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7
Streams and Lakes
fames R. Kramer, Anders W. Andren, Richard A. Smith
Arthur H. Johnson, Richard B. Alexander, and Gary OehZert
INTRODUCTION
Various attempts have been made to assess changes in
the acidity of surface waters that may have occurred over
the past 50 years. An excellent review of the methods
used in the analyses as well as the basic conclusions
from a large number of investigations may be found in the
EPA's Critical Assessment Review Papers (Environmental
Protection Agency 1984). For example, Henriksen (1979,
1980, 1982), Almer et al. (1978), Dickson (1980),
Christophersen and Wright (1981), Thompson (1982),
Galloway et al. (1983a), and Wright (1983) used basic
geochemical concepts to derive general models that are
designed to predict both the sensitivity and the degree
of response of a water body to acid inputs. More complex
mechanistic and time-dependent models that are intimately
synchronized to hydrological, biological, and geomorpho-
logical factors have also been used (for example, Chen et
al. 1982, Schnoor et al. 1982, Booty and Kramer 1984).
These models have provided much useful information, but
currently none can provide detailed, quantitative assess-
ments of past or future trends in lake and stream
acidification from acid deposition. (For an evaluation
of the strengths and limitations of these models see
Church (1984).)
Another approach has been to compare the acidic status
of lakes, rivers, and ponds in North America using his-
torical and current data on pH, alkalinity, and sulfate.
Studies in the United States include, for example, those
of Schofield (1976) for New York lakes, Davis et al.
(1978) for lakes in Maine, Johnson (1979) for streams in
New Jersey, Pfeiffer and Festa (1980) for lakes in New
York, Hendrey et al. (1980) and Burns et al. (1981) for
231
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232
headwater streams in North Carolina and New Hampshire,
Arnold et al. (1980) for Pennsylvania streams, Crisman et
al. (1980) for lakes in northern Florida, Norton et al.
(1981) for lakes in New Hampshire, Maine, and Vermont,
Lewis (1982) for lakes in Colorado, Haines et al. (1983)
for lakes in New England, and Eilers et al. (1985) for
lakes in northern Wisconsin. Similar studies have also
been published on lakes in Canada (Beams and Harvey
1972, Beamish et al. 1975, Dillon et al. 1978, Watt et
al. 1979, Thompson et al. 1980) and Scandinavia (Wright
and Gjessing 1976, Rebadrosf 1980). These studies
analyzed water quality data using a variety of methods.
Some sets include continuous data records and others only
data at discrete points in time. Many of the analyses
account for such complicating factors as changes in
analytical methods and land use practices. The
conclusions from a variety of studies are that at least
some lakes exhibit a decrease in pH and alkalinity when
historical and recent data are compared.
Similarly, a review by Turk (1983) compares historical
and geographical trends in the acidity of precipitation
with trends in North American surface waters. Based on
the synthesis of a variety of data collected during
discrete time periods (mainly the 1930s and late 1970s)
and examined by Schofield (1976), Pfeiffer and Festa
(1980), Davis et al. (1978), Norton et al. (1981), Burns
et al. (1981), and Haines et al. (1983), he concludes
that decreases in pH and alkalinity have occurred in
lakes in New York and New England.
In addition, water quality data are available from the
U.S. Geological Survey's Hydrologic Bench-Mark Network.
These data, collected since the middle 1960s, provide a
continuous record of high-quality data for pa, alkalinity,
and sulfate as well as the major_cations and anions for
small watersheds in the United States. Smith and
Alexander (1983) have studied these records and conclude
that "In the northeastern quarter of the country, SO2
emissions have decreased over the past 15 years and the
trends in the cited chemical characteristics (alkalinity
and sulfate) of Bench-Mark streams are consistent with a
hypothesis of decreased acid deposition in that region.
Throughout much of the remainder of the country, SO2
emissions have increased and trends in stream sulfate,
alkalinity and alkalinity/total cation ratios are con-
sistent with a hypothesis of increased acid deposition.
There are, however, several acknowledged problems in
the interpretation of "historical n lake water chemistry
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233
data. Perhaps the chief drawback is the lack of docu-
mentation of sampling and analytical procedures. A major
problem encountered in our study has been the lack of
sufficient documentation, before 1950, of the procedures
for calculating pH and alkalinity. For example, whereas
the current method for measuring pH and alkalinity employs
standard electronic instruments, before about 1950 the
method of choice was calorimetry using indicator dyes,
which, when added in small quantities to solutions of
unknown pH, cause color changes at specific pHs. Methyl
orange, a commonly used indicator for measuring the
alkalinities of lake waters in the 1930s, undergoes
subtle color changes over a range of pH values, and the
exact endpoint used by analysts is often not clearly
specified in the historical records. In this chapter, we
review some of these records and assess trends based on
the most likely endpoints employed in the historical
studies.
