THE EFFECTS OF AIR POLLUTION
ON WATER QUALITY
PEDCo ENVIRONMENTAL
-------
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.
-------
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
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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
-------
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
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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
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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
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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.
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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
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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
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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
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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
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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.
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4.0 REFERENCES
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9. Klein, D.H., et al. Trace Element Measurements at the
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18. Hopatcong and Musconetcong Lakes, Morris and Sussex
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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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Evanston, Illinois. June 17, 1976.
26. Mosier, A.R., C.E. Andre, and F.G. Viets, Jr. Identi-
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28. Robinson, E., and R.C. Robbins. Gaseous Nitrogen Com-
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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
Atmosphere and Their Significance to Oligotrophic
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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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4-17
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36. Young, D.R., D.J. McDermott, and T.C. Heesen. Poly-
chlorinated Biphenyl Inputs to the Southern California
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and Water Pollution Control. U.S. Environmental Pro-
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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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