of the results Mid-1989
of an international cooper-
ative experiment in which
similar experimental proto-
col was used to evaluate
the effects of ambient lev-
els of ozone in ten differ-
ent countries on visible
injury, growth and yield of
the same crop species. Two
different sites in the U.S.
participated in the 1988
experiment.
Determination of the role Mid-1990
of free-radical oxygen
scavenging enzymes in pro-
tecting plants against
ozone injury through the
measurements of three of
such enzymes in ozone-
treated and untreated
plants and through studies
of biotypes with geneti-
cally induced differences
in these enzymes.
Differences in ozone sen- Mid-1990
sitivity will be examined
for several soybean culti-
vars under varying short-
term ozone profiles by
measuring gas exchange and
free-radical scavenging.
Further investigation of Mid-1990
the effect of acidic rain
on the structures, proces-
ses, temporal relationship,
and dynamics of pollination
and seed set in corn.
This first year of international
cooperation was meant to demon-
strate the interest in and fea-
sibility of conducting coordi-
nated and integrated experiments
on an international scale to ev-
aluate crop loss from air pol-
lutants.
Will provide information on the
possible mechanism by which
ozone damages plants.
Possible mechanisms of genetic
tolerance to ozone will be
determined along with the in-
fluence of different exposure
dynamics.
Will provide additional informa-
tion to evaluate preliminary
results that suggest that acidic
rain may reduce the yield of
field corn by affecting repro-
duction processes when the plant
is under stress by other fac-
tors.
48
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DELIVERABLE
DATE
SIGNIFICANCE
Quantification of changes
in freezing resistance of
citrus and avocado plants
following exposure to
chronic levels of ozone and
acidic rain in a field
study.
Early 1990 Provides information in an area
where there are significant gaps
in the knowledge base; that is,
effects of pollutant combina-
tions on perennial tree fruit
crops. Also complements work
being done in the forest re-
sponse program.
Assessment of the possible Mid-1990
interactive effects of
ozone and elevated carbon
dioxide levels on several
field-grown soybean cul-
tivars through measurements
of plant water relations
and photosynthate partiti-
oning.
Publication describing the Mid-1989
effects of acidic rain on
soil fauna in corn and
soybean fields in different
locations and with differ-
ent soil types.
Examination of the effects Early 1990
of ambient levels of ozone
and sulfur dioxide on wa-
termelon in the indus-trial
midwest where pollutant
levels are generally high.
Investigation of fungal and Early 1990
bacterial disease progres-
sion in celery and lettuce
exposed to acidic fog.
Examines the possible repercus-
sions of one aspect of global
climate change (elevated carbon
dioxide) in combination with
current levels of ozone on an
important crop plant and pos-
sible genetic differences in the
response to such change. Few
studies have examined this
combination of pollutants,
although both are by-products of
fossil fuel combustion.
Provides information on the
possible indirect effects of
acidic deposition on annual
crops through impacts on bene-
ficial and detrimental soil
organisms.
Will aid in the determination of
the cause for the foliar injury
and yield decreases recently
observed in watermelons in
Indiana.
Provides information to estimate
the influence of acidic fog on
disease management in California
crops exposed to winter fogs
having high acidity levels.
49
-------
DELIVERABLE
DATE
SIGNIFICANCE
Completion of a field study
to determine the relative
impact of ozone on soybean
physiology and yield when
chronic exposures occur
during different growth
stages.
Results of phytotron stud-
ies to determine the impor-
tance of peak ozone epi-
sodes on plant response.
Further investigations of
possible mechanisms of the
direct effects of ozone on
Geranium reproduction.
Completion of greenhouse
studies of tomato plants to
determine the effect of
simulated rain acidity and
duration of rain event on
visible injury, vegetative
growth, and fruit numbers.
Evaluation of near real-
time variations, peak
pollutant concentrations,
and physical
characteristics of the high
elevation cloud/atmospheric
environment.
Electronically accessible
monthly summaries of exist-
ing monitoring data (1978-
1986) for the Ohio Valley
corridor (including quality
assurance information).
Early 1989 Determination of ozone-sensitive
growth stages in soybean to
assess the importance of tem-
poral aspects of pollutant
exposures.
Early 1990 Will help to separate the influ-
ence of short-term exposures to
high levels of ozone versus
long-term exposures at lower
concentrations. Results from
the above two studies may
influence the selection of
control strategies to reduce
ozone damage to crops.
Mid-1989 Provides information on possible
effects of ozone on reproductive
processes in plants.
Early 1989 Provides needed information on
the importance of rainfall
duration in affecting plant
response to rainfall acidity
since previous experimental
designs have principally consis-
ted of short-duration rain
events.
Early 1990 Near real-time cloud chemistry
characterization will be useful
in assessing signifcance of
cloud processes in deposition
and resulting canopy interac-
tions.
Early 1989 Will provide summaries from
forested areas at monthly in-
tervals which may be more
meaningful for studies of forest
effects than hourly averages or
7-hour means.
50
-------
DELIVERABLE
DATE
SIGNIFICANCE
Relative sensitivities of Early 1989
10 eastern hardwood species
to S02, 03, and acid pre-
cipitation.
Interim report on rate of Late 1989
change in sugar maple con-
dition ratings for years
1988-1990 on plots in
Ontario, Quebec, New
Brunswick, ME, MI, NH, NY,
VT, MA, and WI.
Inventory of geographic Early 1990
variation in visual crown
symptoms and frequency of
occurence for red spruce
and balsam fir in the
Northeast. Vigor ratings
based on (1) needle reten-
tion, (2) FDR damage clas-
ses, and (3) American
Foliage and Tree Vigor
Rating.
Interim report quantifying Mid-1990
loblolly, slash, and short-
leaf pine response to acid-
ic precipitation and ozone.
Evaluation of effects of Mid- and
acidic deposition on forest Late 1990
nutrient cycling (slash
pine and commercial red
spruce).
Seedling response under
controlled conditions will
provide means to evaluate
response of trees along depo-
sition gradients in the North-
east.
Will evaluate the influence of
S04 and sugaring (production of
maple syrup or sugar) on report-
ed maple decline.
Will provide information on the
extent and magnitude of reported
decline in NY, VT, NH, ME, MA,
and WV.
Will provide information on the
role of airborne pollutants in
forest health (growth, nutri-
tion, and physiology).
Will address two proposed
mechanisms by which sulfur
and/or nitrogen pollutants might
affect forests: (1) increased
leaching of foliar nutrients and
(2) increased leaching of soil
nutrients.
51
-------
DELIVERABLE
DATE
SIGNIFICANCE
Evaluation of the effect of Mid-1990
ambient ozone (between 20
and 134 ppb) and water
stress on net carbon ex-
change and growth of 11-
year old loblolly pine
branches using a branch
cuvette fumigation system.
Evaluation of relationship Early 1990
of sulfur, nitrogen, and
acidity to frost hardiness
of red spruce in the field
along with model relating
deposition to risk of frost
injury for red spruce in
the eastern United States.
Interim report assessing Early 1990
long-term effect of
precipitation chemistry on
soil chemistry (high eleva-
tion spruce-fir).
Dose/response function Mid-1990
comparing effects of ozone
and acid rain on photosyn-
thesis and growth of red
spruce seedlings and
saplings.
Interim report comparing Early 1990
phenological, physiolog-
ical, biochemical, and
morphological changes in
foliage for controlled
field experiments and un-
controlled field sites.
Report on the response of Mid-1990
branch export of photosyn-
thate to alternative depo-
sition scenarios for red
spruce, loblolly pine, and
ponderosa pine.
Use of branch chambers will
provide a link between responses
observed in seedling exposure
studies and those observed on
established trees in the field.
Will adress the effect of sulfur
and/or nitrogen pollution on red
spruce through the mechanism of
delayed cold hardening or early
break in dormancy.
Will address the effect of
sulfur and/or nitrogen pollution
on spruce-fir through the
mechanism of direct toxicity to
roots by mobilized metals in
acidified soil water.
Will address the effect of
airborne pollutants on red
spruce through the mechanism of
altered carbon allocation.
Will identify alterations in
seasonal patterns of red spruce
physiology that may be caused by
exposure to ozone and/or acidic
precipitation.
The report will synthesize the
foliar effect of acidic deposi-
tion and examine sensitivity to
pollution.
52
-------
DELIVERABLE
DATE
SIGNIFICANCE
Sensitivity ranking of five
western conifers to: (1)
simulated acid fog/ozone
exposure in seasonal inter-
action, and (2) simulated
S02 exposure.
Evaluation of extent and
magnitude of recent changes
in forest condition.
Evaluation of the role of
non-air pollution factors
in growth reduction and
visible decline.
Early 1990
Quantitative estimates of
seedling respone to sulfur,
nitrogen, and associated
pollutants at ambient con-
ditions.
Evaluation of the role of
sulfur, nitrogen, and as-
sociated pollutants in
forest damage.
Interim reports on
physiological and biomass
response of red spruce
seedlings to acidic cloud
interception and/or ozone
using field exposure cham-
bers at Whitetop Mountain,
VA.
Early 1990
Early 1990
Mid-1989
Late 1989
Late 1989
and early
1990
Will address the effect of
airborne pollutants on western
conifers through the mechanism
of altered carbon allocation and
leaching of foliar nutrients.
Will address correlative
assocations between natural
factors such as climatic vari-
ation, stand maturation, and
known pollutant deposition
patterns.
Will address whether correlative
associations between patterns of
forest damage and patterns of
pollutant exposure can reason-
ably be explained by natural
ecological and environmental
variables.
Will integrate and interpret
results of various controlled
exposure experiments on forest
tree seedlings.
