THE EFFECTS OF AIR POLLUTION




     ON WATER QUALITY
         PEDCo ENVIRONMENTAL

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                                                   950R77O10
                               PEDCo  ENVIRONMENTAL
                                               11499 CHESTER ROAD
                                            CINCINNATI. OHIO 45346

                                                    (513) 783-4700
                  THE EFFECTS OF AIR POLLUTION

                        ON WATER QUALITY
                           Prepared by

                    PEDCo-Environmental,  Inc.
                       11499 Chester Road
                     Cincinnati, Ohio  45246
                    Contract No.  68-02-2515
                           Task No.  2
              Project Officer:  Justice A. Manning
                    Task Officer:  Don Lokey
                          Prepared  for

             Strategies and Air Standards Division
          Office of Air Quality Planning and Standards
              U.S. Environmental Protection Agency
                    Research Triangle Park,
                     North Carolina 27711
                         March 15,  1977

                               BRANCH OFFICES
CHESTER TOWERS
                         Crown Center
                        Kansas City. Mo.
Professional Village
 Chapel Hill. N.C.

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     This report was written for the U.S. Environmental



Protection Agency by PEDCo Environmental, Inc., Cincinnati,



Ohio, under Contract No. 68-02-2515, Task No. 2.  The con-



tents of this report are reproduced herein as received from



the contractor.  The opinions, findings, and conclusions



expressed are those of the author and not necessarily those



of the U.S. Environmental Protection Agency.
                           11

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                       ACKNOWLEDGMENT






     This report was prepared for the U.S. Environmental



Protection Agency by PEDCo Environmental, Inc., Cincinnati,



Ohio.  David W. Armentrout was the principal investigator



and author.



     Mr. Don Lokey was the task officer for the U.S. Environ-



mental Protection Agency.  We wish to thank him and also Mr.



John Bachmann of the Agency for their technical assistance



and comments throughout this task.
                              111

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                      TABLE OF CONTENTS


                                                       Page

ACKNOWLEDGEMENT                                        iii

LIST OF TABLES                                         V

1.0  EXECUTIVE SUMMARY                                 1-1

     1.1  Conclusions and Recommendations              1-1

     1.2  Survey Results                               1-2

2.0  INTRODUCTION                                      2-1

     2.1  Purpose and Scope                            2-1

     2.2  Evidence of Atmospheric Effects on Water     2-2
          Quality

3.0  SURVEY RESULTS                                    3-1

     3.1  Trace Metals                                 3-1

     3.2  Nutrients                                    3-14

     3.3  Toxic Organics                               3-23

     3.4  Airborne Acids                               3-27

4.0  CONCLUSIONS AND RECOMMENDATIONS                   4-1

     4.1  Conclusions                                  4-1

     4.2  Recommendations                              4-8

     4.3  Intra-Agency Considerations                  4-11

REFERENCES

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                       LIST OF TABLES
No.                                                    Page

 1   Estimates of Potential Trace Metal Input To       3-2
     Lake Michigan

 2   Estimates of Trace Metal Input To Lake Washington 3-3

 3   Trace-Element Input to Lake Superior From Four    3-5
     Major Source Categories as Estimated in the
     Upper Lakes Study

 4   Trace-Element Input to Lake Huron From Four Major 3-5
     Source Categories as Estimated in the Upper Lakes
     Study

 5   Elemental Ratios in Rain,  Soil, and Fly Ash in    3-8
     the Walker Branch Watershed

 6   Summary of Trace-Element Mass Balance Results     3-9
     for January-June 1974 at Walker Branch Watershed

 7   Estimated Wet Deposition vs. Dry Deposition of    3-9
     Selected Elements in the Walker Branch Watershed

 8   Nitrogen and Phosphorous Input to Lake Superior   3-18
     From Four Major Source Categories as Estimated
     in the Upper Great Lakes Study

 9   Nitrogen and Phosphorous Input to Lake Huron      3-18
     From Four Major Source Categories as Estimated
     in the Upper Great Lakes Study

10   Drift vs. Particle Size Pesticides                3-24

11   Estimated Inputs to the Southern California Bight 3-26
                             VI

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                   1.0  EXECUTIVE SUMMARY





     This report summarizes the results of a literature re-



view performed for the purpose of defining the known and



potential impacts of air pollution on water quality.  The



literature survey was supplemented by a limited number of



conversations with researchers who have been involved with



intermedia pollution problems.



     Air pollution effects on water quality have been a



significant part of environmental research in Europe, espe-



cially in Scandinavia, for several decades.  These effects



have more recently become a topic of environmental research



in the United States and Canada.  For convenience, the



potential effects are discussed for four categories of



pollutants:  trace metals, nutrients, toxic organic com-



pounds, and airborne acids.



1.1  CONCLUSIONS AND RECOMMENDATIONS



     For every pollutant category reviewed, the research



evidence indicates that the atmosphere can be a significant



source of pollutant input to water.  The development of



continuous data bases to provide statistically significant



data has been limited by problems with sampling methodology



and by a total absence of interagency project coordination
                           1-1

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within the United States.  Intergovernmental cooperation and

information exchange among the United States and foreign

governments has been good, but a serious effort to coordi-

nate studies within the United States is needed.  Too many

small-scale projects are being funded through various agen-

cies.  It is believed that better data and better project

quality control could be obtained through a planned research

program dealing with intermedia effects.

     The survey concludes that expanded research is neces-

sary to accomplish the following specific tasks:

     0    Identify pollutant sources and relative source
          contributions to the total pollutant impact on
          water.

     0    Improve technology for sampling the dry deposition
          of pollutants onto water surfaces.

     0    Expand the data base through expanding geograph-
          ical coverage of precipitation chemistry networks
          and through more long range studies of specifi"
          watersheds.

     0    Determine cross-media impacts, including direct
          impacts of air pollutants on water and the in-
          direct impact of air pollution control technology
          on water quality.

     0    Expand research to define effects of pollutants on
          aquatic life forms and to determine the mechanisms
          of those effects.

1.2  SURVEY RESULTS

1.2.1  Trace Metals

     Insufficient data have been documented to allow reason-

able predictions to be made of the impact of atmospheric
                            1-2

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trace metals on water in any specific geographic locations.



The presumptive evidence shows, however, that the air is



probably a significant source of trace metals detected in



some water systems.  Data from Lake Michigan studies show



that the atmosphere could be a primary source of input for



at least nine trace metals into that lake.  Studies of the



Lake Washington Watershed in western Washington and the



Walker Branch Watershed in Tennessee present similar con-



clusions for their associated water systems.



     The effects of trace-metal levels on the biota in water



are not thoroughly understood.  A major theory is that



excess concentrations of trace metals are toxic at acid pH.



More research is required to define excess concentrations



and to determine the mechanisms of toxicity.



     The increased application of emissions controls on some



fossil-fuel-burning installations may have little effect on



decreasing the potential atmospheric loading of trace metals



into water.  Studies show that trace metals are concentrated



during the combustion process, and that a significant amount



of these metals are included on the particulate fractions



that escape electrostatic precipitators.



1.2.2  Nutrients



     Lakes naturally evolve from an oligotrophic (nutrient-



poor) to a eutrophic (nutrient-rich) state.  Human activi-



ties can accelerate the eutrophication process, causing an
                           1-3

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overabundant concentration of nutrients and subsequent



stimulation of life cycles and depletion of oxygen within



the eutrophic lake.



     Nitrogen and phosphorous are the most frequently



studied nutrients.  Several studies show that whereas pre-



cipitation is a significant source of nitrogen in surface



water, it appears to be a less significant source of phos-



phorous.  Other studies show that precipitation is not a



significant source of either nitrogen or phosphorous to the



watersheds or water systems studied.  The importance of



atmospheric input of nutrients to water appears to be a



function of increased industrial or agricultural activity.



     Problems with sampling methodology limit the data



available on the determination of dry deposition of nutri-



ents into water.  These problems also limit emission source



identification.



1.2.3  Toxic Organic Compounds



     The toxic organic compounds most often cited in the



literature reviewed are polychlorinated biphenyls (PCB's)



pesticides and, more recently, nitrosamines.



     The toxicity mechanisms of the toxic organic compounds



are not completely understood.  PCB's and DDT have been



implicated as causative agents of cancer, however, and since



these compounds can bioconcentrate in fish, their presence



in water presents a hazard to humans.
                            1-4

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     It is estimated in a study of the sources of PCB input



to the Southern California Bight that the atmosphere may be



at least as significant as municipal wastewater systems as a



source of PCB input to that area.  Little significant in-



formation appears in the literature to quantify the contri-



bution of atmospheric sources of toxic organic compounds to



concentrations of these compounds in water.



1.2.4  Airborne Acids



     Extensive literature is available concerning acid pre-



cipitation.  The results of acid precipitation studies in



Europe, the United States, and Canada in recent decades



present strong evidence that increased acidity of precipita-



tion is the result of atmospheric pollutants from fossil-



fuel combustion.  The pH of precipitation in much of the



northern United States is reported to average between 4.0



and 4.2.  Values as low as 2.1 to 3.0 have been reported



during isolated storms.  In Europe, particularly in Norway,



the consumption of fossil fuel, the increased acidity of



precipitation, and the increased number of barren lakes can



be correlated.