Furthermore, for reasons that are described in detail
in Appendix D, titration of lake water solutions to a
methyl orange endpoint requires a correction for "over-
titration." Assumptions about the magnitude of the
correction are especially important when analyzing low-
alkalinity waters. In most previous studies, researchers
have assumed that the correction factor is a constant
independent of the original alkalinity. Values ranging
from zero to greater than 100 microequivalents per liter
(peq/L) have been employed in such studies. A uniform
method for analyzing these types of samples is highly
desirable, and one goal of this chapter is to present a
method for determining the historical corrections by
calculations rather than by assumption. The method
accounts for the fact that the relation between the
correction factor and alkalinity is sensitive to the
alkalinity of the test solution. In addition, the method
provides a means for checking the internal consistency of
the data set.
Additional factors that must be considered in inter-
preting current and historical data include (1) clima-
tology, since the hydrology of lakes and rivers may vary
considerably from year to year in response to fluctuations
in precipitation and climatic factors affecting evapora-
tion, (2) regional patterns of emissions of acid pre-
cursors, since natural waters downwind of sources may be
expected to exhibit greater changes in water quality than
those situated upwind, (3) changes in land use (although
Drably et al. (1980) found that land use changes in
Norway did not seem to be related to regional acidifica-
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234
tion patterns, local changes in alkalinity and pH regimes
were evident), (4) the statistical validity of using data
separated by 20 to 40 years to examine trends, and (5)
representativeness of data sets for various regions.
Inferences about trends obtained from data on a limited
number of lakes within a region should reflect the
distribution of values of alkalinity and pH (and other
physical, chemical, and biological parameters) for the
whole region.
In the current study, we have tried to overcome some
of the difficulties mentioned above by examining temporal
and spatial variations in several water quality
parameters--pH, alkalinity, sulfate, and selected major
anions and cations--that simultaneously give some
information about the acidic status of lakes. The
analysis is restricted to a few sets of data of high
quality selected to provide both a determination of
regional trends in lake and stream acidification and an
illustration of a consistent methodologic approach.
In this chapter, we first examine the hypothesis that
sulfate levels in lakes and wet precipitation in the
northeastern United States and eastern Canada are
correlated. Many concepts of lake acidification focus on
the titration of a surface water body by sulfuric acid
deposited from the atmosphere (e.g., Henriksen 1980).
The result of this simple titration is to substitute
sulfate ion for bicarbonate ion, thus lowering the
alkalinity and the pH of the affected surface water.
Wright (1983, 1984) has shown a linear correlation
between averages of sulfate concentrations for selected
lakes and average sulfate concentration in precipitation
in eastern North America, and Thompson and Hutton (1985)
show a similar relationship in eastern Canada.
To link sulfate ion concentration in atmospheric
deposition to the sulfate ion concentration of surface
waters, a direct relationship must exist between atmo-
spheric and lake sulfate fluxes for a steady state
assumption. A fundamental condition for this relation-
ship to be valid is that there be no overriding internal
sources or sinks of sulfate ions in the watersheds. If
such sources and sinks do occur, then the method of
averaging sulfate concentrations of large sets of lakes
may mask the large variability in the data, particularly
if averaging cancels factors equal in magnitude but
opposite in sign. We examine data from a set of 626
lakes and assign to each a value of precipitation
sulfate flux. We draw general conclusions about spatial
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235
associations between precipitation and lake sulfate
fluxes from a statistical analysis of both the aggregated
data and the data subdivided by regions.
Next we address sulfate-driven changes in stream-water
chemistry, using data from the U.S. Geological Survey
Bench-Mark Network. The network provides a continuous
record of monthly data on major ions in stream water
beginning in the middle 1960s. Data are from pre-
dominately undeveloped watersheds in 37 states. Con-
tinuous sampling and unchanged analytical methods for the
period make the data particularly well suited for
examining atmospheric influences on water quality as a
function of spatial and temporal SO2 emission patterns.
The study of sulfate-driven changes in surface water
chemistry is accomplished with the aid of a general
paradigm that links acidic deposition to changes in the
water quality in watersheds with acidic soil.
Finally, we compare pH and alkalinity data of lakes
taken at discrete time intervals, i.e., from the 1920s
and 1930s to the 1970s and l980s. Three lake surveys
were chosen for analysis; two in the northeastern United
States (New York and New Hampshire) and one in the upper
Midwest (Wisconsin). These lakes were selected because
they provide, in our judgment, some of the most complete
historical and recent data available, allowing us to test
them for internal consistency according to the protocol
of Kramer and Tessier (1982). We present this analysis
to illustrate a chemically rigorous interpretation of
historical pH and alkalinity measurements and to estimate
the magnitude of changes in the acidic status of these
lakes that may have occurred over the past 50 to 60 years.
In our approach we limited our data to those lakes for
which historical data on pH, alkalinity, and free CO2
acidity were available. The availability of simultaneous
data for the three parameters allows us to perform a check
for internal consistency of the data as an indicator of
their reliability. Without this constraint a larger
historical data base is available over wider geographic
areas. Although our method allows us to screen the data
for internal consistency, a larger (unscreened) data base
may provide more expansive regional information and be
amenable to more powerful statistical tests, although the
data may be less reliable and hence the results of the
tests less meaningful. Differences that may exist between
the results obtained in this chapter and elsewhere must
be viewed in light of the assumptions made and how the
assumptions affect the selection and analysis of the data.