This Forest Response Program
analysis will compare response
of species and/or regions and
evaluate hypothesized mechanisms
of decline (soil-mediated,
foliar leaching, altered carbon
allocation, and winter injury).
Chronic ozone exposure and
deposition of acidic cloud water
increase with elevation in the
Appalachian Mountains. These
factors have been hypothesized
as causal mechanisms for decline
and mortality of red spruce at
high elevations.
53
-------
DELIVERABLE DATE SIGNIFICANCE
Interim report on com- Early 1990 Use of branch chambers will
parison of the response of provide a link between effects
seedlings and mature observed in seedling exposure
branches of ponderosa pine studies and those observed on
and red spruce to air pol- mature trees in the field.
lution.
54
-------
AQUATIC EFFECTS
1988 RESEARCH HIGHLIGHTS
Chemical Status of Surface Waters
The National Stream Survey-Phase I
(NSS-I) was conducted in 1986 in the
Mid-Atlantic and Southeast regions of
the United States as part of the Na-
tional Surface Water Survey. The NSS-
I focused on regions of the United
States where, on a national scale, (1)
acidic deposition rates are relatively
high, (2) the numbers of acidic
streams and streams with low acid neu-
tralizing capacity (ANC) were expected
to be highest, and (3) the dominant
aquatic resource was streams rather
than lakes. Spring baseflow chemistry
was measured in a probability sample
of 504 stream reaches comprising ap-
proximately 1 percent of the total
target population. This design allows
population estimates to be made re-
garding characteristics of that popu-
lation (64,300 reaches or 224,000 km
total length). Nine subregions within
the Mid-Atlantic and Southeast were
surveyed (Figure VI-1). For the
FIGURE VI-1. Regions and Subregions Surveyed in Phase I of the National
Stream Survey
Northern
Appalachians (2Cn)
Valley and Ridge (2Bn)
Poconos/CatskillsdD)
Southern Blue Ridge (2As)
(Pilot Study)
Mid-Atlantic
Coastal Plain (3B)
Southern Appalachians (2X)
-------
purpose of data analysis, results from
similar subregions were also combined
to provide estimates for stream reach-
es in the Interior Mid-Atlantic and
Interior Southeast.
The resource targeted within these
regions included all streams with
drainage areas less than 60 mi2
(155km2), but which are large enough
to be represented as blue lines on
l:250,000-scale USGS topographic maps.
Most streams in this size range have
baseflow channel widths between 1 and
8 meters and depths between 7 and 50
centimeters. The target population
was further restricted to exclude
stream reaches with highly urbanized
drainages, tidal impacts, no measur-
able flow, and those which are acidic
due to acid mine drainage. The NSS-I
estimates presented below are made
from 478 sample reaches, representing
this "refined" target population of
approximately 57,000 reaches (201,000
km).
Acid neutralizing capacity is commonly
used to examine the susceptibility of
surface waters to acidification and
was a key variable measured in the
study. Regional and subregional ANC
differences during spring baseflow
were compared using the estimated per-
centages of stream length with ANC
concentrations equal to or less than
several reference values. Although
the survey can be used to provide es-
timates for any reference value, four
values and their definitions, used
TABLE VI-1. Population Estimates of the Percentage (Based on Stream
Reach Length) of Target Reaches1 with Spring Baseflow ANC Less than the
Reference Values2-3-4
Subregion/Region (Code)
Poconos/Catskills (ID)
N. Appalachians (2Cn)
Valley & Ridge (2Bn)
Mid-Atlantic Coastal Plain (3B)
S. Blue Ridge (2As)
Piedmont (3A)
S. Appalachians (2X)
Ozarks/Ouchitas (2D)
Florida (3C)
Interior Mid-Atlantic 5
Interior Southeast 6
Mid-Atlantic 7
Southeast
Total
' Target population is defined
2 Calculated using linear interc
Total Length (km)
15,144 (1,912)
21,738 (2,746)
32,687 (4,492)
40,2% (5,799)
9,036 (960)
33531 (4,4(J2)
21,892 (2,807)
22,480 (2307)
3,848 (678)
69369 (5,601)
86,939 (5,871)
109,865 (8,063)
90,787 (5,910)
200,652 (9,9%)
in the text.
tolation between upper and
ANC (tieq/L)
SO
3.6 (1.8)
7.0 (33)
0.8 (0.6)
6.3 (2.9)
03 03)
12.0 4.1)
3.3 1.4)
0.1 0.1)
4.4 1.4)
0.6 0.2)
2.7 (0.8)
lower sampling sites
s50
10.6 (3.3)
17.1 (4.2)
63 (3.0)
23.9 (6.6)
7.8 (2.8)
7.1 (3.9)
33 (3.0)
0.9 (0.6)
61.2 (14)
10.7 (2.4)
4.7 (1-5)
153 (2.8)
7.1 (1.7)
11.7 (1.7)
fSlOO S200
23.8 6.2 36.2 7.3)
31.9 7.1 593 10)
14.8 6.3 39.2 10)
27.0 6.9 52.3 11)
44.1 8.3 78.4 (10)
21.0 5.9 40.4 (83)
12.7 5.1 28.0 (8.0)
19.2 53 67.1 (11)
69.4 (14.2) 76.4 (15)
22.1 (4.1) 44.9 6.2
20.8 (3.1) 48.1 4.9
23.9 (3.7) 47.6 5.6
22.9 (3.1) 49.3 4.8
23.4 (2.4) 48.4 (3.8)
on the reach (see text for explanation). Standard
errors are shown in parentheses. The 95 percent upper confidence limit can be obtained by multiplying the standard error by
1.645 and adding the result to the estimate.
3 Population estimates of the percentage of stream length with ANC > 200 ueq/L can be calculated by subtracting from 100% the
percentage with ANC S200 u«q/L (the stated reference value).
This table excludes the streams whose acidity was proven to be attributed to acid mine drainage.
The Interior Mid-Alantic subregions are ID, 2Cn, and 2Bn.
The Interior Southeast subregions are 2As, 3A, 2X, and 2D.
The Mid-Alantic includes the Interior Mid-Atlantic and subregion 3B.
The Southeast includes the Interior Southeast and subregion 3C
56
-------
TABLE VI-2. Population Estimates of the Percentage (Based on Stream
Reach Length) of Target Reaches1 with Spring Baseflow pH Less than the
Reference Values2-3
Subrcgion/Rcgion (Code)
Total Length (km)
PH
Total
200,652 (9,996)
S5.0
2.9 (0.8)
Poconos/Catskills (ID)
N. Appalachians (2Cn)
Valley & Ridge (2Bn)
Mid-Atlantic Coastal Plain (3B)
S. Blue Ridge (2As)
Piedmont (3A)
S. Appalachians (2X)
Ozarks/Ouchitas (2D)
Florida (3C)
Interior Mid-Atlantic 4
Interior Southeast 5
Mid-Atlantic 6
Southeast 7
15,144 (1,912)
21,738 (2,746)
32,687 (4,492)
40,296 (5,799)
9,036 (960)
33,531 (4,402)
21,892 (2,807)
22,480 (2,507)
3,848 (678)
69,569 (5,601)
86,939 (5,871)
109,865 (8,063)
90,787 (5,910)
3.6 ri.9)
6.6 (3.2)
0.8 (0.8)
7.8 (3.3)
<1.0 (-
< 1.0 (-
200 jieq/L are gen-
erally agreed not to be sensitive to
acidification.
The percentage of the total target
stream reach length with ANC or pH
below a given reference value, as
shown in Tables VI-1 and VI-2, is es-
timated by linear interpolation bet-
ween upstream and downstream ends
(nodes) of sample reaches. These es-
timates depend upon the difference
between upstream and downstream
chemistry, the reach length, and the
population weighting factor for each
sample reach. Therefore, population
percentages based on interpolation do
not necessarily fall between those
describing the percentage (by number)
of upstream and downstream reach
nodes. For example, the estimated
percentage of stream reach length
(based on the interpolated value) in
the Valley and Ridge (2Bn) with ANC <0
is 0.8. Based on numbers using the
upper and lower node samples, however,
the percentages of acidic reaches are
5 percent and <1 percent, respective-
ly.
Of the total estimated target length
of eastern reaches, an estimated 48
57
-------
percent (97,000 km) had ANC <200
(xeq/L, 11.7 percent (23,000 km) had
ANC <50 u.eq/L, and 2.7 percent had ANC
<0 fieq/L (5,400 km) (Table VI-1). The
results also indicate notable differ-
ences between the Mid-Atlantic and
Southeast with respect to the percent-
age of stream reach length that was
acidic and that had ANC <50 p,eq/L.
Less than 1 percent of the surveyed
acidic streams were in the surveyed
portions of the Southeast, except in
Florida, where most streams (including
acidic streams) also contained high
concentrations of dissolved organic
carbon. The length of stream reaches
that are acidic during spring baseflow
was estimated to be 4.4 percent in the
Mid-Atlantic and 0.6 percent in the
Southeast. Nearly twice the percent-
age of stream length in the Mid-Atlan-
tic (15.5 percent, 17,067 km) had ANC
<50 neq/L, compared to the Southeast
where 7.1 percent (6,420 km) had ANC
in this category. Estimates for ANC
also varied among subregions. The
lowest percentage of acidic reach
length was found for the Southern Ap-
palachians and the highest for the
Northern Appalachians and Florida.
The estimated 2.7 percent (5400 km
total length) of the streams in the
NSS population that were acidic are of
special interest to NAPAP. Not in-
cluded in Table VI-1 are an additional
4600 km of acidic streams with high
sulfate concentrations and evidence of
mining activity. It is believed that
mining activity is the source of the
sulfate which is the major acid anion
in these streams.