     Although more work is required to determine pH effects



on aquatic life, previous studies indicate that low pH



affects the reproduction and possibly the metabolism of



fish.  Low pH levels also may affect the toxicity of trace



metals.
                          1-5

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                      2.0  INTRODUCTION


2.1  PURPOSE AND SCOPE

     The Strategies and Air Standards Division of the Office

of Air Quality Planning and Standards (OAQPS), U.S. Environ-

mental Protection Agency (EPA) has become interested in the

effects of air pollution on water quality.  Preliminary

evidence that air pollutants can have a significant impact

on water resulted in the initiation of a contractual effort

to further document that potential.3

     This report summarizes research related to defining the

effects of air pollutants on water quality.  Runoff of

terrestrially deposited atmospheric pollutants and leaching

or runoff of residuals from air pollution control activities

constitute two indirect effects of air pollution on water

quality.  Direct impacts occur as a result of gas phase

interaction between air and water, dry fallout of aerosols

on water surfaces, and rainout or washout of atmospheric

compounds directly onto water surfaces.   The direct impacts

from trace elements, nutrients, toxic organic compounds, and

airborne acids are reviewed in this report.
a Internal memo by John D. Bachmann and Don Lokey, U.S.  EPA,
  Research Triangle Park, NC.  "Effects of Air Contaminants
  on Water Quality", September 2, 1976.
                            2-1

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     The information in this report was derived from a

literature review and from personal conversations with

researchers.  The sections discussing each of the four major

pollutant categories summarize the extent to which both

quantitative and qualitative data have been reported.  The

report also summarizes required further research and coordi-

nation of interagency research activities.

2.2  EVIDENCE OF ATMOSPHERIC EFFECTS ON WATER QUALITY

     Several organizations other than the U.S. EPA have

conducted research on one or more subjects relating to the

effects of air pollution on water quality.  The most sig-

nificant among these organizations are:

     0    U.S. Department of Agriculture

     0    U.S. Geologic Survey

     0    National Oceanographic and Atmospheric Admini-
          stration (NOAA)

     0    National Space Administration (NASA)

     0    National Science Foundation  (NSF)

     0    International Joint Commission  (coordination of
          U.S. - Canadian studies)

     0    Atomic Energy Commission [now Energy Research and
          Development Administration (ERDA)]

Several of these organizations have carried on research in

this field for some time.  NOAA, for example, has cooperated

with the World Meteorological Organization in precipitation

chemistry studies for several years.
                          2-2

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     The effects of air pollution on water quality have been



studied more extensively in Europe than in the United States.



The preliminary evidence derived from both U.S. and European



studies indicates that a significant proportion of the



atmospheric pollutants that impact on water surfaces are of



anthropogenic origin.  In Europe, the changes in water



quality correlate with changes in the use of fossil fuels



and with increased urbanization and industrialization in



general.  Emissions inventory techniques coordinated with



water and air-quality-sampling projects in the United States



lead to similar conclusions.  Studies from both areas also



indicate that atmospheric input of some pollutants into



lakes represents a significant percent of the total loading



of those pollutants.
                           2-3

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                     3.0  SURVEY RESULTS






3.1  TRACE METALS



     The mechanisms characterizing atmospheric trace-metal



input into lakes are functions of particle size distribution



and particulate aerosol transport and deposition properties.



The literature reviewed indicates that one focus of the



research in this area has been a more precise description of



the physical parameters involved in the atmospheric loading



of trace metals onto lakes.  Field measurements obtained



from the studies that have been performed, however, are not



sufficient to provide a reliable data base.  Although most



of the preliminary data found in this survey do not appear



to be derived from statistically significant field measure-



ments, they do provide evidence that the atmosphere is an



important source of trace-metal input into lakes.  More work



is required to identify sources of each element, to measure



deposition onto lake surfaces, and to build reliable histori-



cal data bases.  From the survey it appears that the most



significant work in the United States has been performed on



the Great Lakes and on the Walker Branch Watershed in



Tennessee.
                           3-1

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3.1.1  Loading Estimates


     Table 1 partially summarizes data reported in one study


of Lake Michigan.   The estimates shown were derived from


emissions data and from National Air Surveillance Network


(NASN) ambient air data for Chicago, Milwaukee, and north-


east Indiana.  The study concluded that the atmosphere may


be a significant source of input of at least nine trace


metals into Lake Michigan:  cobalt, copper, manganese,


nickel, lead, selenium, titanium, vanadium, and zinc.  The


conclusion that an element from the atmosphere may have


significant impact on lake loading was based on the hypo-


thesis that approximately 10 percent of the atmospheric


emissions might be transferred into the water.  Other more


recent estimates of transfer efficiency have ranged as high

                 2
as 20-25 percent.


    Table 1.  ESTIMATES OF POTENTIAL TRACE METAL INPUT TC

                       LAKE MICHIGAN1
Element
Arsenic
Beryllium
Cadmium
Cobalt
Copper
Iron
Manganese
Nickel
Lead
Selenium
Tin
Titanium
Vanadium
Zinc
Stream input,
103 kg/yr
59

6
209
19,958
208
9
91
6

91
26
590
Air emissions
inventory,
10 3 kg/yr a
40
4.5
11
45
2903
78,019
4173
907
1996
18
12
2177
553
3538
Potential loading
air to water"
103 kg/yr
4
0.4
1
4
290
7802
417
91
200
2
1
218
55
354
                                                    •
  Based on pre-1970 data.  Does not reflect p^st-1970 con-

  trol strategy effects.

  Based on an assumed 10 percent transfer efficiency.
                           3-2

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     A study of the Lake Washington Watershed  in western

Washington also included estimates of atmospheric loadings

of six trace metals:  iron, sodium, lead, zinc, copper, and

mercury.  Table 2 summarizes estimated annual atmospheric

input of these metals compared to estimated annual stream

input.  Stream input was estimated from river samples;

atmospheric dnput was estimated by subtracting net fluvial

input from annual sediment input.

         Table 2.  ESTIMATES OF TRACE METAL INPUT TO

                      LAKE WASHINGTON3

                        (103 kg/yr)a
Element
Iron
Sodium
Lead
Zinc
Copper
Mercury
Annual Input
Stream
2331
4917
1
30.8
5
0.06
Air
1996
163
27
13.6
2.5
0.05
  Numbers are approximate and have been converted from
  English units originally reported.
     Neither the Lake Michigan nor the Lake Washington study

is based on extensive field measurements of atmospheric

fallout.  Other studies found in the literature reviewed

provide similar presumptive evidence of the significance of

atmospheric input of metals into lakes or oceans.  A joint

U.S.-Canadian study and a study of the Walker Branch Water-
                            3-3

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shed in Tennessee appear to be most comprehensive in quan-



tifying atmospheric trace-metal input to lakes by using



field measurements.



     A 2-year study of Lake Superior and Lake Huron wag


                   4 5
recently completed. '   The study was coordinated by the



International Joint Commission, and the research was funded



jointly by the United States and Canada.  This study of the



upper Great Lakes was initiated to estimate the annual



atmospheric loadings of 16 pollutants onto Lake Superior and



Lake Huron and to identify the relative contributions from



30 major large-area sources.  A mathematical model was



applied to estimate pollutant loadings.  Precipitation sam-



ples were collected and analyzed from a network of 70 sam-



pling stations on and around the two lakes.  Tables 3 and 4



summarize the mean annual atmospheric loading estimates for



the trace elements analyzed in this study.  Inputs from four



major source categories - direct municipal, direct indus-



trial, tributary, and atmospheric - were estimated for Lake



Superior and Lake Huron.



     The tributary loadings include all upstream sources,



including municipal, industrial, and land drainage.  The



percent contribution of each element from atmospheric load-



ing is expected to increase as cleanup of aqueous point



sources continues.
                            3-4

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      Table 3.  TRACE-ELEMENT  INPUT  TO  LAKE SUPERIOR FROM FOUR MAJOR SOURCE CATEGORIES


                            AS ESTIMATED  IN THE  UPPER LAKES STUDY4


Element
Cadmium
Copper
Iron
Potassium
Magnesium
Sodium
Nickel
Lead
Total Input, 10 kg/hectare (ha)
Direct
municipal
0.024
1.4
74
177
216
847
0.234
0.383
Direct
industrial
3285
10
239
2825
3146
30,733
10
3285

Tributary
351,000
1015
65,335
86,140
361,350
196,000
613
1105

Atmospheric
55,000
369
9700
13,000
5584
15,000
120
650
Contribution from
precipitation, %
13
26
13
13
2
6
16
13
OJ
I
Ul
Does not include dry deposition,
       Table 4.  TRACE-ELEMENT  INPUT  TO  LAKE  HURON FROM FOUR MAJOR SOURCE CATEGORIES


                             AS ESTIMATED  IN  THE  UPPER LAKES STUDY5
                                          Total  Input,  10  kg/ha
Element
Cadmium
Copper
Iron
Potassium
Magnesium
Sodium
Nickel
Lead
Direct
municipal
0.8
7
136
628
668
6680
7
3
Direct
industrial
0.8
6.8
2376
1565
650
10,950
3.7
5
Tributary
796
1358
32,960
76,285
456,250
405,150
1478
1200
a
Atmospheric
79
760
4600
32,000
8200
45,000
210
780
Contribution from
precipitation, %
9
36
11
29
2
10
12
39
       Does not include dry deposition.

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     The atmospheric loading estimates in this study do not

include the potential contribution from dry deposition,

which is the fallout of particulate separate from precipi-

tation events.  If the atmospheric input from dry deposition

is significant, then the total atmospheric contribution of

trace metals to these lakes will be more important than the

results of this study indicate.