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236
SULFATE FLUXES IN PRECIPITATION AND LAKES
In this section, we test the hypothesis that the
fluxes of sulfate into lakes from atmospheric deposition
generally determine the fluxes of sulfate outflow from
lakes over a broad geographical area. Such a relationship
must be demonstrated to exist before we can assume with
any confidence that water chemistry and related data on
fisheries records and lake sediment stratigraphy (de-
scribed in the following chapters) are accurate indicators
of atmospheric acid deposition.
Studies of the mass balance of sulfate in a few water-
sheds have been reported for which parameters such as
atmospheric deposition, streamflow, and geology are
sufficiently well determined to permit more detailed
analyses (e.g., the Hubbard Brook watershed, Likens et
al. 1985; and three lakes in the Adirondacks, Galloway et
al. 1983b). The studies conclude that sulfate concentra-
tions in these waters are controlled by atmospheric
deposition of sulfur. In a different type of analysis,
Wright (1983) found an approximately linear relationship
between the mean concentration of sulfate in 15 groups of
lakes in North American and mean excess (i.e., nonmarine)
sulfate in wet precipitation.
In our analysis, we compare sulfate input fluxes in
wet deposition with the estimated sulfate output fluxes
from 626 lakes in New York, New England, Quebec, Labrador,
and Newfoundland. Fluxes of sulfate from wet deposition
were obtained by multiplying the concentration of sulfate
in rain by the intensity of rainfall (meters/year). Lake
output fluxes of sulfate were estimated as the product of
sulfate concentration in lake water and the intensity of
net precipitation (i.e., meters/year measured as rainfall
minus evaporation). (See Appendix B for specific methods
and references.) It was possible to perform a detailed
statistical analysis to test the relation between sulfate
inputs and outputs for linearity (or some other monotonic
relationship) and regional variance on subdividing the
area into smaller regions. Such an analysis suited the
particular needs of this study, which addresses the
question of broad regional patterns in eastern North
America. However, we note that this analysis is subject
to uncertainty because for each of these lakes we
generally lack important information on dry deposition,
transpiration, observed streamflow from the watershed,
soil chemistry, and processes within the watershed that
are sources of sulfur.
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237
Results
Figure 7.1(a) is a plot of sulfate inputs to 626 faxes
from wet-only deposition as a function of annual sulfate
outputs from the lakes based on data for 1980-1982. It
is apparent that there is a greater variability in lake
sulfate outflow fluxes than in precipitation sulfate
fluxes. The scatter is greatest for lakes in
Massachusetts (Figure 7.1(b)) owing to some extreme
outliers and is of similar, smaller magnitude for other
regions. In some cases, the output flux of sulfate from
[ekes is greater than the flux from wet precipitation,
suggesting that significant sources of sulfur other than
from wet deposition exist in these watersheds. In other
cases, the reverse is apparently true, perhaps suggesting
that atmospheric sulfur may be retained in the watershed,
or that sulfate is chemically reduced in the lake and
deposited in the sediment.
The apparent lake sulfate output flux normalized to
the wet-only precipitation sulfate input flux is analyzed
by geographic region in Table 7.1. Deficiencies in lake
sulfate outputs compared with inputs from wet-only
deposition Generally occur in remote regions such as
Newfoundland and Labrador, whereas excesses occur in more
populated areas such as New York, Connecticut, and
Massachusetts. The origins of the deficiencies and
excesses are not known on a lake-specific basis, but dry
deposition, watershed processes involving sulfur cycling,
and other sulfur sources of unknown origin are expected
to be important contributors.
Analysis
In an effort to stabilize the variability in the
sulfate output fluxes of lakes, the data were analyzed on
the logarithmic (base e) scale (Figure 7.2). As a whole
the data do not follow the y = x line (i.e., the case in
which sulfate outputs equal sulfate inputs). Linear
regression yields an estimate of a line log y = a log x +
mi' in which the intercept, ml', is -0.306 (standard
error, 0.041) and the slope, a, is 1.593 (standard error,
0.046). The slope of this line is significantly different
from one, so the overall relationship on the natural
scale, y = mixa in which mi is +0.736 (antilogarithm
(base e) of ml') and a is 1.593, is significantly
different from linear.
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238
1 5
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FIGURE 7.1 (a) Comparison of sulfate input fluxes to
lakes from wet-only deposition with sulfate output fluxes
from lakes in the northeastern United States and eastern
Canada. (b) A similar plot for lakes in Massachusetts
only.
OCR for page 239
239
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OCR for page 240
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41 1
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LOG OF WET PRECIPITATION SULFATE INPUT FLUX
FIGURE 7.2 Comparison of the logarithm (base e) of
sulfate fluxes to lakes from wet-only deposition with the
logarithm (base e) of sulfate fluxes from lakes in the
northeastern United States and eastern Canada. Solid
line is the y = x line (i.e., condition in which sulfate
flux from the lakes equals the sulfate flux to the lakes
from wet-only deposition); dashed line is the line
estimated from linear regression with slope of 1.593.