In the Florida Subregion, organic
acids, presumably derived from decom-
position, are surmised to play a dom-
inant role in controlling the acidity
of these streams. The acidic stream
reaches observed there were largely
low in sulfate (mean = 12 p-eq/L) and
high in DOC (mean = 77 mg/L). Organic
anions (estimated from the Oliver mod-
el) dominated the anion balances in
these reaches.
Nitrate, sulfate, and naturally oc-
curring organic acids are substantial
contributors to the strong acid anion
composition of streams in the Mid-At-
lantic Coastal Plain.
In contrast to these findings in
Florida and the Coastal Plain, sulfate
is the major acid anion in the acidic
reaches for the three Interior Mid-
Atlantic subregions. These acidic
streams were observed in upland, for-
ested drainages of less than 20 km2
and their pH ranged from 4.2 to 5.3.
Sulfate was found at relatively high
concentrations (mean = 153 |xeq/L);
concentrations of chloride (mean = 22
jxeq/L), organic anion (mean = 14
u.eq/L) and nitrate (mean = 8.7 M-eq/L)
were low and contribute only a small
fraction of the total anion concentra-
tion. Thus, sulfate is by far the
dominant acid anion in these acidic
streams. In most cases, sulfate con-
centrations exceed the sum of base
cation concentrations (after sea-salt
correction), providing strong evidence
for the presence of sulfuric acid.
The predicted steady-state streamwater
sulfate concentrations in these three
subregions, assuming only atmospheric
deposition as a source, range from 158
jxeq/L in the Poconos/Catskills to 214
|ieq/L in the Valley and Ridge sub-
region. Given the mean observed sul-
fate concentration of only 153 jieq/L
in these acidic streams, it is unlike-
ly that substantial watershed (non-
atmospheric) sources of sulfate were
present. Therefore, acidic deposition
is likely to provide the majority of
sulfate to these streams.
Differences in median values for ANC,
pH, and sulfate among subregions and
regions were also evident (Figure VI-
2). In general, upper nodes had lower
median ANC values than did lower
nodes, while sulfate and pH differen-
ces between the nodes were relatively
small. Stream water sulfate concen-
trations were markedly higher in the
four Mid-Atlantic subregions (medians
from 125 to 138 u.eq/L) than in the
58
-------
FIGURE VI-2. Population Estimates for Median Acid Neutralizing Capacity,
pH, and Sulfate Concentrations at Upper and Lower Sampling Sites (Nodes)
in Stream Reaches for the National Stream Survey - Phase I. Data are for
the target population of reaches as defined in the text. Median values for
Florida (3C) are based on a special subset of streams with low acid neutraliz-
ing capacity and are not directly comparable to those for other subregions
(see Kaufmann et al. 1988).
400-
200-
300-
200-
100-
Upper node I
Acid Neutralizing Capacity (jteq/L) Lower node|
n^
pH
Sulfate (/ieq/L)
Upper nodel
Lower nodel
I
1D
2Cn 2Bn 3B 2AS 3A
2X
2D
3C
Mid-Atlantic
Southeast
five Southeast subregions (10 to
71 u.eq /L).
The relationship between median stream
sulfate concentrations and sulfate
deposition rates was examined across
the nine subregions in a manner previ-
ously done for the National Lake Sur-
vey. For this analysis, those surface
waters with the largest sources of
terrestrial sulfate were excluded.
For streams in the Mid-Atlantic Sub-
regions (ID, 2Cn, 2Bn, 3B) and in the
Ozarks/Ouchitas (2D), the regional
pattern of increasing surface water
sulfate concentration associated with
increasing atmospheric sulfate load-
ings closely tracks that observed for
lakes in the West, Upper Midwest, and
East (Figure VI-3). The comparison
with the lake data indicates that
streams in the Southeast have lower
sulfate concentrations than expected,
given their sulfate deposition rates.
This observation is consistent with
other research showing substantial
sulfate retention in some parts of the
Southeast.
o Data from the National Surface
Water Survey (NSWS) indicate that reg-
ional median sulfate concentrations in
lakes reflect estimated median region-
al wet sulfur deposition levels in
northern and western parts of North
America. It is inferred from these
data that surface water sulfate has
increased since pre-industrial times
in a manner roughly similar to changes
in sulfur deposition in these areas.
59
-------
FIGURE VI-3. Relationship Between Median Wet Sulfate Deposition (1980-
1984) and Median Sulfate Concentration in Surface Waters With SO4^<400
M-eq/L in Subregions for the National Surface Water Survey. This analysis is
based on the target population as defined in the text, except that those
-
streams with S04 >400 (xeq/L were eliminated for this analysis. Wet SO,
deposition rates are derived from Wampler and Olsen (see Aquatic Effects
Publications, 1987 NAPAP Annual Report).
2504
o- 200
3 150-
LJ
o 100
ir
10
50-
NLS Subregions NSS-I Subregions
<5
2BN
2AS
LEGEND
. NSS-! SUBREGIONS
ONLS SUBREGIONS
WET SULFATE DEPOSITION (g m~2yr~')
Concerning within-lake and within-
stream chemical relationships, examin-
ation of NSWS data on the total popu-
lation of lakes and streams does not
show a relationship between surface
water sulfate and acidity. However,
other analyses on a subset or subpopu-
lation of low alkalinity lakes and
streams show that sulfur deposition
has influenced their chemistry and
suggest that their acidity has in-
creased. At least two of the NAPAP
State of Science/Technology reports
will examine approaches to quantifying
the subpopulations of lakes and
streams which respond to sulfur depo-
sition by a change in acidity and es-
timating the magnitude and intensity
of this response.
o The Episodic Response Project was
initiated to examine episodic acidifi-
cation and associated biological ef-
fects in streams of the Northern Ap-
palachian Plateau of Pennsylvania and
the Catskills and Adirondacks of New
York. As part of the development of
the project design, a two-box mixing
model was used to estimate the poten-
tial influence of episodic acidifica-
tion on regional estimates of surface
water chemistry. Together with re-
gional chemistry and deposition data,
the results from application of the
preliminary model indicated that acid-
ic episodes are likely to be a chemi-
cally important regional phenomenon.
Population estimates of the total pro-
portion of acidic stream reaches would
6C
-------
increase by 40-640 percent in six sub-
regions of the eastern United States
if episodes are taken into account.
In addition, data from a small sample
of lakes in the Adirondacks show that
fall "index" ANC is an excellent pre-
dictor of the minimum episodic ANC
measured at the outlets of these lakes
during spring snowmelt. While 11 per-
cent of the Adirondack lakes were es-
timated to be acidic at fall overturn
based on National Lake Survey data, a
preliminary linear regression model
predicted that more than 35 percent
would have been acidic at their out-
lets during the spring of 1986.
o Episodic acidification of surface
waters in the Emerald Lake, California
watershed has occurred following in-
tense summer rainstorms. During these
episodes surface water ANC has been
reduced to zero. Similarly, ionic
pulses have been detected during early
spring snowmelt in the inflow streams
concurrent with increases in concen-
trations of nitrate and sulfate.
Factors Controlling Surface Water
Response
o Chemical weathering of minerals is
a major process that provides long-
term neutralization of acidic deposi-
tion. Organic compounds have been
hypothesized to control weathering
rates of primary minerals (and release
rates of base cations) either by di-
rect complexation reactions or indi-
rectly by influencing solution pH. As
part of the Watershed Manipulation
Project in Maine, a series of labora-
tory studies has been completed. The
studies have demonstrated that neither
pH nor concentration of oxalic acid (a
metal-binding organic compound) influ-
ence the weathering rates of two pri- .
mary minerals, oligoclase and tremo-
lite, found in low weathering environ-
ments. Extrapolation of these results
to the field is premature at this
time, but the research suggests that
acidic deposition may have minimal
effects on the weathering rate of (and
rate of base cation supply from) these
pure minerals. Nonetheless, mineral
weathering does neutralize incoming
precipitation acidity and adds to the
alkalinity of the surface water.
o Alteration of precipitation chemis-
try by mature boreal conifer and hard-
wood forest canopies and by forest
soil is being examined as part of an
ongoing study in Isle Royale, Northern
Michigan. The forest canopy signifi-
cantly increased the concentration of
calcium, magnesium, and potassium ions
in throughfall and decreased the con-
centration of hydrogen ion beneath
aspen-birch. For both forest types,
concentrations of calcium, magnesium,
and sodium ions and sulfate signifi-
cantly increased and nitrate decreased
in soil solution, relative to their
concentrations in precipitation.
Within the soil ecosystem, potassium
ion, nitrate, and hydrogen ion were
strongly conserved. Concentration of
soil solution sulfate is higher, and
its flux two-to threefold greater un-
der conifers than hardwoods. This
suggests the possibility that boreal
conifer forests may be more suscept-
ible than hardwood forests to cation
leaching by mobile anions such as sul-
fate from atmospheric inputs, and may
therefore contribute more base cations
to surface waters.
o Research at Loch Vale Watershed in
the Rocky Mountains has focused on
tracing the hydro logic pathways of
melting snow and summer rainstorms and
on identifying crucial watershed-med-
iated processes along those pathways.
Results indicate that organic acids in
forest soils mobilize surprisingly
high concentrations of potentially
toxic aluminum. This research is also
providing evidence that mineral
weathering processes may be highly
important in ameliorating episodic
responses to acidic deposition. On an
annual basis, much of the water moving
through the watershed is related to
the spring melting of the snowpack.
It now appears that mineral weathering
is active even in this early spring
61
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period. Further evidence of the im-
portance of weathering is provided by
summertime studies. Summer thunder-
storms are, in general, much more
acidic than winter snows and could
cause episodes of acidic streamflow.