     The sampling network used in the Upper Great Lakes

Study is being expanded to include the other Great Lakes.

U.S. EPA Region V has the responsibility for implementing

and operating the surveillance network on the U.S. side.

The expanded Great Lakes surveillance should provide an

expanded data base, one that will allow more comprehensive

estimates of atmospheric loading of trace metals and other

pollutant classes and better validation of models.

     Accurate estimates of dry deposition of particulate

onto the Great Lakes will require refined sampling method-

ology.  To date, most work to characterize dry deposition

phenomena has been performed in laboratory environments.

Measurements in the field are hindered by problems such as:

     0    contamination by insects and other foreign matter

     0    sample loss from wind currents

     0    restrictions in sampling small particles

     0    a lack of particle size distribution data asso-
          ciated with previous experiments

     0    logistics of operating remote samplers.
                            3-6

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Current estimates of dry deposition are based on emission


inventory and meteorological data applied to mathematical

       126
models. ' '   The deposition functions in the models are


based on laboratory experiments.  Better estimates may be


possible only by refining sampling techniques and emission


inventory techniques.


     A second major study was performed on the Walker Branch


Watershed in Tennessee.   This study was supported by the


National Science Foundation and the U.S. Energy Research and


Development Administration, and the work was performed by


the Oak Ridge National Laboratory, Oak Ridge, Tennessee.


Field data were derived from precipitation, stream, and Hi-


vol samples.  Precipitation samples were collected during


the period from June 1973 to July 1974.  Dry samples col-


lected in July 1974 were analyzed for 34 elements to esti-


mate the elemental concentration in ambient air at ground


level.  Enrichment factors were calculated to relate the


atmospheric concentration of each element to the expected


concentration from natural sources.  This technique provided


estimates of the relative importance of anthropogenic source


contribution to atmospheric concentrations of each element.


     Ratios of cadmium, copper, mercury, lead, and chromium


to manganese were calculated for rain and soils in the


Memphis area and for flyash collected at the Allen Steam


Plant in Memphis.  The Memphis data were the only data avail-


able for this study, and they were determined to be suffi-
                           3-7

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ciently representative of conditions around the Walker
Branch area.  The calculations indicated that cadmium,
copper, mercury, and lead in rain are enriched with respect
to soil in this area; therefore, they must have another
source.  It was concluded that flyash ratios are comparable
to rain ratios for copper and cadmium, and possibly for
zinc.  Chromium appears to be derived from the soil in this
area, and lead is probably derived from automobile exhausts.
Table 5 shows the elemental ratios in rain, soil, and fly
ash.
Table 5.  ELEMENTAL RATIOS IN RAIN, SOIL, AND FLY.ASH IN THE
                  WALKER BRANCH WATERSHED7

Rain
Soil
Fly Ash
Cd/Mn
0.39
0.002
0.12
Cr/Mn
0.11
0.13
2.1
Cu/Mn
1.47
0.043
1.1
Hg/Mn
0.01
6x10-5
0.0001
Pb/Mn
1.8
0.04
0.27
Zn/Mn
3.8
0.7
13.7
     Total input of selected elements from stream sources
and from the atmosphere were compared to total estimated
output.  An estimate was made of total watershed retention
as a function of percent total atmospheric impact of seven
elements.  Table 6 summarizes the trace element mass balance
for the watershed as estimated for the 6-month period Jan-
uary-June 1974.  These estimates are significant, because
they illustrate the possibility of predicting the total
impact on the watershed resulting from an increase in atmos-
pheric concentration of each element.  Predictions of this
type can be valuable in planning future land use in any
geographical area.
                           3-8

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       Table 6.  SUMMARY OF TRACE-ELEMENT MASS BALANCE

              RESULTS FOR JANUARY-JUNE 1974 AT

                  WALKER BRANCH WATERSHED7
Element
Cadmium
Chromium
Copper
Mercury
Managanese
Lead
Zinc
Atmospheric
Input, g/ha
O-
62.4-65.4
22.1
143.4
1.51-1.89
136.7
115.4-171.9
269.4
Total Stream3
Output, g/ha
a
3.5
9.1
23.09-26.37
0.47
59
2.9
67.9-73
Watershed
Retention, % of ,
Atmospheric Input
lod *(*~3)/V
94-95
58.8
82-84
69-75
56.8
97.98
73-75
b,
Total stream output is the combination of dissolved trace
elements and suspended particulate species.


That portion of each element entering the total watershed
and not being exported by the streams as a result of runoff
or direct deposition into the streams from the atmosphere.
     Table  7.   ESTIMATED WET DEPOSITION VS.  DRY DEPOSITION

     OF  SELECTED ELEMENTS IN THE WALKER BRANCH WATERSHED7

                          (July 1974)
Element
Cadmium
Chromium
Copper
Mercury
Manganese
Nickel
Lead
Zinc
Wet
Deposition, g/ha
4.5
0.5
6.5
0.04
4.4
0.9
7.9
16.8
Dry Deposition
g/ha
<0.21
0.13
0.15
<0.01
0.87
-
<3.9
1.7
% of Total Deposition
<4.5
30.6
2.3
<20.0
16.5
—
<33.1
9.2
                            3-9

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     Table 7 shows a comparison of total dry deposition

input to wet deposition input for eight elements.  Dry

deposition estimates are extrapolated from only one month's

data; expanded sampling would be necessary to draw firm

conclusions.  Although based on limited field sampling data,

the preliminary estimates are nevertheless important because

they imply that the contribution to total watershed loading

from the atmosphere is significant for some elements.  This

preliminary evidence also illustrates the need for expanded

studies to sample dryfall deposition over lakes and water-

sheds.

3.1.2  Source-Receptor Relationships

     Determining source-receptor relationships for trace

elements requires an understanding of the emissions from

selected industrial processes and from the combustion of

fossil fuels.  A significant amount of work has been com-

pleted or is under way to characterize the distribution of

trace elements from various industrial processes and from

fossil-fuel-burning sources and to study the atmospheric

distribution of these elements.  An improved means has been

reported for determining elemental chemistry as a function

of particle size using a commercial cascade impactor and the
                                  Q
ion-excited X-ray analysis method.   This has proved to be

an important application for studying the enrichment of
                            3-10

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trace elements during fossil fuel combustion.  Other studies



concentrate directly on characterizing removal efficiencies



and on the enrichment and particle size distribution rela-



tionships of trace element emissions from fossil fuel com-



bustion.9'10'11'12'13  All of these studies are important



for understanding the potential loading of the atmosphere,



and consequently of water surfaces, with trace elements from



combustion sources.



     The expected impact of trace-element atmospheric emis-



sions on surface-water trace-element concentrations appears



to be a function of land-use configuration, of industry-type



distribution, and of fuels burned within an area.  A recent



study of power plant boilers indicates that trace metals are



volatilized and enriched during coal combustion.    In



addition, aerosol studies of six U.S. cities indicate that a



significant percentage of the particle mass of aerosols in



selected cities exists in the size fraction less than 2



micrometers (ym) diameter.   These observations are signifi-



cant because they provide preliminary evidence that long-



range transport of particles enriched in trace elements,



i.e., the smaller particles that may escape some conventional



control devices like electrostatic precipitators, presents



a potential threat to water quality.  This potential threat



might remain regardless of the degree to which major fossil-



fuel-burning plants control their emissions.



     The Upper Great Lakes study estimated trace-element



loadings by applying an atmospheric transport model.  The





                           3-11

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particulate emissions from 30 major source areas were input



into the model as trace-element constituent emissions.  The



trace-element constituent emissions were estimated by



applying a constituent fraction matrix, derived from a



literature survey, to the emissions categorized by major



industrial groups for each major source area.  The study



concluded that major trace-metal input to Lake Superior came



from Chicago, Cincinnati, and the State of Michigan, and the



major trace-metal input to Lake Huron came from Detroit,



Saginaw, and Cincinnati.  This is the only study reviewed in



this survey in which estimates were made of trace-element



contribution from sources beyond the immediate area of the



body of water in question.



     The Walker Branch Watershed study included a consid-



eration of minimum atmospheric discharges from coal-fired



steam plants in the Oak Ridge area.  The purpose was to



derive enrichment factors to distinguish between relative



contributions from anthropogenic sources and from natural



sources.  A comparison of aerosol enrichment factors to fly



ash enrichment factors led to the assumption that atmos-



pheric levels of seven trace metals in this study were



significantly influenced by the power plants in the area.



     Better estimates of source-receptor relationships,



especially in the Walker Branch Watershed study, might have
                           3-12

-------
been possible with better sampling time resolution and



particle size distribution sampling.  Estimating specific



source contributions to an area such as the Upper Great



Lakes may not be possible using current techniques; or, if



possible, it may be too expensive.  An area like the Walker



Branch Watershed appears to be better suited for source-



receptor research because it is influenced by a relatively



few large emission sources, thus allowing the collection of



more precise source emissions data.



3.1.3  Effects of Trace Elements on Water Quality and

       Aquatic Ecosystems



     Little information is available on the effects of trace



elements on aquatic life.  One theory proffered on the



effect of acidification on aquatic life is that extinction



of fish populations is caused by heavy metal toxicity thab



results from low pH.  Zinc concentrations were considered to



be potentially hazardous to fish in the LaCloche Mountain


                             14
lakes, near Sudbury, Ontario.    Other metals appeared to be



present in safe concentrations in this area.