As noted earlier there is a tendency for lakes in some
regions to lie above the line of equal fluxes (excess
lake sulfate flux in Table 7.1) and other regions to lie
below it (excess precipitation sulfate flux in Table
7.1). This tendency may result from regional differences
in geology, dry deposition, or other factors causing the
regional ratios of input to output fluxes to differ from
the overall relationship. To account for regional
differences we performed an analysis of covariance in
which we allowed each region to have its own intercept,
but fitted the same slope for all regions.
To analyze the data on a regional basis, we have
chosen the following six regions: Connecticut,
Massachusetts, and Rhode Island (CT-MA-RI); Maine,
Vermont, and New Hampshire (ME-VT-NH); New York (NY);
Newfoundland (NF); Labrador (LB); Quebec (QU). The
linear regressions shown for each region in Figure 7.3
yield the following estimates:
OCR for page 241
241
Region Intercept (mi') Standard Error
CT~ RI 0.691
MEVTNH 0 . 2 57
NY 0.280
NF -0.004
LB -0 .515
QU 0.098
Slope (a) 1.089
0.0791
0.0729
0.1082
0.0626
0.0407
0.0781
0.0712
~ The improvement in fit in going from a single regres-
sion line to the six regional lines is highly significant,
having a p value less than 10-6. Furthermore, the
common slope (a) is not significantly different from
one. Thus, there is no evidence that the relationship on
the natural scale (y = mica) is nonlinear once
regional differences have been taken into account.
The multipliers mi' are regionally specific. Thus
lake sulfate output flux y is estimated to be a multiple
of precipitation sulfate input flux x. (Note, that on
the natural scale, our model will not in general estimate
the arithmetic mean of the lake sulfate flux.) The
multiple depends on such factors as the ratio of total
deposition to wet-only deposition, the rate at which
sulfur is demobilized in the watershed or sediments, the
magnitude of sulfur sources in the watershed, and the
magnitude of any bias in our estimate of wet-only sulfate
flux. The values of mi may be calculated from the
antilogarithms of the intercepts (mi') shown in Figure
7.3. The values are as follows: 2.00 (CT-MA-RI), 1.32
(NY), 1.29 (ME-VT-NH), 1.10 (QU), 1.00 (NF), and 0.60
(LB). These multiples are greatest in regions close to
strong sulfur source areas and smallest in remote areas,
suggesting that dry deposition plays a major role. Since
the 0.60 value for Labrador indicates that output fluxes
are smaller than input fluxes, watershed processes that
retain sulfate may be important.
To obtain more detailed information of sulfur mass
balance from these data, each location and perhaps each
watershed needs to be considered separately. In some
cases internal sources of sulfate may be important
contributing factors to the sulfur mass balance (Wagner
et al. 1982). For example, in Table 7.2, the geological
setting is described for the locations of lakes in
Massachusetts and Maine having large excesses of lake
sulfate fluxes. Since strike zones, amphibolites,
OCR for page 289
289
literature of the pH of this endpoint range between about
4.0 to higher than 4.3. The color of the endpoint in
this range has been variously described as "faint pink,"
"pink," and "salmon pink." The Wisconsin survey provides
the best documentation of the pH of the MO endpoint,
citing a range of pH values from 4.06 to 4.18 for the
"fainter" pink color and recommending that a value of
4.18 be used in calculating titrations.
Our analysis shows that changes in alkalinity and pH
in New York lakes are sensitive to the assumption made
about the pH of the MO endpoint. Assuming an endpoint pH
of 4.2 (or greater), New York lakes, on average, appear
to have increased substantially in acidic status over the
past 50 years, as reflected in reductions in both
alkalinity and pH. Alternatively, if a value of the pH
endpoint close to 4.0 is assumed and if the historical
data are compared with the 1984 data set, then there
appears to have been little change, on average, in the
acidic status of New York lakes over the past 50 years.
However, if the historical data are compared with the
1980 New York data set, there may have been an overall
decline in alkalinity. New Hampshire lakes do not appear
to be so sensitive to the choice of tne endpoint pH of
MO. If an endpoint pH close to 4.2 is assumed, these
lakes, on average, show little or no decrease in
alkalinity and show a slight increase in pH. With an
endpoint near 4.0 there is again little or no change, on
average, in alkalinity, but an increase in pH of about
0.4 pH unit. Wisconsin lakes, on average, appear to show
a significant increase in alkalinity (38 peq/L) and pH
(+0.5 unit) if an MO endpoint of 4.2 is assumed. The
increases are even larger if an endpoint close to 4.0 is
assigned.
Currently, the question regarding the correct endpoint
pH in historical alkalinity titrations is unresolved. In
the judgment of the authors of this chapter the endpoint
lies in the range from 4.19 to 4.04, but evidence is not
sufficient to specify a most likely value. Tests done
with indicator dyes which have been preserved for the
past 50 years may be valuable in resolving this question.
We have not attempted to indicate the mechanisms for
change in acidic status of these lakes. Any discussion
of mechanisms must consider each lake separately and
include all the hydrological and biogeochemical factor
For most lakes, data are not available currently to
permit this kind of analysis.
OCR for page 290
290
One possible avenue of future research is to conduct a
detailed study of the outliers in the three data sets.