To investigate this potential, resear-
chers collected samples of streamwater
runoff from a summer thunderstorm in
the upper part of the watershed, which
is above the tree line and is the area
of the drainage that is most suscep-
tible to acidic inputs. This alpine
stream passes over bedrock and through
talus fields with very little soil
contact. The sampled stream runoff
was almost 100 times less acidic than
the rain water itself, indicating that
weathering of granitic bedrock can
substantially influence the acidity of
storm water flowing into receiving
surface waters.
Verifying Rates of Change in Surface
Water Chemistry
o Sampling strategies for the detec-
tion of long-term trends in surface
water acidification were analyzed as
part of the Temporally Integrated
Monitoring of Ecosystems Project.
Several statistical techniques were
tested on the basis of their power of
trend detection for data sets typical
of long-term monitoring programs deal-
ing with acidic deposition effects.
The performance of seven tests was
compared over a range of conditions
for eight statistical characteristics
of temporal data sets, e.g., seasonal
pattern of mean, trend magnitude, and
lag-one autocorrelation coefficients.
Detectable change in regional means
was also examined for various combina-
tions of numbers of sites, spatial
correlation among sites, and length of
record for various levels of power and
significance. These results reduce
uncertainty in monitoring network de-
sign for surface water acidification,
by specifying the probability of trend
detection for various combinations of
numbers of sites and length of record,
given estimated temporal variances for
sites and constituents of interest.
For example, for drainage lakes in the
Northeast, the level of detectable
change in regional ANC means over 10
years using four lakes with an average
spatial correlation of 0.2 is 23
M-eq/L, given that the probabilities of
making Types I and II errors are both
only 0.1. With the same assumptions,
if 16 lakes are used, the detectable
change is 17 jxeq/L. For seepage lakes
in the Upper Midwest, temporal vari-
ance is higher, and the equivalent
levels of detectable change are 36
fieq/L for four lakes and 27 |xeq/L for
16 lakes.
o Results of a detailed study of
diatom remains in sediments of 30
lakes in the Sierra Nevada were used
to establish a relationship between
diatom communities and pH. This "cal-
ibration set" was then used to recon-
struct the pH (using Pb210 from a
"short" sediment core) and alkalinity
history of Emerald Lake, in the
Sequoia National Park, from 1825 to
the present. Over the 150-year period
the estimated pH variance was 6.1-6.6,
with no obvious trends. Alkalinity
ranged from 40-80 neq/L, nearly within
the current range of alkalinities re-
corded for Emerald Lake. Thus, these
data show no apparent long-term trend
toward chronic acidification of Emer-
ald Lake.
Biological Effects
o Forty-nine lakes in the Upper
Peninsula of Michigan (pH 4.4 to 8.2)
were surveyed in summer 1987 to eval-
uate the status of fish communities in
the region relative to potential ef-
fects from acidic deposition. The
sampled lakes are all >4 ha in size
and >1.5 m deep and had no major anth-
ropogenic watershed disturbances or
fish stocking likely to confound cor-
relative analyses of fish population
status and lake acidity. These lakes
are a subset of those sampled for
water chemistry in fall 1984 as part
of Phase II of the Eastern Lake Sur-
62
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vey. One or more species of fish were
caught in 47 of the 49 lakes, which,
when extrapolated to the target popu-
lation, represents an estimated 99.4
percent of the lakes in the region.
Yellow perch, which are quite acid
tolerant and are commonly caught in
waters with pH levels as low as 4.5,
were the most common species, caught
in 31 of the target lakes. Several
minnow and darter species were notably
absent from lakes with low pH (<5.7-
6.0), perhaps reflecting an intoler-
ance of acidic conditions. This study
provides a comprehensive survey of the
present-day status of fish communities
in a region of the country with a rel-
atively high frequency of acidic lakes
(an estimated 9.8 percent of the lakes
have ANC <0) and with little existing
data on fish community composition in
lakes potentially sensitive to acidic
deposition.
o Brood and duckling survival of
ring-necked ducks was examined in wet-
land areas of Maine having a range of
alkalinity and pH. Brood survival
does not appear to be related to wet-
land pH or alkalinity. While duckling
survival also did not differ among
wetlands with high and low alkalinity,
it does appear to be influenced by pH.
The daily survival rate of ducklings
was lower on low-pH (<6.0) wetlands
than on high-pH (>6.1) wetlands.
Older ducklings (25-45 days old) ap-
peared to be the most sensitive, hav-
ing both the lowest survival rate when
in wetlands with pH <5.5 and the high-
est survival rate when in wetlands
with pH >6.5. The response of older
ducklings on low-pH wetlands is most
likely due to the effects of low pH on
the invertebrate food source. The
only difference found among the wet-
lands that could affect survival seems
to be the quantity and quality of in- .
vertebrate foods. Diets of ducklings
from high-pH wetlands were more di-
verse than those of ducklings on low-
pH wetlands, which consumed smaller
quantities of invertebrate food from
fewer invertebrate taxa. When species
diversity is low, ducklings may be
forced to feed on less nutritious or
more mobile species, and may spend
more time and energy foraging to ob-
tain sufficient nutrients for growth
and survival. The effect of acidic
deposition on the pH of wetlands is
not clear at this time.
o Experiments performed by adding
acids (nitric, sulfuric, and
hydrochloric) and nutrients (phosph-
ate) to large replicate bags suspended
in Emerald Lake showed population
changes in a number of zooplankton
species. Two genera, Diaptomus and
Daphm'a, were eliminated from the bags
in which the pH was lowered to 4.4.
Other species, including Bosmina and
Keratella, did better at intermediate
pH levels (pH 5.2), which may indicate
that some competitive species had been
eliminated by the acid addition. Sim-
ilarly, experimental acidification of
stream channels showed that certain
benthic invertebrates which are eaten
by trout, e.g., Baetis, are adversely
affected by low pH, comparable to
those recorded in the outflow stream
during spring snowmelt. Increased
severity and frequency of episodic
acidification might, through the loss
of important dietary components, af-
fect trout growth and survival in
these food-limited systems.
o Completion of a second year of ex-
posure to pH 5.1 produced additional
changes in the biota of artificially
acidified Little Rock Lake, a seepage
lake in north-central Wisconsin.
Shifts in invertebrate organism abun-
dance have varied widely: upward and
downward; changed in the second but
not the first year of each pH incre-
ment (5.6 and 5.1); increased abun-
dance but stable diversity among daph-
nids as compared to stable abundance
and reduced diversity of rotifers.
Unexpectedly, the Mougeotia algal mat
and water transparency were reduced,
and the growth rate of fishes was in-
creased as compared to the previous
year, perhaps related to the unusually
warm and dry weather. Laboratory ex-
posure, in situ field exposure, and
63
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field population data are providing a
basis for comparison of various data
types for estimating the effects of
acidity on fish. All data indicate
rock bass and black crappie are more
vulnerable than largemouth bass and
yellow perch, relationships first in-
dicated by 30-day exposures of juven-
ile life stages. When comparing re-
sults from exposures of early-life
stages (embryos and larvae), in situ
data tend to overestimate and labora-
tory data to underestimate toxicity.
Field data indicate rock bass are the
most sensitive species and that acid
stress might be reducing over-winter
survival of young-of-the-year large-
mouth bass. Water column concentra-
tions of calcium, manganese, aluminum
and iron have increased. Lower bac-
terial numbers and microbial community
activity have been associated with
reduced decomposition of oak leaves.
Indirect Human Health Effects
o The effect of acidification on mer-
cury accumulation in yellow perch in-
habiting Little Rock Lake, Wisconsin,
is being studied. Mercury concentra-
tions in one-year old whole perch in-
creased in response to whole-lake
acidification from pH 6.1 to 5.6.
Mean body burdens of mercury in these
yellow perch were greater in the
lake's treatment basin than in the
reference basin. Acidification of the
treatment basin may have increased the
net production of methylmercury, the
form of mercury that is most readily
accumulated by fish. The influence of
a decrease in pH on the direct uptake
of methylmercury by fish remains
unclear.
Ecological Effects of Mitigation
o Analysis of liming data on ten
small lakes in New York has shown that
dose rate alone is the best predictor
of the initial dissolution efficiency
of limestone applications to mitigate
acidification in lakes. A number of
dissolution model parameters were
tested in this analysis. The study
also examined lake flushing rate,
mixing, and dissolution of calcite,
all of which influence the rate of
acidification. Dissolution rates
declined exponentially, reaching un-
detectable levels within 2-3 years
following treatment. Total limestone
dissolution efficiencies in these
lakes ranged from 17 to 59 percent,
comparable to levels observed in Scan-
dinavian lakes treated with similar
materials. In another study on miti-
gation, a Minnesota lake was treated
with five tons of powered limestone to
study the duration of neutralization
effects and ecological effects.
o Collection of baseline pretreatment
data including biology, chemistry, and
habitat characterization has been com-
pleted for stream studies in
Massachusetts, West Virginia, and Ten-
nessee. Stream liming will begin in
fall 1988 based on dose rates that
have already been calculated.
Forecasting Rates of Change in Surface
Water Chemistry
o The Direct/Delayed Response Project
is focusing on chronic sulfate deposi-
tion effects to determine the rate at
which average annual surface water ANC
might be expected to reach zero, given
various rates of sulfate deposition.