     Mosses dependent on atmospheric sources for a large



portion of their mineral supply have been shown to be strong-



ly contaminated with cadmium, nickel, chromium, and mercury



in southern Scandinavia.    Sphagnum mosses appear to in-



crease in density in lakes where acidification is a prob-



lem.    These mosses cover sediments and retard recycling of
                           3-13

-------
metal cations from the sediments, thereby depriving other



species of the aquatic system of an important source of



trace metals.



3.2  NUTRIENTS



     Lakes naturally evolve from an oligotrophic (nutrient-



poor) to a eutrophic (nutrient-rich) state.  Nitrogen and



phosphorous are usually considered the most important



nutrients in the eutrophication process.  In some lakes



phosphorous is the nutrient that contributes most to eutro-



phication, i.e., is the limiting factor; in other lakes,



nitrogen.  Nitrates and phosphates are important plant



nutrients, and their presence affects the rate of growth of



many aquatic plant species.  As algae die they sink and



decay, consuming dissolved oxygen in the water and releasing



nutrients for more plant growth.  The decrease in oxygen and



increase in temperature from decaying plant life signifi-



cantly inhibit or alter other types of aquatic life, spec-



ifically commercial and sports fish.  Nutrient concentra-



tions that accelerate the growth of the algae accelerate the



total rate of oxygen depletion.



     The eutrophication process can be accelerated by such



human activities as fertilization of agricultural land;



discharge of pollutants from point sources into lakes,



rivers, and streams; and pollution of the air.  Several



extensive studies provide evidence of increasing harmful
                          3-14

-------
effects on lakes resulting from human activities.  Input of



nitrogen and phosphorous from the air can come from wind-



blown dust from fertilized soil, from direct fallout of



pollutant emissions from fossil fuel combustion, and from



precipitation scavenging.  Dry deposition input of nitrogen



and phosphorous to lakes has been modeled, but extensive dry



sampling has not been done.



     Most of the literature reviewed in this survey indi-



cates that the nitrogen content of precipitation is signifi-



cantly greater than the phosphorous content; and precipita-



tion seems to be a more important surface-water source of



nitrogen for than it is of phosphorous.  The National Eutro-



phication Survey of the U.S. Environmental Protection



Agency, Corvallis, Oregon, has studied lakes throughout the



United States in an effort to determine their trophic status



and to identify the factors contributing most to their eutro-



phication.  A sample of six working papers by the National



Eutrophication Survey were reviewed in this project.  These



papers indicate that the percent precipitation input of both



nitrogen and phosphorous into five of six lakes studied in



New Jersey and Indiana is negligible.17'18'19'20'21'22



Conversely, a study of the Rhode River, a subestuary of



Chesapeake Bay, indicates that precipitation input of



nitrogen into the estuary, along with input from distant
                            3-15

-------
                                                          23
point sources, maintains the estuary in a eutrophic state.



The watershed has no significant point sources, and the



percent nitrogen contribution from runoff is negligible.



Studies of the Great Lakes also show that precipitation can


                                     324
be a significant source of nutrients. '     The degree to



which various point sources and nonpoint sources contribute



to lake eutrophication appears to depend on regional land



use, stream interactions, and land, soil, and vegetation



characteristics.  This review provides strong evidence that



the atmosphere can be a significant nutrient source.



3.2.1  Loading Estimates



     Estimates from studies on the Great Lakes indicate that



precipitation contributions of phosphorous and nitrogen



represent a significant portion of the total lake loadings



of those elements.  One study of Lake Michigan indicates



that approximately 13 percent of the phosphorous entering


                               25
the lake is from precipitation.    The study estimates that



the contribution from precipitation will be as high as 30



percent when the program to control 80 percent of wastewater



phosphorous input is completed.  Phosphorous appears to be



the limiting nutrient in this lake.  This study did not



measure dry deposition; neither did it address the problem



of source identification.
                           3-16

-------
     The Upper Great Lakes Study  includes estimates of the


total precipitation input of nitrogen and phosphorous to


Lake Superior and Lake Huron, as summarized in Tables 8


and 9.  Dry deposition estimates are not included.  Accord-


ing to the study, a large portion of the total phosphorous


loadings on Lake Superior come from the Chicago area; on


Lake Huron a significant amount emanates from Chicago, Detroit,


and Cincinnati.  Estimates of pollutant-loading contribu-


tions from 20 U.S. cities and from 10 Canadian sources were

                                           4
derived from a long-range dispersion model.   The model


loading estimates were compared to precipitation chemistry


results for several elements.  The authors indicate that


they obtained reasonable agreement between precipitation


chemistry data and predicted values, considering the ac-


curacy limits of the methods.


     Nutrient levels in precipitation have been measured in


many studies.  Most appear to be short-term sampling studies,


usually 1 to 2 months or less, and care should be taken not


to generalize from these results.  The studies do not at-


tempt source identification, nor do they include dry deposi-


tion sampling.


     Gaseous flux of nitrogen as ammonia has been shown to


be significant around cattle feedlots.  Studies by the U.S.


Department of Agriculture show that ammonia volatilized from
                           3-17

-------
        Table  8.   NITROGEN AND PHOSPHOROUS INPUT TO LAKE SUPERIOR FROM FOUR MAJOR SOURCE


                     CATEGORIES AS ESTIMATED IN THE UPPER GREAT LAKES STUDY5
Element
Nitrogen
(total as N)
Phosphorous
(total as P)
Total Input, 103 kg/yr
Direct
municipal
500
132.5
Direct
industrial
565
99
Tributary
36,000
2832
Atmospheric
55,845
799
Contribution from
precipitation, %
60
21
U)
I
M
00
             Table 9.   NITROGEN AND PHOSPHOROUS INPUT TO LAKE HURON FROM FOUR MAJOR


                  SOURCE CATEGORIES AS ESTIMATED IN THE UPPER GREAT LAKES STUDY5
                                              Total Input,  10  kg/yr
Element
Nitrogen
(total as N)
Phosphorous
(total as P)
Direct
municipal
1044
190
Direct
industrial
7081
81
Tributary
58,830
4416
Atmospheric
51,830
620
Contribution from
precipitation, %
44
12

-------
cattle feedlots is absorbed by nearby surface waters.  A



study of northeastern Colorado feedlots attempted to deter-



mine the rate at which ammonia is absorbed directly from the



air at various distances from feedlots under different


                       2 6
atmospheric conditions.    The study concluded that the



amount of atmospheric washout of nitrogen was not large



compared to the direct absorption of ammonia by the water



surface.  Effects were measured as far as 2 km from the



feedlot.  A study in Georgia produced similar results and



indicated that the nitrogen contribution to streams and



soils by ammonia absorption from the atmosphere appears to


                                   27
be greater than from precipitation.    The Georgia study



also indicated that fertilizer nutrients in precipitation



were negligible when compared to the content of the elements



in the soils.



     Estimates of NO  flux by washout and rainout, dry
                    X


deposition, and gaseous deposition are documented in the



literature; however, our survey of this literature indicates



the estimates are usually global in scope and based on NO
                                                         **


absorption rates and reactions derived from laboratory



experiments.  The survey produced no information on NO
                                                      H


contribution of nitrogen to specific water surfaces.
                           3-19

-------
3.2.2  Source-Receptor Relationships



     The nitrogen cycle is one of the most familiar ele-



mental cycles in nature.  Oxidized or reduced forms of



nitrogen undergo a variety of chemical and biochemical



transformations.  Reduction of nitrate or nitrite occurs



when these species are absorbed by plants or animals and are



converted to plant or animal tissue.  When the plant or



animal tissue dies and is returned to the soilr microbial



oxidation converts the nitrogen back to nitrate.  Nitrate



added to the soil in excess quantities required by plant



uptake or losses by denitrification is subject to leaching



and can be carried by percolating water into the ground



water system and ultimately into streams and lake systems.



Precipitation scavenging of nitrogen compounds can add to



the total nitrate content directly and indirectly through



soil leaching.  Global estimates have been made of the


                                                  28
quantities of nitrogen present in the environment.    These



estimates indicate that natural sources of nitrogen con-



tribute more nitrogen to the soil and water than do pollu-



tion sources.  Studies in Europe and in the United States



indicate that increased industrial or agricultural activity



can contribute to increased levels of nitrogen compounds in



the atmosphere.   A 10-year study of the Hubbard Brooke



Experimental Forest in New Hampshire shows that nitrate
                          3-20

-------
concentration in precipitation and input of nitric acid are


                       29
increasing in the area.    Precipitation nitrate concentra-



tion changes correlate well with increased nitrogen oxide



emissions from combustion of fossil fuels.  This correlation



provides presumptive evidence that increased industrial



activity can increase nutrient loadings in the atmosphere,



with a potential for subsequently increasing the nutrient



levels in bodies of water.  The literature indicates, how-



ever, that the evidence is only presumptive, and atmospheric



reactions may be contributing to the changes in nitrate



concentrations.  These atmospheric reactions, which result



in acid precipitation, require further research.  Very high



correlations have been shown between the total input of



sulfate and nitrate concentrations into the Hubbard Brooke



Experimental Forest and the annual input of sulfate and



nitrate ions from precipitation over the 10-year period from



1964 to 1974, indicating the importance of the atmosphere as



a source of these ions.