If the maximum change in lake alkalinity from deposition
of atmospheric sulfur is about 100 peq/L, then study of
the larger changes subjected to the most careful scrutiny
for quality may offer a rational explanation for other
acidification mechanisms.
REFERENCES
Almer, B., W. Dickson, C. Eckstrom, and E. Hornstrom.
1978. Sulfur pollution and the aquatic ecosystems. Pp.
273-311 of Sulfur in the Environment, Part Il.
Ecological Impacts. J. O. Nriagu, ed. New York: J.
Wiley and Sons.
Arnold, D. E., R. W. Light, and V. J. Dymond. 1980.
Probable effects of acid precipitation on Pennsylvania
waters. U.S. Environmental Protection Agency.
EPA-600/3-80-012. 21 pp.
Baker, J., and T. Harvey. 1985. Critique of acid lakes
and fish population status in the Adirondack region of
New York State. Draft final report for NAPAP Project
E3-25, U.S. Environmental Protection Agency.
Beamish, R. J., and H. H. Harvey. 1972. Acidification of
the La Cloche Mountain Lakes, Ontario and resulting
fish mortalities. J. Fish. Res. Board Can.
29:1131-1143.
Beamish, R. J., W. L. Lockhart, J. C. van Loon, and H. H.
Harvey. 1975. Long-term acidification of a lake and
resulting effects of fishes. Ambio 4:98-102.
Blakar, I. A., and I. Digernes. 1984. Evaluation of
acidification based on former calorimetric
determination of pH: The effect of indicators on pH in
poorly buffered water. Verh. Int. Ver. Limnol.
22:679-685.
Booty, W. G., and J. R. Kramer. 1984. Sensitivity and
analysis of a watershed acidification model, Phil.
Trans. R. Soc. London Ser. B 305:441-449.
Burns, D. A., J. N. Galloway, and G. R. Hendry. 1981.
Acidification of surface waters in two areas of the
eastern United States. Water Air Soil Pollut. 16:
277-285.
Chen, C. W., J. D. Dean, S. A. Gherini, and R. A.
Goldstein. 1982. Acid rain model: hydrologic module.
J. Env. Eng. Div. Am. Soc. Civ. Eng. 108:455-472.
OCR for page 291
291
Christophersen, N., and R. F. Wright. 1981. Sulfate
budget and a model for sulfate concentrations in
stream water at Birkenes, a small forested catchment
in southernmost Norway. Wat. Resour. Res. 17:377-389.
Church, M. F. 1984. Predictive modeling of acidic
deposition on surface waters. Pp. 4-113--4-128 of The
Acidic Deposition Phenomenon and Its Effects. Critical
Assessment Review Papers. Vol. II. Effects Sciences.
A. P. Altshuller and R. A. Linthurst, eds.
EPA-600/8-83-016 BE. U.S. Environmental Protection
Agency.
Clark, W. M. 1928. The Determination of Hydrogen Ions.
Baltimore, Maryland: The Williams and Wilkins Company.
Cobb, E. D., and J. E. Biesecker. 1971. The national
hydrologic Bench-Mark network. Circular 460-D, U.S.
Geological Survey. 38 pp.
Colquhoun, J., W. Kreter, and M. Pfeiffer. 1984. Acidity
states of lakes and streams in New York State. New
York Department of Environmental Conservation,
Raybrook, New York. 49 pp + viii app.
Crisman, T. L., R. L. Schulze, P. L. Brezonik, and S. A.
Bloom. 1980. Acid precipitation: the biotic response
in Florida lakes. Pp. 296-297 of Ecological Impact of
Acid Precipitation. D. Drably, and A. Tollan, eds.
Proceedings of an international conference,
Sandefjord, Norway. Sur Nedb~rs Virkning Pa Skog Og
Fisk (SNSF) Project, Oslo.
Critical Assessment Review Papers (CARP). 1984. The
acidic deposition phenomenon and its effects. A. P.
Altschuller and R. A. Linthurst, eds. Report
EPA-600/8-83-016AF. U.S. Environmental Protection
Agency.
Cronan, C. S., and C. L. Schofield. 1979. Aluminum
leaching response to acid precipitation: effects on
high-elevation watersheds in the Northeast. Science
204(20):304-306.
Davis, R. B., M. O. Smith, J. H. Bailey, and S. A.
Norton. 1978. Acidification of Maine (U.S.A.) lakes by
acidic precipitation. Verh. Int. Ver. Limnol.
10:532-537.
Dickson, W. 1980. Properties of acidified waters. Pp.
75-83 of Proceedings of an International Conference.
Ecological Impact of Acid Precipitation, D. Drabl
OCR for page 292
292
Dillon, P. J. 1983. Chemical alteration of surface water
by acidic deposition in Canada. Pp. 275-286 of
Ecological Effects of Acid Deposition. Report P. 1636
National Swedish Environmental Protection Board.
Dillon, P. J., D. S. Jeffries, W. Snyder, R. Reid, N. D.
Yan, D. Evans, J. Moss, and W. A. Scheider. 1978. Acid
precipitation in south-central Ontario: recent
observations. J. Fish. Res. Board Can. 35:809-815.