Forecasts are being made with three
watershed acidification models. As
part of this project, relative
contributions of in-lake alkalinity
generation to total basin alkalinity
budgets for drainage lakes in selected
regions of the eastern United States
were estimated using two independent
procedures. Projections from the two
methods are comparable and show that
for most drainage lakes in the
Northeast, Southern Blue Ridge
Province, and Upper Midwest, in-lake
alkalinity generation is a minor con-
tributor to net basin alkalinity
production. Regional assessments of
current or future effects of acidic
64
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deposition on surface water chemistry
in the Northeast and Southern Blue
Ridge Province, or in other areas
dominated by drainage lakes with high
watershed to lake area ratios, are not
seriously compromised by use of models
limited to consideration of terres-
trial processes. For areas such as
the Upper Midwest that contain high
proportions of seepage lakes, or for
lakes with long hydrologic residence
times, in-lake processes and hydraulic
influences must be considered. The
accuracy of acidification forecasts
will be enhanced by quantifying the
relative importance of internal alka-
linity generation to total basin alka-
linity budgets.
o Regional-scale estimates of runoff
are needed as input parameters in the
watershed acidification models being
used in the Direct/Delayed Response
Project to forecast surface water
acidification. Many of the sites
being examined in this project do not
have gauges installed, an important
component in obtaining runoff esti-
mates. Thus, to obtain regional es-
timates, interpolation methods must be
used for ungauged sites. An analysis
to quantify uncertainty associated
with interpolating runoff to specific
sites was conducted on 100 gauged
watersheds using a runoff contour map
by (1) hand interpolation to the
watershed outlet, (2) a computer
interpolation to the watershed outlet,
and (3) hand interpolation to the
watershed centroid. Interpolated
values were then compared to the ac-
tual gauged values. On the average,
interpolated values for runoff estima-
ted at basin outlets were slightly
less than gauged values. Results from
the hand interpolation method were not
significantly different from the com-
puter interpolation method. Addition-
ally, the absence of strong spatial
correlations or regional patterns in
the runoff interpolations indicated
that no regional biases were intro-
duced in the development of the con-
tour map. Runoff can be estimated, on
the average, to within approximately
15.0 percent of the measured value
using the three methods. These
results indicate that runoff contour
maps can be used in regional studies
to extrapolate runoff to ungauged sys-
tems with quantifiable uncertainty.
The analysis of uncertainty in this
component is one part of a more com-
prehensive uncertainty analysis
underway.
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MAJOR DELIVERABLES
DELIVERABLE
DATE
SIGNIFICANCE
Report on dynamic model Early 1990
forecasts for regional
changes in acid neutraliz-
ing capacity in streams in
the mid-Appalachians.
Acid-base status of streams Late 1988
in the eastern United
States—results of the
National Stream Survey.
Status and extent of acid Early 1989
mine drainage impacts and
internal sulfate sources in
the National Stream Survey
target population.
Geological controls on the Early 1990
acid-sensitivity of streams
in a number of subregions
of the eastern United
States.
Watershed factors control 1- Late 1989
ing water chemistry in
streams of the National
Stream Survey.
The report will provide a re-
gional forecast with quantifi-
able certainty of the rate of
change in acid neutralizing cap-
acity for surface waters in two
areas of the United States sus-
ceptible to acidic deposition.
Interprets regional distribution
of stream water chemistry as re-
lated to potential sources of
acidity and current hypotheses
on sulfate retention and delayed
effects of acidic deposition.
Assess the location, number, and
combined length of streams af-
fected by acid mine drainage
within the nine National Stream
Survey subregions. Reduces un-
certainty regarding effects at-
tributable to weathering of sul-
fide minerals.
Clarifies the association be-
tween basin geology and stream-
water acidity. Improves region-
al classification system and ap-
propriate selection of models
used to estimate historical
change, future acidification and
episodic change.
Examines factors controlling
streamwater chemistry. Refines
assessments of stream sensitiv-
ity to anthropogenic acidifica-
tion, and helps explain the
roles of deposition, hydrology,
and geology.
66
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DELIVERABLE
DATE
SIGNIFICANCE
Estimated changes in lake-
water chemistry in the Nor-
theast from pre-1900 to the
present based on paleoecol-
ogical inferences.
Components of variance in
lakewater chemistry in a
regional (Northeastern) as-
sessment of lake character-
istics.
Acid Deposition and Aquatic
Ecosystems: Regional Case
Studies.
Early 1989
Mid-1989
Late 1989
Chemical response of an
alpine stream in Loch Vale
Watershed to an intense
summer rainstorm.
Influence of experimental
acidification on key
chemical processes in a
forested watershed.
Late 1989
Late 1989
Provides the first regional es-
timates of historical changes in
lakewater chemistry based on
paleoecological methods.
Reduces uncertainty in regional
estimates of lake chemistry made
during Phase I of the Eastern
Lake Survey. Quantifies
temporal and spatial variability
associated with the single fall
index sample.
Summarizes intercomparisons
among ten regions of the United
States and eastern Canada con-
cerning what is known about the
effects of acidic deposition on
lakes and streams. Will assess
the relative importance of proc-
esses controlling surface water
chemistry in low-alkalinity
lakes.
Documents effects of rapid
inputs of acidic deposition on
an alpine watershed-stream
system. Explores relative
importance of watershed
processes in alkalinity
generation.
Will improve process
representations used in modeling
sulfur fluxes through
ecosystems, aluminum transport,
soil and water responses
affecting aluminum mobilization,
changes in forest growth related
to nitrogen reduction and
release, and subsurface flow
pathways at the hillslope scale.
67
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DELIVERABLE
DATE
SIGNIFICANCE
Long-term depletion of
calcium and other nutrients
in eastern forests.
Late 1989
Precipitation and
streamwater chemistry from
undisturbed watersheds in
the Cascade Mountains of
Oregon.
Late 1989
Biogeochemistry of two
Appalachian deciduous
forest sites in relation to
episodic stream
acidification.
Throughfall chemistry, soil
solution chemistry, and
ionic budgets in a Sierra
Nevada mixed conifer
forest.
Late 1989
Late 1989
to
Early 1990
Watershed processes related
to buffering and
concentrations of organic
materials in surface waters
of Loch Vale Watershed.
Early 1989
to
Mid-1989
Reduces uncertainties regarding
the impact of increased leaching
of nutrient ions, particularly
calcium, resulting from
atmospheric deposition, which
may affect aquatic chemistry and
forest productivity.
Provides deposition stream
chemistry data from a research
site that are comparable to date
from sites that appear to be
relatively unaffected by acidic
deposition. Provides a
reference point for comparison
to watersheds subject to larger
amounts of acidic deposition.
Reduces uncertainty in the
understanding of the importance
of biochemical processes in
controlling episodic
acidification.
Provides information on
biogeochemical cycling
mechanisms, including capacity
of a forested ecosystem to
buffer effects of acidic inputs,
and processes influencing
precipitation chemistry as it
passes through the conifer
canopy and major soil horizons.
Elucidates mineral-water
interactions, including
weathering dynamics, that
control production of alkalinity
in a granite bedrock site with
poor soil development. Helps
explain the role of organic
production in generating
alkalinity and mobilizing metals
during snowmelt.
68
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DELIVERABLE
DATE
SIGNIFICANCE
Steam export, uptake rates,
and cycling of sulfur and
organic carbon in a
pristine conifer-dominated
watershed.
Early 1989
to
Mid-1989
Multiyear trends in
snowpack ion accumulation
and loss and pattern of
solute movement from
snowmelt episodes at Isle
Royale, Northern Michigan.
Early 1989
to
Mid-1989
Long-term monitoring
analysis of temporal
patterns and trends in a
regionally diverse group of
surface waters spanning a
range of deposition
gradients.
Chemical and biological
responses to reduction in
pH from 6.2 to 5.1 in an
experimentally acidified
seepage lake.
Mid-1989
Mid-1989
Presents site-specific data on
input-output budgets for sulfate
and nitrate from wet deposition.
Estimates base-flow nitrate and
hydrogen ion uptake which will
serve as reference for surface
water response at sites with
high acidic deposition loads.
Improves understanding of
sources, cycling, and fates of
sulfur and organic carbon.
Supports the hypothesis that
longer-term patterns of snowmelt
and pathways of ionic movement
are important factors in
determining whether streams
undergo an ionic pulse upon
snowmelt. Suggests that initial
snowmelt dynamics have little
effect on streamwater chemistry
and that forest soils do not
appear to enrich sulfate
concentration in subsequent
meltwaters. Nitrate
concentrations in meltwater
entering the stream, however,
indicate that these forest soils
are contributing nitrate.
Provides data on recent changes
in surface water chemistry of
low ANC surface waters
potentially related to acidic
deposition.
Provides data on acid-stressed
populations of freshwater
organisms and on biogeochemical
processes that will support
development of acid impact
models and help define regional
and national effects.
69
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DELIVERABLE
DATE
SIGNIFICANCE
Influence of experimental
acidification on the
biology and chemistry of a
warmwater lake ecosystem
(Little Rock Lake).
Acid-sensitivity of
cutthroat trout.
Early 1990
Late 1989
Use of benthic
macroinvertebrates as
indicators of the
sensitivity of stream
communities to
acidification.
Effect of cations mobilized
by acidic precipitation on
productivity and survival
of terrestrial vertebrates.
Fish communities in lakes
in the Upper Peninsula of
Michigan in relation to
lake acidity.
Mid-1989
Late 1989
Early 1989
The potential effects of
lake acidity on the
bioaccumulation of mercury
by fish in the Upper
Peninsula of Michigan.
Mid-1989
Examines the effects of
progressive acidification on the
structure and function of a
warmwater seepage lake and
evaluates the state of the art
of predicting these effects.
Describes the sensitivity of
western salmonid species to low
pH and elevated concentrations
of aluminum, providing
information necessary to assess
potential effects of acidic
deposition on fishery resources
in the western United States.
Describes a technique that uses
the presence of certain
macroinvertebrate taxa,
individually and combined, to
evaluate the biological
sensitivity of stream
communities in the Southern Blue
Ridge Province to acidification.