     A study for the U.S. Department of the Interior pro-



vided estimates of probable sources of atmospheric phos-



phorous in the Chicago area.    The estimates were derived



by determining elements that could be used as tracers for



specific industries emitting particulates and the atmos-



pheric concentrations of those elements.  An estimate of



relative contributions of each source category was made from



estimated source contributions to total particulate concen-
                           3-21

-------
trations, precipitation sample analyses, and estimates of



percent phosphorous for particulate emissions from each



industry.  This study concluded that the atmosphere contrib-



utes from one-fifth to one-third of the phosphorous going



into Lake Michigan and that 60 percent of the atmospheric



phosphorous input is from anthropogenic sources.  The major



source categories considered were:  (1) phosphorous indus-



try, including phosphate rock mining, phosphoric acid manu-



facturing, and fertilizer manufacturing; (2) iron and steel



manufacturing; (3) cement manufacturing; (4) refuse incinera-



tion; and (5)  fuel oil and coal combustion.  Agricultural



burning and forest fires were not considered.  Although



problems exist with the source identification technique,



this study is the only one found in this survey, except the

   a

feelot studies, that attempted to identify atmospheric

   A

nutrient sources.



     Around croplands, runoff is considered to be a more



significant source of nutrient loading than precipita-



tion.  '  '     No references to the windblown agricultural



dust potential for nutrient loading of water surfaces were



found in this survey.  Loading factors have been determined



for assessing water pollution potential from nonpoint


        32
sources.    The loading factor for phosphorous does not



include a term for either precipitation or windblown dust.



The function for nitrogen includes a term for precipitation
                          3-22

-------
but not for windblown dust.  Although fugitive dust from

agricultural tilling operations has been sampled, sufficient

work has not been done to characterize either the particle

size or elemental distribution of agricultural fugitive

dust.  Water-surface nutrient loadings from agricultural

dust could be significant in high-agricultural areas, and

the potential loading warrants investigation.

3.3  TOXIC ORGANICS

     Toxic organic compounds have been measured both in air

and in water.  The compounds most often cited in the liter-

ature are polychlorinated biphenyls (PCB's) and pesticides,

specifically DDT and related compounds.  The U.S. EPA Office

of Pesticide Programs, in cooperation with the U.S. Geologic

Survey, compiles data on surface water samples four times

annually and on sediment samples twice annually from 150

sampling points nationwide.3  The pesticides and herbicides

of interest in this program are primarily water-insoluble

compounds; consequently, significant amounts of pesticides

have not been found.  The Office of Pesticide Programs is

currently conducting an air- monitoring program for pesti-

cides.

     Although water-soluble pesticides in urban aerosols

have been measured, it is not clear whether these are in the

vapor phase or if they are adsorbed on particulates.
  Personal conversation with Mr. Fred Kutz, U.S. Environmental
  Protection Agency, Office of Pesticide Programs, Washington,
  D.C.

                         3-23

-------
     Extensive surface organic films or microlayers have



been observed in freshwater lake systems, but the rela-



tionships between organic compounds in air and the nature of



these organic microlayers have not been established.



     Many pesticides have a high affinity for soil parti-



cles.  Agricultural runoff, then, is an important source of



pesticide pollution of surface water.  The deposition of



windblown particles on water surfaces has apparently not



been studied in relation to pesticide loading levels.  The



potential of long-range transport of pesticide aerosols,



however, is illustrated by Table 1.0.    Solubility, vola-



tilization, leaching, and surface runoff properties of


                                        32
leading pesticides have been documented.
       Table 10.  DRIFT VS. PARTICLE SIZE PESTICIDES
                                                    35
Particle
type
Aircraft spray
Coarse
Medium
Fine
Air carrier sprays
Fine sprays/dusts
Usual dusts/aerosols
Aerosols
Diameter, ym
400
150
100
50
20
10
2
Drift, a
meters
2.6
6.7
15
54
338
1352
33,795
  Distance particle would be carried by a 4.8 km/hr wind

  while falling 3 meters.
                           3-24

-------
     PCB deposition into Lake Michigan is a current research


      25
topic.    PCB's have been detected in Lake Michigan fish,



and they are a threat to selected fish species in the lake.



Sampling is being conducted to determine the amounts of



PCB's present in precipitation and in the air.  Current



research is hindered by sampling problems and by the many



possible species of PCB's.  Preliminary estimates indicate



that 725 kg/yr of PBJC's are input to Lake Michigan from aqueous



point sources and 645 kg/yr from precipitation.



     A study was conducted from 1972 to 1974 to determine



sources and input rates of PCB's into the Southern California



Bight.    The sources of PCB's investigated were municipal



wastewater, surface runoff, aerial fallout, industrial



discharges, antifouling paint, harbor flushing, and ocean



currents.  The major sources proved to be municipal waste-



water and aerial fallout.  Table 11 summarizes the results



of the study.  The estimates of aerial fallout were derived



from sampling data collected from a network of glass sam-



pling plates sprayed with a mixture of 5:1 hexane and min-



eral oil and exposed for approximately 1 week.  Five sam-



pling stations were used for three 1-week sampling intervals,



with an estimated collection efficiency of 50 percent.  The



significance of this survey is that it points to the atmos-



phere as a primary source of PCB input to water systems.
                           3-25

-------
             Table 11.  ESTIMATED INPUTS TO THE

                 SOUTHERN CALIFORNIA BIGHT36
Route
Municipal wastewater
Surface runoff
Aerial fallout
Industrial discharges
Antifouling paint
Harbor flushing
Ocean currents
Year
1974
1972-73
1973-74
1973-74
1973
1974
1973
PCB ' s , kg/yr
1242*
4300
£550
-
£180
<1
-
-
1254a
1100
250
1800
60
<1
<150
4000
Total
5400
£800
-
<250
<1
•
-
  PCB mixtures with gas chromatographic profiles most
  closely resembling those of Aroclor 1242 and Aroclor 1254.
     The Office of Water Planning and Standards of the U.S.

EPA is currently conducting research to determine safe

levels of toxic substances in water.   They are also trying

to identify areas in which transfer of toxic substances

between air and water appears to be significant.  They will

try to accomplish this by integrating historical data from

air, precipitation, and surface water with sediment analyses.

Part of this total effort includes the development of reli-

able sampling methods for toxic organic substances.
  Personal conversation with Mr. Rober Greenspu|A> Water Qual-
  ity Analysis Branch, Monitoring and Support Division, Office
  of Water Planning and Standards, U.S. EPA, Washington, D.C.
                           3-26

-------
     The two-year study of the upper Great Lakes  included

the study of organic compounds.  Organics entering the Great

Lakes can be classified as follows:

     0    Compounds that readily degrade biologically or
          chemically reducing the available oxygen levels.

     0    Compounds that bioconcentrate and may be directly
          toxic to aquatic life or metabolized to a more
          toxic form in higher organisms, e.g., PCB's and
          DDT.

     0    Compounds that cause taste and odor problems in
          commercially important aquatic species.

Studies of Lake Huron and Lake Superior fish revealed that

fish from both lakes contained detectable concentrations of

PCB's.  Samples of rainbow trout from Lake Huron and a

subspecies of lake trout from Lake Superior frequently show

levels of PCB's in excess of Canadian or U.S. food guide-

lines.  DDT residues are still found in fish in Lake Supe-

rior despite past efforts to control DDT contamination, and

available data provide no evidence that DDT levels have

declined in Lake Superior fish during the past five to six

years.  An 80 percent reduction of DDT residues in fish in

Lake Michigan has been noted since the use of DDT was banned

in 1969-70 in the states bordering the lake.   DDT was

banned in Canada in 1970 and its ban was extended nationwide

in the United States in 1972.

3.4  AIRBORNE ACIDS

     Acid precipitation has been studied extensively in both

the United States and Europe for several years, and its

effects on ecosystems is documented in the European litera-


                           3-27

-------
ture.  The atmospheric chemistry of acid formation is also


                                                    37
documented.  A recent review by a leading researcher   indi-



cates that strong acids such as sulfuric, nitric, and



hydrochloric dominate the acid precipitation chemistry in



most of northeastern United States and northern Europe, and



that anthropogenic sources are the major causes of acid



precipitation in these regions.  Results of acid precipita-



tion studies in Norway show a relationship between atmos-



pheric concentration of sulfate ions in precipitation and



lake water acidity.  Consumption of fossil fuels in Europe,



increased acidity of precipitation in southern Norway, and



an increase in the number of barren lakes there also seem to



show a correlation.  The pH of precipitation in much of



northeastern United States is reported to average between



4.0 and 4.2 annually.  Values between 2.1 and 3.0 have been



reported during storms in some regions.



     Significantly more literature is available dealing with



acid precipitation and its effects than is available for the



other pollutant categories discussed in this report.  Pro-



ceedings of the First International Symposium on Acid Pre-


                                   38
cipitation and the Forest Ecosystem   documents a large



volume of work on this subject.  Most of the information



reviewed and summarized herein is qualitative rather than



quantitative.   The following sections summarize the kinds of



results that have been reported.
                          3-28

-------
3.4.1  Acid Precipitation Effects on Lake Chemistry



     A large volume of acid precipitation work has been done



around the Sudbury area in Canada, at the Hubbard Brooke



Experimental Forest in New Hampshire, and in Norway.  Water



quality data for 150 lakes within a 100-km radius of Sudbury


                                    39
were collected during 1974 and 1975.    Surface water pH



varied between 4.0 and 8.5.  Lakes in the lowest pH zone in



the study area have low buffering capacity and are oriented



in line with the predominant wind direction that blows from



the Sudbury smelting complex.  High concentrations of .



metals associated with the smelter emissions were found in



these lakes, compared with low concentrations normally found



in air, water, and soil, which would indicate that Sudbury



smelting emissions significantly affect the water quality of



these lakes.  High S02 emissions from the smelting opera-



tions are probably responsible for the pH depression in



these lakes.  Acidification of lakes in this area has re-



sulted in the extinction of several fish species.  The



mechanism of toxicity has not been determined.