Drabl~s, D., D. I. Sevaldrud, and J. A. Timberlid. 1980.
Historical land-use changes related to fish status
development in different areas in southern Norway. Pp.
367-369 of Proceedings of an International Conference.
Ecological Impact of Acid Precipitation, D. Drably
and A. Tollan, eds. Sur Nedb~rs Virkning Pa Skog Og
Fisk (SNSF) Project, Oslo, Norway.
Driscoll, C. T., and G. E. Likens. 1982. Hydrogen ion
budget of an aggrading forested ecosystem. Tellus
34:283-292.
Driscoll, C. T., and R. M. Newton. 1985. Chemical
characteristics of Adirondack lakes. Environ. Sci.
Technol. 19:1018-1024.
Eilers, J. M., G. E. Glass, and A. K. Pollack. 1985.
Water quality changes in northern Wisconsin lakes,
1930-1980. RL-D Draft 539. U.S. Environmental
Protection Agency.
Environmental Protection Agency. 1984. The Acidic
Deposition Phenomenon and Its Effects. In Critical
Assessment Review Papers, Vol. II. Effects Sciences.
A. P. Altshuller and R. A. Linthurst, eds.
EPA-600/8-83-016 BE.
Fitzgerald, J. W., T. C. Strickland, and W. T. Swank.
1982. Metabolic fate of inorganic sulfate in soil
samples from undisturbed and managed forest
ecosystems. Soil Biol. Biochem. 14:529-536.
Galloway, J. N. 1984. Long-term acidification. In The
Acidic Deposition Phenomenon and Its Effects. Critical
Assessment Review Papers. Vol. II. Effects Sciences.
A. P. Altshuller and R. A. Linthurst, eds.
EPA-600/8-83-016 BF.
Galloway, J. M., S. A. Norton and M. R. Church. 1983a.
Freshwater acidification from atmospheric deposition
of sulfuric acid: A conceptual model. Environ. Sci.
Technol. 17:541A-545A.
Galloway, J. N., C. L. Schofield, N. E. Peters, G. R.
Hendrey, and E. R. Altwicker. 1983b. The effect of
atmospheric sulfur on the composition of three
Adirondack lakes. Can. J. Fish. Aquat. Sci. 40:799-806.
OCR for page 293
293
Gran, G. 1952. Determination of equivalence point in
potentiometric titrations. Analyst 77:661-671.
Haines, T. A., J. J. Akielagzek, and P. J. Rago. 1983. A
regional survey of chemistry of headwater lakes and
streams in New England: vulnerability to
acidification. Air Pollution and Acid Rain Series.
U.S. Fish and Wildlife Service Report.
Hendrey, G. R., J. N. Galloway, S. A. Norton, C. L.
Schofield, P. W. Schaffer, and D. A. Burns. 1980.
Geological and hydrochemical sensitivity of the
eastern United States to acid precipitation.
~ EPA-60013-80-024. U.S. Environmental Protection
Agency. 100 pp.
Henriksen, A. 1979. A simple approach for identifying
and measuring acidification of freshwater. Nature
278:542-545.
Henriksen, A. 1980. Acidification of freshwaters--a
large scale titration. Pp. 68-74 of Ecological Impact
of Acid Precipitation. D. Drabl~s and A. Tollan,
eds. Sur Nedb~rs Virkning Pa Skog Og Fisk (SNSF)
Project, Oslo.
Henriksen, A. 1982. Changes in Base Cation Concentrations
Due to Freshwater Acidification. Acid Rain Research
Report 1/1982. Norwegian Institute for Water Research
(NIVA), Oslo.
Hirsch, R. M., J. R. Slack, and R. A. Smith. 1982.
Techniques of trend analysis for monthly water quality
data. Water Resour. Res. 18:107-121.
Hoover, E. E. 1937. Biological Survey of Androscoggin
Saco and Coastal Watersheds. New Hampshire Fish and
Game Commission, Concord.
Hoover, E. E. 1938. Biological Survey of the Merrimack
Watershed. New Hampshire Fish and Game Commission,
Concord.
Johnson, A. H. 1979. Evidence of acidification of
headwater streams in the New Jersey pinelands. Science
206:834-836.
Johnson, D. W. 1980. Site susceptibility to leaching by
H2SO4 in acid rainfall. Pp. 525-536 of Effects of
Acid Precipitation on Terrestrial Ecosystems. T. C.
Hutchinson and M. Havas, eds. New York: Plenum Press.
Johnson, D. W., and G. S. Henderson. 1979. Sulfate
absorption and sulfur fractions in a highly weathered
soil under mixed deciduous forest. Soil Sci.
128:34-40.
OCR for page 294
294
Juday, J., E. A. Birge, and V. W. Meloche. 1935. The
carbon dioxide and hydrogen content of the lake waters
of northeastern Wisconsin. Trans. Wis. Acad. Sci.
Arts Letters 29:1-82.
Kolthoff, I. M. 1931. Pp. 30-31, 52-53 of The
Colorimetric and Potentiometric Determination of pH.
New York: John Wiley and Sons.
Kolthoff, I. M., and V. A. Stenger. 1947. Titration
methods. Pp. 61-62 of Volumetric Analysis, Vol. II.