Provides information on the food
chain response to mobilized
cations in acidified freshwater
environments.
Provides regional-level
information on fish community
response in potentially
sensitive lakes. Results review
fish community status as a
function of water chemistry for
a defined probability sample of
lakes.
Provides information on whether
lake acidity and fish mercury
content are significantly
correlated. Estimates the
number and extent of lakes in
the Upper Peninsula of Michigan
with enhanced fish mercury
levels.
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DELIVERABLE
DATE
SIGNIFICANCE
Effects of liming on fish
populations.
Late 1989
Effects of lime addition to
lakes.
Direct/Delayed Response
Project (DDRP) model
sensitivity and uncertainty
analysis.
Dynamic model forecasts for
regional changes in acid
neutralizing capacity in
surface waters in the
Northeast, Southern Blue
Ridge Province, and Mid-
Appalachians.
Current status, historical
changes, and episodic
changes in surface water
acid-base chemistry related
to acidic deposition
including watershed and
lake processes affecting
surface water response,
biological effects,
mitigation, and methods for
forecasting future changes
in surface water chemistry.
Late 1989
to
Early 1990
Early 1989
Mid-1989
and
Mid-1990
Mid-1990
Discusses the dose-response
relationship between liming and
surface water chemistry and
freshwater organisms and the
effects of liming on metals and
nutrient flux. Contributes to
understanding of the potential
for mitigation techniques to
benefit fish survival and
health.
Documents and models the effects
of base addition on light
attenuation and thermal
stratification, which strongly
influence lake biology.
Evaluates three dynamic models
of catchment acidification used
to project the number of
watersheds that may become
acidic under current or altered
deposition. Provides a means to
estimate sensitivity and
performance of models used for
DDRP forecasts.
Provides regional forecasts with
quantifiable certainty of the
rate of change in acid
neutralizing capacity for
surface waters in three areas of
the United States susceptible to
acidic deposition.
Provides comprehensive state-of-
science with quantified
uncertainty, forming a partial
basis for NAPAP's 1990
Integrated Assessment. Presents
models for forecasting and
hindcasting acid-base chemistry
and biological effects based on
various scenarios of acidic
deposition loading.
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EFFECTS ON MATERIALS AND CULTURAL RESOURCES
1988 RESEARCH HIGHLIGHTS
Atmospheric Corrosion Testing Of Zinc,
Galvanized Steel And Other Metals
A preliminary dose-response function
for predicting the corrosion of gal-
vanized steel by wet and dry deposi-
tion has been developed from the ther-
modynamics and kinetics of atmospheric
corrosion chemistry, supported by lab-
oratory and controlled field experi-
ments. The function mathematically
expresses the competing reactions for
the build up and dissolution of the
basic zinc carbonate corrosion film
with exposure time. The model quan-
titatively accounts for the following
factors: (1) Basic zinc carbonate,
formed by exposure to C02, is soluble
in clean rain, and the removal rate
depends on the residence time of the
rain on the galvanized steel surface;
(2) Rain acidity reacts stoichiometri-
cally with the zinc coating; (3) The
deposition of gaseous S02 during peri-
ods of wetness controls the rate of
corrosion of galvanized steel struc-
tures; (4) During periods of surface
wetness, S02 reaching the surface re-
acts stoichiometrically with the zinc.
The effects of acidic deposition on
the corrosion of zinc, galvanized
steel, and other metals is being in-
vestigated at five materials exposure
sites, as well as in laboratory exper-
iments using atmospheric exposure
chambers. The annual corrosion rates
estimated from the five-year exposure
data were observed to vary by nearly a
factor of three, with a ten-fold vari-
ation in sulfur dioxide concentration
among the five sites. Measured depo-
sition rates of sulfur dioxide to
weathered zinc surfaces were observed
to increase substantially with in-
creasing exposure time, but decreased
with time to weathered Cor-Ten A and
110 copper surfaces. These results
indicate that the nature of the cor-
rosion product formed on metal sur-
faces influences the rate at which
sulfur dioxide is deposited.
Galvanized steel runoff experiments at
the Research Triangle Park, North
Carolina and Steubenville, Ohio sites
have been completed. Runoff samples
were collected on a rain-event basis
from each panel followed by detailed
chemical analysis of the collected
solutions. Preliminary data analysis
suggests that neutralization of acidic
species by dry deposited coarse alka-
line particles could be significant at
the Ohio site. A study to determine
how corrosion rates change with vary-
ing sample size and orientation is
currently underway. Preliminary re-
sults suggest that the rate of uptake
of S02 to galvanized steel surfaces
depends on the size of the sample,
with the deposition rate per unit area
increasing with decreasing size.
The Effects of Acidic Deposition on
Carbonate Stone
Acidic deposition to carbonate stone
surfaces causes surface erosion
through dissolution of stone exposed
to rain, and causes gypsum deposits to
form on surfaces sheltered from rain.
Run-off experiments on limestone and
marble slabs at four materials expo-
sure sites can be used to partition
the effects of hydrogen ion loading,
the dry deposition of sulfur oxides
and nitrogen oxides vis-a-vis the
natural solubility of calcium carbon-
ate in pH 5.6 rain. The excess sul-
fate and nitrate in the stone runoff
73
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solutions relative to corresponding
glass blanks can be used as a measure
of stone recession due to the loss of
reaction products from the dry deposi-
tion of sulfur and nitrogen oxides.
Data from three years of runoff exper-
iments suggest that dry deposition
accounts for 50-80 percent of the sul-
fate in runoff from quarry fresh mar-
ble and limestone surfaces. These
data suggest that hydrogen ion
accounts for approximately 10 percent
of the stone recession at the exposure
sites, while recession due to the re-
action with sulfur oxides varies from
6 percent at the Adirondacks site to
20 percent at the downtown Washington,
D.C. site. Sulfate accumulates on the
sheltered undersides of the stone test
samples. Estimates of annual sulfate
accumulations based on four years of
data agree within a factor of two with
the cumulative measure of the excess
sulfate removed from the quarry fresh
marble and limestone slabs in the run-
off experiments.
Additional experiments were initiated
using samples of weathered marble and
80-year old limestone. The weathered
surfaces, especially limestone, showed
a higher concentration of gypsum
(penetrating more than 1.5 mm into the
stone) than was detected in fresh
stone after four years of exposure at
the field sites. The analysis of
weathered stone in parallel with quar-
ry fresh samples is expected to pro-
vide insight on the rate of gypsum
accumulation and dissolution erosion
over more typical lifespans of stone
materials.
Progress was made in several labora-
tory studies addressing the deposition
of pollutants to stone surfaces.
Surface moisture is an important fac-
tor in determining dry deposition
rates to stone surfaces. Wetting and
drying characteristics of limestone
briquettes have been analyzed through
the use of a CAT scanning technique.
The study was undertaken in order to
better define the moisture cycling
important to sulfur deposition,
reaction, and crystallization. The
experiments showed that rain water
wetting limestone becomes uniformly
distributed within the sample, presum-
ably by capillary forces. After a
rainfall, the sample dries uniformly
throughout its entire volume. Solar
radiation appears to have little or no
effect on the interior drying pattern,
although wind appears to result in
preferential drying on the windward
side of the briquette.
Laboratory Experiments on the Deposi-
tion of Acidic Pollutants to Paint
Films, and the Effects on Polymer
Coatings and at the Paint/Substrate
Interface
Laboratory experiments are being con-
ducted to determine the uptake of acid
gases on paints covered with thin
layers of moisture, the permeation of
acid gases through polymers, and the
effects on polymers and at the paint/-
substrate interface. An environmental
test chamber, capable of exposing
samples to S02, N02, and 03, has been
designed, built, and tested. Initial
exposures of alkyd paints were made in
1-ppm S02. Some samples had previous-
ly been exposed to ultraviolet radia-
tion. Samples were either kept at a
constant temperature for dry deposi-
tion or were cyclically cooled for
both wet and dry deposition. X-ray
photoeletron spectroscopic (XPS) mea-
surements of the surfaces revealed
that S accumulation on dry surfaces
was 3-10 times greater than on sur-
faces exposed under diurnal wet-dry
cycle conditions. Surface moisture
apparently allows deposited S to per-
meate the paint film, which has also
been observed in samples immersed in
diluted H2S03. Studies are ongoing to
confirm the permeation.
An in-situ electrochemical monitor
capable of detection of paint degrada-
tion in atmospheric exposure via
electrochemical impedance spectroscopy
(EIS) has been developed. The
electrochemical monitor will be
74
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utilized in the environmental exposure
chamber and will represent the first
technique which can be performed en-
tirely in-situ to dectect coating
deterioration. The additional benefit
of the monitor lies in its applicabil-
ity for EIS measurements, since EIS is
capable of prediction/detection of
coating deterioration at very early
exposure times. It is expected that
this technique will contribute to un-
derstanding of coating failure mechan-
isms and the early detection of coat-
ing failure.
Effects of Acidic Deposition on the
Permeability and Chemical Structure of
Paint Films
The leaching of extender components
alters the characteristics of paint
films, in particular affecting the
moisture and pollutant transport
through the film and, thus, the abil-
ity to protect the substrate. Paints
without carbonate extenders lose con-
siderably less weight after immersion
in acid than those with carbonate. For
paints containing CaC03, all of the
CaC03 is removed by immersion in acid,
with a rate that is dependent on pH.
The leaching process affects the
mechanical properties of the paint
under certain temperature conditions.
The kinetics of extender removal have
been quantified from pH 2.0 to pH 5.6
for immersion in aqueous sulfurous
acid solutions. The polymer itself is
unaffected by immersion in acid.