     The longest record of precipitation pH in the United



States is for the Hubbard Brooke Experimental Forest, which



is maintained by the U.S. Forest Service.  Mean annual pH of



precipitation in this area between 1964 and 1974 was re-


                               29
ported to be from 4.03 to 4.21.    The annual input of
                            3-29

-------
hydrogen ion increased 36 percent in the same period.  Pre-


cipitation chemistry data indicate that precipitation in the


eastern U.S. was already acid by the 1950's, and more recent


data show a southwestward and westward extension of the re-


gion of acid precipitation since the mid-1950's.  Comprehen-


sive precipitation chemistry data necessary to characterize


the entire nation are not available.  The contribution of


sulfate to the ambient acidity of precipitation in this area


is reported to have decreased from 83 percent in 1964-65 to


.66 percent in 1973-74; the contribution of nitrate increased


from 15 percent to 30 percent.  Reasons for the increased


nitrate concentration have not been firmly established, but


the increased nitrate concentration parallels increases in


amounts of fossil fuels burned in the area.  Contributions


from nitrogen fertilizers have not been determined.


     Precipitation chemistry has been extensively monitored

                                           40
throughout Europe for the last two decades.    At most


stations the pH trend is downward.  During the same period


nitrate in precipitation shows a pronounced increase.


Although the sulfur content of precipitation has increased


steadily while the pH has decreased, the correlation coeffi-


cient calculated between these data trends is not high.


Chemical or meteorological interferences may influence


short-term data irregularities.


     Extensive water quality testing shows a decrease in pH


of surface waters in Scandanavian countries over several
                         3-30

-------
years.  Low soil buffering capacity and increased acidity of

precipitation are shown for the same regions.

3.4.2  Acid Precipitation Effects on the Aquatic Ecosystem

     In the United States, Canada, and Europe studies have

been performed on entire lake systems to characterize the

effects of acid precipitation on aquatic life.  A 1974

survey of 155 lakes in Norway shows that unpolluted lakes in

granitic basins in central Norway have pH values above 6.0,

and bicarbonate is the major anion.    On the other hand,

lakes in large areas of western, southern, and southeastern

Norway have pH values below 5.0, and sulfate has replaced

bicarbonate as the major anion.  This would seem to imply

that the sulfate is derived from sulfuric acid in precipita-

tion since the lakes in these regions have minimal local

sources of pollution.  The conclusions drawn from the study

of these lakes are summarized as follows:

     0    Bacterial decomposition is retarded at low pH
          levels.  Decomposition of cellulose is reduced 50
          percent when the pH is lowered from 7.0 to 5.2.
          Inhibition of decomposition results in an in-
          creased accumulation of organic debris and a de-
          creased rate of nutrient cycling.

     0    Fewer species of phytoplankton and zooplankton are
          observed in water with a pH around 6.0 or less.
          This is true in both Norway and Sweden.

     0    Some aquatic vertebrates that are important as
          fish food are inhibited or absent in low-pH water.

     Data on 79 rivers throughout Norway indicate that the

salmon population in nine of the rivers declined to zero

between 1885 and 1968.  These nine rivers are highly acidic,
                           3-31

-------
with a pH range of 4.5 to 5.5.  Of 2083 lakes studied in



Sorlandet, 741 have no fish, and 516 in which the pH is



around 5.5 or lower, either have no fish at all or their



numbers have been greatly reduced.  The disappearance of



fish in most lakes occurs over a period of many years.  In



some instances, however, a shock effect from a sudden de-



crease of pH can result in massive fish kills.  This effect



is related to the melting of snow and ice accumulating from



winter acid precipitation.


                                41
     In the Adirondack Mountains   in the United States,



fish populations have been adversely affected by acidifica-



tion in approximately 75 percent of the high-elevation



lakes.  The effects range from extinction to alterations in



density, size, structure, and growth rates of fish popula-



tions.



     The lakes in the LaCloche Mountains near Sudbury,


                                14
Ontario, have also been studied.    These lakes are believed



to be significantly impacted by air pollution from the



Sudbury smelting complexes.   Sulfate in these lakes repre-



sents approximately 90 percent of the anions compared with



approximately 40 percent in the Experimental Lakes Area in



northwestern Ontario.  A survey of 150 lakes in the LaCloche



Mountain area shows that 33 lakes had a pH of 4.5 or less,



and one-half of the lakes had a pH of 5.5 or lower.  Differ-



ent species of fish apparently respond to different levels
                         3-32

-------
of acidification.  Reproduction appears to be the most


sensitive physiological process affected in fish popula-


tions.  According to this study, the extinction of fish did


not appear to be an indirect effect of an earlier loss of


food items.  Major prey species remained abundant, while


some predator species became extinct.  It is possible that

                                                  'A
acid stress may have caused reduced feeding or fooj£ utiliza-

tion or both in some species.  It was «e* noted that normal

calcium metabolism may be affected by acid stress.
                          3-33

-------
            4.0  CONCLUSIONS AND RECOMMENDATIONS





4.1  CONCLUSIONS



     A significant amount of research on air/water inter-



actions is documented in the literature reviewed.  More work



has been done in Europe, especially in the Scandinavian



countries, than in the United States and Canada.  A large



proportion of the Scandinavian work deals with acid precipi-



tation.  The Scandinavian studies conclude that a signifi-*



cant volume of pollutant input into lakes and watersheds is



transported through the atmosphere and probably originates



from anthropogenic sources.



     Studies in the United States and Canada support these



conclusions, although few long-term, i.e. one year or longer,



studies have been conducted in either country.    Studies of



the Great Lakes, the Walker Branch Watershed in Oak Ridge,



Tennessee, and the Hubbard Brooke Experimental Forest in New



Hampshire comprise the most significant work reviewed.



     In making this survey, PEDCo found more estimates of



atmospheric input of trace metals and nutrients into lakes



and watersheds than of airborne acids and toxic organic



materials.  The sampling and analytical techniques for



particulates are better developed than are those for air-
                          4-1

-------
borne acids and vapor-phase organic materials.  Vapor-phase



organic pollutants present sampling and analysis problems,



primarily because they are usually present in very low



concentrations in large volumes of air, because they have a



reactive nature, and because they are susceptible to adsorp-



tion.  Most estimates of source contributions to total



atmospheric input of pollutants to lakes and watersheds



result from the application of emissions estimates and



meteorological data to atmospheric transport models.  These



source contributions, consequently, are first-order esti-



mates.  The best estimates of source contributions appear to



be those made for the Walker Branch Watershed.



     Estimates of atmospheric loading onto water surfaces



are usually based on precipitation studies.  An estimate of



dryfall input is usually not included.  Extensive sampling



for dryfall has been hampered by sampling methodology prob-



lems.  Precipitation scavenging effects vary by pollutant,



and it is reasonable to believe that dryfall effects also



vary considerably by pollutant.



     Effects of atmospheric pollutants on biota appear to



have been studied more extensively in Europe than in the



United States and Canada.  Pollutant effects on water quality



and on the biota seem to depend partly on the buffering



capacity of the water.  The most significant effects of acid
                         4-2

-------
precipitation on water quality and biota are observed in

poorly buffered lakes.  The mechanism of toxicity of biota

in lower pH waters is not understood.  It may involve metal

toxicity that manifests itself below a specified pH.

     Our evaluation of all factors that have been reported

and discussed indicates that expanded research is required

to accomplish the following tasks:a' 'c

     0    Identify sources and relative source contribu-
          tions.

     0    Sample dry deposition of pollutants onto water
          surfaces.

     0    Expand the data base.

     0    Determine cross-media impacts.

     0    Define the effects of altered water quality for
          various pollutants.

The following sections expand upon these general research

requirements and cite current related projects.

4.1.1  Source Identification

     Current estimates of source contributions of atmos-

pheric pollutants to water quality are based on emission
a
  Personal conversation with Dr. Martin Bratzell, Interna-
  tional Joint Commission, Windsor, Ontario.

  Personal conversation with Mr. Floyd Elder, Canada Centre
  for Inland Waters, Burlington, Ontario.

c Personal communication with Dr. Michael Mullin, U.S. EPA
  Grosse lie Laboratory, Gross lie, Michigan.
                            4-3

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inventory techniques.  Some work has been done to character-


                   42 43 44
ize urban aerosols.  '  '    Most of these studies, however,



concentrate on identifying trace elements as a function of



total particulate loading.  Source identification adequate



for predictive modeling of trace element transport and depo-



sition onto lake surfaces requires expanded knowledge of



emissions from specific source types, the elemental compo-



sition of those emissions, and the distribution of elements



as a function of time and particle size.  Industrial sources


                                     45 46 47
of trace metals have been documented,   '  '   and major



efforts to characterize trace element emissions and their



fate in the atmosphere are under way.  The National Science



Foundation Research Applied to National Needs (NSF-RANN)



program has funded research related to trace contaminant


                                    48
emissions and atmospheric transport.



     Current research on the emission and fate of trace



elements includes studies of power plant emissions.  '



Fossil-fuel-fired power plants are a major source of trace



elements in the atmosphere, and the characterization and



atmospheric distribution of emissions will become increas-



ingly important as coal becomes a more important fuel.



     The techniques currently used to study urban aerosols



include analyses of Hi-vol samples for multiple elements.