New York: John Wiley and Sons.
Kramer, J. R., and A. Tessier. 1982. Acidification of
aquatic systems: a critique of chemical approaches.
Environ. Sci. Technol. 16:606A-615A.
Krug, E. C., and C. R. Frink. 1983. Acid rain on acid
soil: a new perspective. Science 221:520-525.
Lewis, W. M. 1982. Changes in pH and buffering capacity
of lakes in the Colorado Rockies. Limnol. Oceanogr.
27:161-171.
Likens, G. E., F. H. Bormann, R. S. Pierce, and N. M.
Johnson. 1977. Biogeochemistry of a Forested
Ecosystem. New York: Springer-Verlag. 146 pp.
Likens, G. E., F. H. Bormann, R. S. Pierce, and J. S.
Eaton. 1985. The Hubbard Brook Valley. Chapter II of
An Ecosystem Approach to Aquatic Ecology: Mirror Lake
and Its Environment, G. E. Likens, ed. New York:
Springer-Verlag.
Mohn, E., E. Joranger, S. Kalvenes, B. Sollie, and R.
Wright. 1980. Regional surveys of the chemistry of
small Norwegian lakes: a statistical analysis of the
data from 1974-1978. Pp. 240-241 of Ecological Impact
of Acid Precipitation, D. Disables and A. Tollens, eds.
Sur Nedb~rs Virkning Pa Skog Og Fisk (SNSF) project.
Morrison, I. K. 1984. Acid rain: a review of literature
on acid deposition effects in forest ecosystems. For
Abstr. 4S:483-506.
National Research Council. 1984. Acid Deposition:
Processes of Lake Acidification. Washington, D.C.:
National Academy Press.
Newell, A. E. 1970. Biological survey of the lakes and
ponds in Cheshire, Hillsborough, and Rockingham
Counties. New Hampshire Fish and Game Commission,
Concord.
Newell, A. E. 1972. Biological survey of the lakes and
ponds in Coos Grafton and Car rol Counties. New
Hampshire Fish and Game Commission, Concord.
.
OCR for page 295
295
Newell, A. E. 1977. Biological survey of the lakes and
ponds in Sullivan, Merrimack, Belknap and Strafford
Counties. New Hampshire Fish and Game Commission,
Concord.
New York Department of Conservation. 1930. Biological
Survey of the St. Lawrence Watershed, Vol. V. Albany,
New York.
New York Department of Conservation. 1931. Biological
Survey of the Oswegatchie and Black River Systems,
Vol. VI. Albany, New York.
New York Department of Conservation. 1932. Biological
Survey of the Upper Hudson Watershed, Vol VII. Albany,
New York.
New York Department of Conservation. 1933. Biological
Survey of the Raquette Watershed, Vol VIII. Albany,
New York.
New York Department of Conservation. 1934. Biological
Survey of the Mohawk-Hudson Watershed, Vol. IX.
Albany, New York.
Norton, S. A., R. B. Davis, and D. F. Braekke. 1981.
Responses of Northern New England Lakes to Atmospheric
Inputs of Acids and Heavy Metals. Completion Report:
Project A-048-ME. U.S. Department of the Interior,
Office of Water Research and Technology. 90 pp.
Oliver, B. G., E. M. Thurman, and R. L. Malcolm. 1983.
The contribution of humic substances to the acidity of
colored natural waters. Geochim. Cosmochim. Acta
47:2031-2035.
Olson, R. J., D. W. Johnson, and D. S. Shriner. 1982.
Regional assessment of potential sensitivity of soils
in the eastern U.S. to acid precipitation. OaK Ridge
National Laboratory, Environmental Sciences Division,
Oak Ridge, Tenn. Publication Number 1899. 50 pp.
Overrein, L. M., H. M. Seip, and A. Tollan. 1980. Acid
Precipitation-Effects on Forests and Fish. Final
report. Sur Nedb~rs Virkning Pa Skog Og Fisk (S~SF)
project, 1972-1980. Oslo. 175 pp.
Pfeiffer, M. H. and P. J. Festal 1980. Acidity status
of lakes in the Adirondack region of New York in
relationship to fish sources. New York Department of
Environmental Conservation, Albany, N.Y.
FW-P168(10/80). 36 pp.
OCR for page 296
296
Rebsdorf, A. 1980. Acidification of Danish softwater
lakes. In Proceedings of the International Conference
on Ecological Impact of Acid Precipitation, D. Drably
and A. Tollan, eds. Sur Nedb~rs Virkning Pa Skog Og
Fisk (SNSF) project, 1432 As, Norway. 383 pp.
Reuss, J. O. 1985. Implications of the Ca-A1 exchange
system for the effect of acid precipitation on soils
J. Environ. Qual. 14:26-31.
Richter, D. D., D. W. Johnson, and D. E. Todd. 1983.
Atmospheric sulfur deposition, neutralization and ion
leaching in two deciduous forest ecosystems. J.
Environ. Qual. 12:263-269.
Rosenquist, I. Th., P. Jorgensen, and H. Rueslatten.