Fourier-transform infrared spectros-
copy, using the attenuated total
reflectance sampling method (FTIR-
ATR), has proven to be an invaluable
technique for assessing the effects of
acidic deposition on the chemical com-
position of paint films. Changes in
the chemical structure of the base
polymer have been noted after rela-
tively short exposure periods to UV
light + S02. Changes in the chemical
composition of the paints, due to
leaching or other removal processes,
can be followed, and the kinetics of
removal can be determined. The exper-
iments completed to date have verified
the feasibility of the ATR sampling
method. Future experiments will be
directed at in-situ monitoring of
changes in the chemical structure and
composition of the paints during ex-
posure to pollutant gases and acidic
environments.
The solubility and diffusivity of S02
in latex paints has been determined at
room temperature and at varying pres-
sures of S02. A linear relation has
been confirmed between the partial
pressure of S02 and its concentration
in the polymer. Dissolution of S02
occurs only in the polymer, with the
inorganic additives acting simply as
impenetrable fillers. The base poly-
mer in the paint absorbs about 13 per-
cent by weight of S02 at an S02 pres-
sure of 1 atm. The diffusivity of S02
in the paints can be measured, is pre-
ssure dependent, and when combined
with the solubility (S), the permea-
bility (P - SD) of the paints to S02
can be determined. This research has
increased our understanding of the
transport of S02 through paint films
to the underlying substrate.
In Situ Studies of Materials Damage
The correlation between day-night
timing of wetting/drying cycles and
day-night variations in the concentra-
tions and deposition of acidic pollu-
tants has been investigated near a
150-year old marble-faced building in
Philadelphia. The building has a
variety of exposure situations that
affect the wet and dry deposition of
pollutants. It has previously been
observed that the deterioration of
stone building exteriors occurs at
greatly differing rates on varying
parts of the building. This observa-
tion is the basis for a series of mea-
surements in which soluble deposits
are sampled at various locations on
the building exterior surfaces. These
samples are collected in regions with
varying degrees of sheltering from
75
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direct exposure to rain and with dif-
ferences in visible surface accumula-
tion and discoloration. The study of
weathered marble on an actual building
in an urban setting enhances our
understanding of materials performance
in an architecturally and historically
important setting. The results are
expected to augment the results of
research directed toward the develop-
ment of dose-response functions in
laboratory and controlled field exper-
iments, by the identification of the
range of conditions that are the re-
sult of varying exposures on actual
structures.
In a study conducted at Gettysburg
National Military Park, Pennsylvania,
field experiments have been conducted
to investigate the dynamics of dry
deposition to complex shapes. An
equestrian statue was selected to pro-
vide a variety of shapes with dif-
ferent aerodynamic characteristics.
The transport of acidic gases and par-
ticulates to the statue is being stud-
ied by using collection surfaces at-
tached to the statue. Surrogate sur-
faces with aerodynamically well-
defined boundary layer characteristics
are also being exposed near the
statue. Initial results indicate that
greater fluxes of nitrate and sulfate
correspond spatially to surfaces on
the statue with greater degrees of
corrosion.
MAJOR DELIVERABLES
DELIVERABLE
DATE
SIGNIFICANCE
Report on laboratory
studies relating to carbon-
ate dissolution processes.
Early 1989 The report will present the in-
terpretation of kenetic experi-
ment results and a geochemical
model for pollutant damage to
carbonate stone.
A report on laboratory
studies relating to the
deposition of atmospheric
precursor gases to stone
surfaces.
Early 1989 The report will describe the
deposition of S02 and NOX to the
surfaces of freshly quarried
and weathered carbonate stone
under ambient environmental
conditions. This data will
assist in predicting stone
damage from dry deposition.
76
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DELIVERABLE
DATE
SIGNIFICANCE
A report on the analysis of
sulfur compounds at the
paint/wood interface after
sulfuric acid treatment.
Early 1989
A report on damage func-
tions for zinc and galvan-
ized steel based on long-
term field exposure data.
Mid-1989
A report on the micro/macro
effects of acidic
deposition on paint/
substrate systems.
A report on a study conduc-
ted at Mesa Verde National
Park, Colorado.
Mid-1989
Late 1989
A report on a study conduc-
ted at Gettysburg National
Military Park,
Pennsylvania.
Late 1989
If sulfur is detected than it
is possible that sulfuric acid
can affect paint adhesion. On
the other hand, if sulur is not
detected, than it is unlikely
that sufficient sulfuric acid
can diffuse through an intact
paint film to affect paint
adhesion.
The report will present an
analysis of the data from long-
term exposure (1-year and
greater) of zinc and galvanized
steel at the materials exposure
sites. It will integrate the
corrosion data base with the
rain chemistry and aerometric
data bases for each site.
The report will characterize
the linkages between
microscopic changes in paint
films and macroscopic modes of
paint failure. This information
is required for economic
assessment activities.
The report will define the ef-
fects of environmental exposure
on the sandstone ruins, based
on the results of four years of
parallel monitoring of
sandstone decay and
environmental factors.
The report will describe the
effects of acidic pollutants on
bronze and carbonate stone
monuments, based on the results
of in-situ runoff experiments
at this rural Pennsylvania
site.
77
-------
DELIVERABLE
DATE
SIGNIFICANCE
A report on the micro-
damage of acrylic latex
paint on wood substrates
exposed to acidic
deposition.
Late 1989
The report will discuss the
development of coating mechan-
isms which will aid in the pre-
diction of coating lifetimes
under various exposure condi-
tions.
A report on painted wood
exposed for 18 months in an
outdoor environment at
sites in Steubenville,
Ohio; Raleigh, North
Carolina; and Madison,
Wisconsin.
Early 1990
A report on dose-response
functions for carbonate
stone.
Mid-1990
A series of reports on 5-
year field exposure tests
on carbonate stone.
Mid-1990
A report on dose-response
functions for selected
coating systems.
Mid-1990
The report covers how samples
will be evaluated for paint ad-
hesion, chemical reactions at
the paint/wood interface, and
surface changes to the paint.
The results of this experiment
should allow the documentation
of different weathering mechan-
isms and rates for various pol-
lution levels.
The report will discuss the al-
gorithms to be used for the
dose-response functions for
carbonate building stone
(including information on
changes in surface composition,
roughness, recession, and
runoff chemistry) in an
economic assessment of the
effects of acidic deposition.
These reports will describe the
results of mineralogical, sur-
face chemistry, roughness/
recession, weight loss, color
change, and runoff measurements
at five field sites in relation
to environmental data supplied
by EPA.
This report will provide
discussions of first generation
dose-response functions
produced under laboratory and
field conditions for the effect
of pH, sulfur dioxide, and
oxides of nitrogen on polymeric
surface coatings.
78
-------
DELIVERABLE
DATE
SIGNIFICANCE
A report on the evaluation Mid-1990
of chemical changes in
lignin and carbohydrates in
wood that has been exposed
to dilute sulfuric,
sulfurous, and nitric acids
at room temperature.
A report on monitoring Mid-1990
studies conducted at Inde-
pendence National
Historical Park,
Philadelphia, Pennsylvania.
The elucidation of these chemi-
cal changes under laboratory
conditions is expected to pro-
vide the background information
which is necessary for evaluat-
ing specimens exposed in out-
door environments.
This document will describe the
results of one year of parallel
monitoring of marble decay and
environmental factors on an
historical marble building at
an urban Philadelphia site. The
study will describe the effects
of orientation and sheltering
on stone damage resulting from
acidic deposition.
79
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PUBLICATIONS
EMISSIONS AND CONTROLS
Benkovitz, C.M. and N.L. Oden. 1987. Uncertainty Analysis of
the NAPAP Emissions Inventory - Progress Report FY 1986.
BNL Formal Report, BNL 52132.
Chun, K.C. 1988. Uncertainty Data Base for Emissions-
Estimation Parameters: Area-Source Supplement to Interim
Report. ANL/EES-TM-353.
Hanson, DA, M.J. Bragen, M. Browdy, and G.A. Boyd. 1988.
Advanced Utility Simulation Model (AUSM): State Level
Projections of Required Electrical Generation and Sources of
Supply. ANL/EES-TM-357
Kohout, E.J., C.L. Saricks, and D.J. Miller. 1988. Estimated
Monthly Emissions of Sulfur Dioxide, Oxides of Nitrogen,
and Volatile Organic Compounds for the 48 Contiguous
States, 1987. ANL/EES-TM-322.
Marinelli, J., DA Hanson, and D.W. South. 1988.
Regionalized Fuel Prices by End-Use Sector for Use in
Testing the Emissions Model Set of the National Acid
Precipitation Assessment Program. Rep. ANL/EES-TM-356.
Pieper, P.J., DA Hanson, D.W. South, and G.A. Boyd. 1988.
Review of the DRI Long-term Macroeconomic Projections
and Their Extension to the Year 2030. Rep. ANL/EES-TM-358.
South, D.W., J.F. McDonald, M.J. Bragen, G.A. Boyd, DA
Hanson, and D.S. Rothman. 1988. Industrial Volatile Organic
Compounds (VOC) Model: Regionalized Projections of
Uncontrolled VOC Emissions by Source Category. Rep.
ANL/EES-TM-306.
South, D.W., M.J. Bragen, C.M. Macal, DA. Hanson, and
D.S. Rothman. 1988. Industrial Sector Technology Use Model
(ISTUM): Regionalized Projections of Industrial Production
Indexes. Rep. ANL/EES-TM-330.
U.S. Environmental Protection Agency. 1988. Anthropogenic
Emissions Data for the 1985 NAPAP Emissions Inventory.
Rep. EPA-600/7-88-022.