Mass-balance approaches, using calculated enrichment factors



for various source categories and paired correlation co-
                           4-4

-------
efficients in conjunction with reference elements, have



provided the most data in the United States.  Expanded



sampling and analyses are needed for further characteriza-



tion of these aerosols in terms of particle size distribu-



tion.



4.1.2  Dry Deposition Estimates



     Most information on the process of dry deposition of



pollutants onto water surfaces comes from laboratory studies.



Consequently, deposition functions used in models also are



based on laboratory studies.  Since it is difficult to



simulate actual lake conditions in the laboratory, these



model functions may not be accurate.  Increased field mea-



surements of dry deposition over lakes is required for



validation of the current models.   Sampling experiments



should consider fluxes in micrometeorological conditions and



pollutant concentrations.  Based on current knowledge of the



mechanisms by which pollutants are transferred from air to



water, large-scale efforts to develop models appear to be



premature.



     Improved sampling and analysis methods are required.



Limitations of current dryfall sampling techniques have been



a major problem in estimating input to lake surfaces by dry



deposition.  Hi-vol sampling and particle sizing have not



been used extensively in lake studies.  Average aerosol
                           4-5

-------
composition with respect to time and particle size, however,



is needed to estimate rates of dry deposition.    Proton-



induced X-ray emission (PIXE) analysis has been suggested as



an analytical technique capable of providing the broad data



base needed to develop and validate predictive models.



     Direct sampling from shipboard or platforms on the



Great Lakes has been suggested.  Parallel sampling programs



at various locations throughout the Northern Hemisphere have



also been suggested.



4.1.3  Expand the Data Base



     Expanded data bases are required for precipitation



chemistry as well as for estimating the effects of dry



fallout.  The current expansion of the precipitation sam-



pling network around Lake Superior and Lake Huron to cover



the remaining Great Lakes should significantly improve the



current data base.  Dryfall samplers are also being used in



this network, but, as stated before, the dry sampling tech-



niques need improvement.   Permanent sampling networks around



other lakes in the United States and Canada would be useful.



4.1.4  Determine Cross-Media Impacts



     The direct impact of air pollutants on water quality



appears to be significant.  The enrichment of heavy metals



on the smaller particulates that escape collection by con-



ventional control devices on fossil-fuel-fired boilers is an
                           4-6

-------
example of the type of problem that should be addressed.


The impact of pollutant fallout, both dry fallout and


precipitation scavenging, on land-runoff loading of water


bodies is another example of a problem that has not been


assessed.


     Indirect impacts from air pollutants include the impact


of combustion and air-pollution-control residuals.    The


soluble portions of ash and scrubber sludge represent a


potential problem for both ground water and surface water


quality.


     The U.S. EPA recognizes the potential for intermedia


effects of control technology for air pollution.  Recent


studies have been conducted to define these effects and to

                                                         52 53
develop a methodology for evaluating cross-media impacts.  '


A preliminary effort to develop a methodology for evaluating


cross-media impacts resulted in an environmental degradation


index for each possible combination of pollution-control


measures by plant or industry.  This was a joint project of


the Council on Environmental Quality and the U.S. EPA.


Example applications to kraft pulp mills and coal-fired


power plants have been documented.


4.1.5  Define Effects


     Defining the problem of fallout of air pollutants on


water surfaces requires more than measuring loading impacts;
                        4-7

-------
it also requires long-term assessment of the effects.  For

instance, the effects of air pollutants on aquatic life have

not been studied extensively in the United States.  One

proposed approach is to study the effects on the entire

ecosystem rather than just those on water.  This approach

may be more meaningful in defining cross-media impacts than

fragmented research on separate segments of the ecosystem

would be.  Studies of watersheds presently tend to concen-

trate on runoff and point-source impacts and to ignore the

impact of atmospheric input.  Inclusion of atmospheric

considerations in these watershed projects would provide an

significant extension of current knowledge.

4.2  RECOMMENDATIONS

     The status and nature of air/water research are sum-

marized as follows:

     0    Too little emphasis is placed on studying the
          effects of air pollutants on the ecosystem.

     0    The lack of a large-scale monitoring network for
          precipitation chemistry studies hinders trends
          assessments and studies of cause/effect rela-
          tionships.

     0    Too many small-scale projects are being funded by
          agencies that do not coordinate with other agen-
          cies that are funding the same type of research.
          The result is significant duplication of effort.
          A central clearing house to coordinate the re-
          search is needed.

     0    Development of models is premature, and emphasis
          should be shifted to defining and solving basic
          pollutant transport and interaction problems.
                           4-8

-------
     The International Joint Commission has categorized

                                                            54
current research needs as critical, essential,  or necessary.

These categories are used in the following list.

Critical

     0    Development and design criteria for an effective
          and efficient monitoring system for ecological
          needs

     0    Optimization of design and operation of monitoring
          programs

     0    Determination of sources of chlorinated organics

     0    Determination of the behavior and fate of chlo-
          rinated hydrocarbons

     0    Development of an analytical and sampling method-
          ology for toxic elements

     0    Identification of source inputs of toxic elements

     0    Determination of methods and rates of transport
          and dispersal of toxic elements

     0    Identification of the fate of toxic elements in
          the water environment

     0    Determination of the dynamics of PCB's within the
          Great Lakes ecosystems

     0    Determination of contaminant budgets in the Great
          Lakes:  sources, fluxes, transformations, and
          sinks

     0    Determination of air/water interface actions.

Essential

     0    Determination of inshore-offshore energy and
          materials transport

     0    Identification and monitoring of potentially
          dangerous organic compounds
                           4-9

-------
     0    Determination of the dynamics of potentially
          dangerous organics in the Great Lakes

Necessary

     0    Identification of sources of halogenated pesti-
          cides to the Great Lakes

     0    Investigation of the environmental dynamics of
          halogenated pesticides.
                                           a ^r\ ft
     Conversations with leading researchers ' '  working on

the subject of air pollutant effects on water quality con-

firm our conclusions that the major problems that should

receive research priority are:

     °    Expand monitoring programs to build a national
          trends data base.

     0    Refine the sampling methodology to include reason-
          ably accurate estimates of dryfall input.

     0    Develop a reliable method for identifying, pollu-
          tant sources.

     0    Determine the relationship between terrestrial
          fallout and runoff contributions to stream and
          lake loadings.

     0    Determine acceptable levels for hazardous pollu-
          tants and determine the effects of those pollu-
          tants.

     A recent analysis  of the intermedia problem, recom-

mended that in order to determine the degree of significance
a Personal conversation with Mr. Floyd Elder, Canada Center
  for Inland Waters, Burlington, Ontario.
  Personal conversation with Dr. Michael Mullin, U.S. EPA
  Grosse lie Laboratory, Grosse lie, Michigan.

c Personal conversation with Dr. Gene E. Likens, Cornell
  University.
  "Discussion of Nonpoint Source Water Pollution Interface
  With EPA's Air Programs, January 24, 1977."  Prepared by
  Wallace E. Reed, Associate Professor, Department of En-
  vironmental Sciences, University of Virginia.


                           4-10

-------
of air pollution to nonpoint source (NFS) water pollution

problems, EPA should:

     0    Assess the location and magnitude of NFS problems
          by pollutant type through the "208" program.

     0    Estimate the air contribution to each problem
          area.

     0    Estimate the degree and cost of air pollution
          control needed locally and regionally.

     0    Estimate the value of improvement in health and
          water use effects that will result from better
          control of air pollution sources.

This approach would require continuation of existing EPA

intermedia research as well as interagency coordination of

research.  It would also identify the most critical pollu-

tant research needs.

4.3  INTRA-AGENCY CONSIDERATIONS

     At the present time, two interrelated programs are in

various stages of implementation within the U.S. Environ-

mental Protection Agency.  These are the Air Quality Main-

tenance Planning/State Implementation Plan Revision pro-

cesses and the Areawide Water Quality Management Plan/"208"

activities.  There is a close analogy between EPA's Air

Program/SIP Process and Water Program/"208" Planning.  The

entire nation is subdivided into "208" planning areas, but

more emphasis is being placed in areas of major problems

(i.e., large urban areas).  State agencies are responsible

for the development and submission of "208" plans on or
                           4-11

-------
before November 1, 1978, much as they were required to

submit SIP's in 1972.  One area of major difference in the

two programs is that under the SIP process states were given

specified regulatory requirements (i.e., Part 51 regulations)

to follow for meeting NAAQS; whereas, under the "208" Plan-

ning Process States are given more flexibility for develop-

ing these plans through the use of nonregulatory guidelines

to control sources to the extent feasible.

     Recognizing the close relationship and common object-

ives of the two programs, the Assistant Administrator for

Water and Hazardous Materials joined with the Assistant

Administrator for Air and Water Management to produce "Pro-

gram Guidance Memorandum:  SAM-8," dated November 15, 1976,

for distribution to all EPA Regional Administrators.  The

purpose of this memo was as follows:

     (1)   to transmit revised guidance on Environmental
          Protection Agency policy on the relationship
          between air quality planning and the state and
          areawide water quality management (WQM)  program,

          and

     (2)   to identify air-quality-related activities eli-
          gible for funding under section 208.

     Relative to the second item, the memo specified various

activities that are illustrative of eligible uses for

section 208 funds.  Keeping in mind that any ancillary data

gathering or development project supported by "208" funding
                            4-12

-------
must be directly related to the objectives of the WQM pro-

gram, the following activity categories appear to be eli-

gible for "208" support and of real interest to OAQPS/SASD

relative to the subject areas previously discussed:

     0    Development of common data bases.

     0    Development and implementation of common public
          participation program.

     0    Development of common institutional mechanisms for
          plan adoption, implementation, and revision.

     0    Development of control strategies or measures that
          will achieve the objectives of both air quality
          and WQM programs.

     0    Development of air quality assessments of current
          or projected development to be served by waste-
          water treatment facilities.

     0    Development of strategies for mitigating any
          adverse air quality effects from WQM plans.
                           4-13

-------
                     4.0  REFERENCES
1.  Winchester, J.W., and G.D. Nifong.  Water Pollution in
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2.  Gatz, D.F.  Estimates of Wet and Dry Deposition of
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3.  Barnes, R.S., and W.R. Schell.  Physical Transport of
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4.  Atmospheric Loading of the Upper Great Lakes:  Volume  I
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5.  The Waters of Lake Huron and Lake Superior:  Volume T
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6.  Hess, G.D., and B.C.  Hicks.  The Influence of Surface
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7.  Andrew, A.W., S.E. Lindberg, and L.C. Bates.  Atmos-
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8.  Ensor, D.S., T.A. CahilL, and L.E. Sparks.  Elemental
    Analysis of Fly Ash from Combustion of a Low Sulfur
    Coal.  Paper 175-33.7 presented at the 68th Annual
    Meeting of the Air Pollution Control Association.
    Boston, Massachusetts.  June 15-20,  1975.
                        4-14

-------
 9.  Klein, D.H., et al.  Trace Element Measurements at the
     Coal-Fired Allen Steam Plant — Mass Balance and Con-
     centrations in Fly Ash.  Paper presented at a Meeting
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10.  Kaakinen, J.W., R.M. Jorden, M.H.  Lawasani, and R.E.
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11.  Natusch, D.S.F.  Physico-chemical Associations of Trace
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12.  Zoller W.H., E.S. Gladney, and G.E. Gordon.  Elemental
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     Philadelphia, Pennsylvania.  April 6-11, 1975.

13.  Coal-Fired Power Plant Trace Element Study.  Volume I.
     A Three Station Comparison.  Radian, Inc.   U.S. En-
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     Number PB-257293.  September 1975.

14.  Beamish, Richard J.  Acidification of Lakes in Canada
     by Acid Precipitation and the Resulting Effects on
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     Columbus, Ohio.  May 12-15, 1975.

15.  Wright, Richard F., T. Dale, E.T.  Gjessing, G.R.
     Hendrey, A. Henriksen, M. Johannessen,  and I.P. Muniz.
     Impact of Acid Precipitation on Freshwater Ecosystems
     in Norway.  Proceedings of the First International Sym-
     posium on Acid Precipitation and the Forest Ecosystem.
     Columbus, Ohio.  May 12-15, 1975.

16.  Gorham, E.  Acid Precipitation and Its  Influence on
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17.  Winona Lake, Kosciusko County, Indiana.  National
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     Working Paper No. 348.  April 1976.
                          4-15

-------
18.  Hopatcong and Musconetcong Lakes, Morris and Sussex
     Counties, New Jersey.  Eutrophication Survey, U.S.
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19.  Long Lake, Steuben County, Indiana.  National Eutro-
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20.  Pompston Lakes, New Jersey.  National Eutrophication
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21.  Sylvan Lake, Noble County, Indiana.  National Eutro-
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22.  Hovey Lake, Posey County, Indiana.  National Eutrophi-
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23.  Correll, D.L.   The Rhode River Program.   Symposium on
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24.  Murphy, T.J.,  and P.V. Doskey.  Inputs of Phosphorous
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25.  Murphy, T.J.  Precipitation:   A Significant Source of
     Phosphorous and PCB's to' Lake Michigan.   Paper pre-
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26.  Mosier, A.R.,  C.E. Andre, and F.G. Viets, Jr.  Identi-
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     Feedyards.  Environmental Science and Technology.
     7:642-644.  July 1973.

27.  Giddens, J.  Contamination of Water by Air Pollutants,
     Especially Ammonia from Animal Manures.   U.S. Depart-
     ment of the Interior, Office of Water Research and
     Technology.  USDI/OWRT Project A-050-GA.
                           4-16

-------
28.  Robinson, E.,  and R.C.  Robbins.   Gaseous Nitrogen Com-
     pound Pollutants from Urban and  Natural Sources.
     Journal of the Air Pollution Control Association,
     Volume 20, No. 5, 303-306.   May  1970.

29.  Likens, G.E.,  F.H. Bormann, R.S. Pierce, and N.M.
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30.  Murphy, T.J.   Sources of Phosphorous Inputs from the
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31.  Control of Water Pollution  from  Cropland, Volume 1, A
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32.  McElroy, A.D., S.Y. Chiu, J.W. Nebgen,  A. Aleti,  and
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33.  Schuman, G.E., and R.E. Burwell.  Precipitation Nitro-
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34.  Andren, A.W.,  A.W. Elzerman, and D.E. Armstrong.
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35.  Methods and Practices for Controlling Water Pollution
     from Agricultural Nonpoint  Sources.  U.S. Environmental
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     EPA/430/9-73/015.
                          4-17

-------
36.  Young, D.R., D.J. McDermott, and T.C. Heesen.  Poly-
     chlorinated Biphenyl Inputs to the Southern California
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37.  Likens, Gene E.  Acid Precipitation.   Chemical and
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38.  Proceedings of the First International Symposium on
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39.  Conroy, N., K. Hawley, W.  Keller, and C.  Lafrance.
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     Environmental Science and Technology  8(6), 551.  1974.
                         4-18

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45.  National Inventory of Sources and Emissions:   Arsenic,
     Beryllium, Manganese, Mercury, Vanadium.   W.E. Davis,
     Associates, Leawood,  Kansas.   U.S. Environmental
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46.  National Inventory of Sources and Emissions:   Barium,
     Boron, Copper, Selenium, Zinc.  W.E.  Davis,  Associates,
     Leawood, Kansas.  U.S. Environmental  Protection Agency.
     1971.

47.  National Inventory of Sources and Emissions:   Cadmium,
     Nickel, Asbestos.  W.E. Davis, Associates, Leawood,
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     tion.   1970.

48.  Trace Contaminants in the  Environment,  Proceedings of
     the Second Annual NSF-RANN Trace Contaminants Con-
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     29-31, 1974.  Lawrence Berkeley Laboratory,  University
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49.  Natusch, N.S.F.  Characterization of  Atmospheric
     Pollutants from Power Plants.  In: Proceedings of the
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50.  Winchester, J.W.  Assessing Air Pollution Particulate
     Fallout Potential for Water Pollution in Lake Michigan.
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51.  Residual Waste Best Management Practices:  A Water
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52.  Stone, R., and H. Smallwood.   Intermedia Aspects of  Air
     and Water Pollution Control.   U.S. Environmental Pro-
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53.  Reiquam, H. , N. Dee,  and P. Choi.  Development of
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54.  Great Lakes Water Quality  Research Needs 1976.  Great
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     national Joint Commission. July 1976.
                          4-19

-------
                              TECHNICAL REPORT DATA
                        (Please read Instructions on llie reverse In-fore completing)
 \. REPORT
4. TITLE AND SUB TITLE
  The Effects of Air  Pollution on Water
  Quality
7. AUTHOR(S)
  David  W.Armentrout
I i. PERFORMING ORGMMIZATION NAME AND ADDRESS
  PEDGo  Environmental,  Inc.
!  11499  Chester Road
|  Cincinnati, Ohio  45246
 12. SPONSORING AGENCY NAME AND ADDRESS
  U.S.  Environmental  Protection Agency
  Office of Air Quality Planning  &  Standards
  Research Triangle Park, N.C.  27711
                                                   3. RECIPIENT'S ACCESS! OPr NO.
          5. REPORT DATE
           Date of Issue:  3/15/77
          6. PERFORMING ORGANIZATION CODE
                                                   8. PERFORMING ORGANIZATION REPORT NO.
                                                   10. PROGRAM ELEMENT NO.
          11. CONTRACT/GRANT NO.

            68-02-2515,  T.O.  2
                                                   13. TYPE OF REPORT AND PERIOD COVERED
                                                     Final
          14. SPONSORING AGENCY CODE
 15. SUPPLEMENTARY NOTES
  EPA  Project Officer:   Justice A.  Manning
 16. ABSTRACT
        This report  summarizes a  literature survey performed  to
  determine the effects of air pollution on water quality.
  Emphasis is on direct fallout  of  atmospheric  pollutants and
  on  precipitation  scavenging.   Preliminary evidence indicates
  the atmosphere is a significant  source of some pollutants
  in  water.  Expanded sampling,  increased effects research,  and
  improved interagency program coordination are emphasized as
  future requirements.                                   .   .
                            KEY WORDS AND DOCUMENT ANALYSIS
                DESCRIPTORS
  Air Pollution
  Water Pollution
  Atmospheric Composition
                                        b.IDENTIFIERS/OPEN ENDED TERMS
Precipitation
 Scavenging
                      c. COSATI l-'icld/Group
13B

AA
 IB. DISTRIBUTION STATEMENT
  Unlimited
                                        19. SECURITY CLASS (This Report)
                                          Unclassified
                      21. NO. OF PAGES
                         67  p.
                                        20. SECURITY CLASS (Thispage)
                                          Unclassified
                                                               22. PRICE
EPA Form 2220-1 (9-73)
                                  4-20

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