U.S. Environmental Protection Agency. 1988. Advanced Utility
Simulation Model Documentation of System Design State
Level Model (Version 1.0). Rep. EPA-600/8-88-071C, PB 89-
101208.
U.S. Environmental Protection Agency. 1988. Documentation
of Spatial Allocation Factor Procedures for the 1980 NAPAP
Emissions Inventory. Rep. EPA-600/7-88-024a.
U.S. Environmental Protection Agency. 1988. Users Manual
for the Personal Computer Version of the Process Model
Projection Technique (Version 3.0) Rep. EPA-600/8-88-0953.
U.S. Environmental Protection Agency. 1988. Comparison of
Historic SO1 and NOx Emission Data Sets. Rep. EPA-600/7-
88-009a/b.
U.S. Environmental Protection Agency. 1988. Cost of
Controlling Directly Emitted Acidic Emissions from Major
Industrial Sources. Rep. EPA-600/7-88-012, PB 88-234190.
U.S. Environmental Protection Agency. 1988. The Volatile
Organic Compound Model Quality Assurance and Sensitivity
Testing (Version 1.8). Rep. EPA-600/8-88-088, PB 88-234166.
U.S. Environmental Protection Agency. 1988. A Projection
Methodology for Future State Level Volatile Organic
Compound Emissions from Stationary Source. Rep. EPA-
600/8-88-090, PB 88-23873.
U.S. Environmental Protection Agency. 1988. Historic
Emissions of Volatile Organic Compounds in the U.S. from
1900 to 1985. Rep. EPA-600/7-88-008a-d. PB 88-208723 (a),
PB 88-250311 (b-d).
U.S. Environmental Protection Agency. 1988. Description of
the Industrial Combustion Emissions Model (Version 6.0).
EPA-600/8-88-077, PB 88-212287.
U.S. Environmental Protection Agency. 1988. Revision of the
Industrial Combustion Emissions Model to a Base Year of
1980. Rep. EPA-600/8-88-078, PB 88-211941.
U.S. Environmental Protection Agency. 1988. Industrial
Combustion Emissions Model (Version 6.0) Users Manual.
Rep. EPA-600/8-88-007a, PB 88-172234.
U.S. Environmental Protection Agency. 1988. Industrial
Combustion Emissions Model (version 6.0) Software
Description. Rep. EPA-600/8-88-009, PB 88-191176.
U.S. Environmental Protection Agency. 1988. Industrial Boiler
Furnace Sorbent Injection Algorithm Development. Rep. EPA-
600/8-88-065, PB 88-184890.
U.S. Environmental Protection Agency. 1988. Volatile Organic
Compound Emission Projection Model User's Manual
(Version 1.8). Rep. EPA-600/7-87-059a, PB 88-157896.
U.S. Environmental Protection Agency. 1988. Development of
the 1980 NAPAP Emissions Inventory. Rep. EPA-600/8-86-
057a, PB 88-132121.
U.S. Environmental Protection Agency. 1988. Flexible
Regional Emissions Data Systems (FREDS) Documentation
for the 1980 NAPAP Emissions inventory. Rep. EPA-600/7-87-
025a&b, PB 88-129499/481.
U.S. Environmental Protection Agency. 1988. Industrial Boiler
Low NOx Combustion Retrofit Cost Algorithm Development.
Rep. EPA-600/8-88-091, PB 88-239074.
U.S. Environmental Protection Agency. 1988.
Ohio/Kentucky/TVA Coal-Rred Utility SO2 and NOx Control
Retrofit Study. Rep. EPA-600/7-88-014, PB 88-24447.
U.S. Environmental Protection Agency. 1988. Development of
the Fuel Choice Module in the Industrial Combustion
Emissions Model, Volume I, Phases 1 & III. Rep. EPA-600/8-
88-064b, PB 88-198585.
U.S. Environmental Protection Agency. 1988. Advanced Utility
Simulation Model Multi-Period Multi-State Module Design
Documentation (Version 1.0). Rep. EPA-600/8-88-017d, PB 89-
204268.
U.S. Environmental Protection Agency. 1988. Advanced Utility
Simulation Model Data Base Maintenance Documentation
(Version 1.0). Rep. EPA-600/8-88-071f, PB 89-204276.
81
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ATMOSPHERIC CHEMISTRY
Andreae, M.O., H. Berresheim, T.W. Andreae, MA Kritz, T.S.
Bates, and J.T. Merrill, 1988. Vertical distribution of
dimethylsulfide. sulfur dioxide, formic acid, aerosol ions, and
radon over the northeast Pacific Ocean. J. Atmos. Chem.
6:149-173.
Baldocchi, D.D, B.B. Hicks and T.P. Meyers. In Press.
Measuring biosphere-atmosphere exchanges of biologically
related gases with micrometeorological methods. Ecology.
Baldocchi, D.D. 1988. A multi-layer model for estimating
sulfur dioxide deposition to a deciduous oak forest canopy.
Atmos. Environ. 22:869-884.
Barrio, LA, S.E. Lindberg. W.H. Chan, H.B. Ross, R.
Arimoto, and T. M. Church. 1987. On the concentrations of
trace metals in precipitation. Atmos. Environ. 21:1144-1135.
Burkholder, J.B., P.O. Hammer, C.J. Howard, and A.R.W.
McKellar. 1988. Fourier Transform Infrared Spectrum of the
v2 Band of the NH2 Radical. J. Mol. Spectrosc. 127:415-424.
Carmichael, G.R., S.Y. Cho, and Y.S. Chang. In Press.
Evaluation of the effect of reductions in ambient levels of
primary pollutants on sulfate and nitrate wet deposition.
Atmos. Environ.
Chang, Y.S.. G.R. Carmichael, H. Kurita, and H. Ueda. In
Press. The transport and formation of photochemical
oxidants in central Japan. Atmos. Environ.
Cho, S.Y., G.R. Carmichael, and H. Rabitz. In Press.
Relationships between primary emissions and acid deposition
in Eulerian models determined by sensitivity analysis. Air,
Water & Soil Pollution.
Cho, S.Y., G.R. Carmichael and H. Rabitz. 1987. Sensitivity
analysis of the atmospheric reaction-diffusion equations.
Atmos. Environ. 21:2589-2598.
Dana, M.T. and W.G.N. Slinn. 1988. Acid deposition
distribution and episode statistics from the MAP3S network
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Daum, P.H., K. Anlauf, J. Bottenheim, KA Brice, and A.
Wiebe. In Press. Processes determining cloudwater
composition: Inferences from field measurements. In:
Proceedings, NATO Advanced Research Workshop: Acid
Deposition Processes at High Elevation Sites, Edinburgh,
Scotland, Sept. 1986.
Dlugokencky, E.J., and C.J. Howard. 1988. Laboratory
studies of NO3 radical reactions with some atmospheric
sulfur compounds. J. Phys. Chem. 92:1188-1193.
Dronamraju, M., LK. Peters, G.R. Carmichael, P.S.
Kasebhotla, and S.Y. Cho. In Press. An Eulerian
transport/chemistry/removal model for SO2 and sulfate: III
Comparison with the July 1974 SURE data base. Atmos.
Environ.
Fall, a, D.L Albritton, F.C. Fehsenfeld, W.C. Kuster, and P.O.
Goldan. 1988. Laboratory studies of some environmental
variables controlling sulfur emissions from plants, J. Atmos
Chem. 6:341-362.
Fehsenfeld, F., O. Hov, G.A. Ancellet, RA Cox, D. Ehhalt, H.
Hakola, M. Legrand, and S. Liu. 1988. NOX in the
troposphere. In: I.SA Isaksen (ed.). Tropospheric Ozone. D.
Reidel Publishing Company, pp. 393-401.
Fehsenfeld, F., D. Parrish, and D. Fahey. 1988. The
measurement of NOX in the non-urban troposphere. In: I.SA
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Company, pp. 393-401.
Gleason, J.F. and C.J. Howard. 1988. Temperature
dependence of HOSO2 + O2. J. Phys. Chem. 92:3414-3417.
Goldman, A., J.B. Burkholder, and C.J. Howard. In Press.
Spectroscopic Constants for the v2 Infrared Band of HNO3.
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Greenblatt, G.D. and C.J. Howard. In Press. Oxygen atom
exchange in the interaction of OH with several small
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Guenther, A., B. Lamb, and H. Westberg. 1988. A U.S.
national biogenic sulfur emissions inventory, In: E.S.
Saltzman and W.V. Cooper (eds.) Biogenic Sulfur in the
Environment. American Chemical Society, Washington, D.C.
Hales, J. M., and W. T. Pennell. 1988. Computer simulation
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chemistry and meteorology in modeling and measuring dry
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R. P. Hosker. 1987. A preliminary multiple resistance model
for deriving dry deposition velocities from measured
quantities. Water, Air and Soil Pollution. 36:311-330.
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atmospheric deposition, stream export, and landscape
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Liu, S.C. and M. Trainer. 1988. Responses of tropospheric
ozone and odd hydrogen radicals to column ozone change,
J. Atmos. Chem. 6:221-223.
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Changing Atmosphere.
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1987. A comparison of estimated and measured S02
deposition velocities, Water, Air and Soil Pollution
36:331-345.
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extended applicability to non-simple terrain. Boundary-Layer
Meteorology 43:231-245.
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of trace gas deposition velocities, Report to EPA.
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of large systems of stiff differential equations. In:
Proceedings AlChE Annual Meeting, Miami, Fla.
Meyers, T.P. and B.B. Hicks. 1988. Dry deposition of O3,
SO? and HNO, to different vegetation in the same exposure
environment. Environ. Pollut. 53:13-25.
Meyers, T.P. and D.D. Baldocchi. In Press. A comparison of
models for deriving dry deposition fluxes to O3 and S02 to
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