1980. The importance of natural H production for
acidity in soil and water. Proceedings of an
International Conference. Pp. 240-241 of Ecological
Impact of Acid Precipitation, D. Drabl~s and A.
Tollan, eds. Sur Nedb~rs Virkning Pa Skog Og Fisk
tSNSF) project, Oslo.
Schnorr, J. L., G. R. Carmichael, and F. A. Van Schepen.
1982. An integrated approach to acid rainfall
assessments. Chapter 13 of Vol. II. Energy and
Environmental Chemistry: Acid Rain, L. H. Keith, ed.
Ann Arbor, Michigan: Ann Arbor Science.
Schofield, C. L. 1976. Lake acidification in the
Adirondack mountains of New York: causes and
consequences. In Proceedings of the First
International Symposium on Acid Precipitation and the
Forest Ecosystem, L. S. Dochinger and T. A. Seliga,
eds. U.S. Department of Agriculture Forest Service
Technical Report NE-2.
Schofield, C. L. 1982. Historical fisheries changes as
related to surface water pH changes in the United
States. Pp. 57-68 of Acid Rain/Fisheries, R. E.
Johnson (ed.). Bethesda, Md.: American Fisheries
Society.
Seip, H. M. 1980. Acidification of Freshwater--Sources
and Mechanisms. Pp. 358-366 of Ecological Impacts of
Acid Precipitation, D. Drably and A. Tollan, eds.
Proceedings of an international congress in
Sandefjord, Norway. Sur Nedb~rs Virkning Pa Skog Og
Fisk (SNSF) Project, Oslo.
Skougstad, M. W., M. J. Fishman, L. C. Friedman, D. E.
Erdmann, and S. Duncan, Eds. 1979. Methods for
Determination of Inorganic Substances in Water and
Fluvial Sediments Techniques of Water-Resources
Investigations of the U.S. Geological Survey. Book 5,
Chapter A1. Washington, D.C.: U.S. Government Printing
Office.
.
OCR for page 297
297
Smith, R. A., and R. B. Alexander. 1983. Evidence for
acid precipitation induced trends in stream chemistry
at Hydrologic Bench-Mark stations. Circular 910. U.S.
Geological Survey. 12 pp.
Smith, R. A., R. M. Hirsch, and J. R. Slack. 1982. A
study of trends in total phosphorus measurements at
NASQAN stations. USGS Water-Supply Paper 2190.
Standard Methods for the Examination of Water and Sewage.
1926. 4th ed. American Public Health Association, New
York.
Standard Methods for the Examination of Water and Sewage.
1930. 6th ed. American Public Health Association, New
York.
Standard
1933.
York.
Standard
1936.
York.
Standard
1960.
York.
Methods for the Examination of Water and Sewage.
7th ed. American Public Health Association, New
Methods for the Examination of Water and Sewage.
8th ed. American Public Health Association, New
Methods for the Examination of Water and Sewage.
11th ed. American Public Health Assocation, New
Stung, W., and J. J. Morgan. 1981. Aquatic Chemistry.
New York: John Wiley and Sons.
Taylor, F. L. 1933. Letter of February 23, 1933, from
F. Lowell Taylor to J. Juday, Department of Chemistry,
University of Wisconsin. Archives of the University of
Wisconsin, Madison.
Thompson, M. E. 1982. The cation denudation rate as a
quantitative index of sensitivity of eastern Canadian
rivers to acidic atmospheric precipitation. Water Air
Soil Pollut. 18:215-226.
Thompson, M. E., and M. B. Hutton. 1982. Sulfate in
lakes of eastern Canada: calculated atmospheric loads
compared with measured wet deposition. National Water
Research Institute, Environment Canada, Burlington,
Ontario.
Thompson, M. E., and M. B. Hutton. 1985. Sulfate in
lakes of Eastern Canada: calculated yields compared
with measured wet and dry deposition. Water Air Soil
Pollut. 24:77-83.
Thompson, M. E., F. C. Elder, A. R. Davis, and S.
Whitlow. 1980. Evidence of acidification of rivers of
Eastern Canada. Pp. 244-245 of Ecological Impact of
Acid Precipitation, D. Drabl0`s and A. Tollan, eds.
Proceedings of an international conference. Sur
Nedbbrs Virkning Pa Skog Og Fisk (SNSF) project, Oslo.
OCR for page 298
298
Towne, R. E. 1983. Past and present pH and alkalinity of
New Hampshire lakes and ponds, New Hampshire Water
Supply Pollution Control Commission, Concord.
Unpublished manuscript. 20 pp.
Turk, J. T. 1983. An evaluation of trends in the acidity
of precipitation and the related acidification of
surface water in North America. Water Supply Paper
2249. U.S. Geological Survey. 18 pp.
Ulrich, B. 1981. Okosystemare Hypothese uber die
Ursachen des Tanneusterbens. Forstwiss. Centralbl.
100:228-238.
Ulrich, B. 1983. Stabilitat van waldokosystemen unter
dem einfluss des "Sauren regens. n Allg. Forstz.
26/27:670-677.
Van Breeman, N., P. A. Burrough, F. J. Velthorst, H. F.
van Dobben, T. deWitt, T. B. Ridder, and H. F. R.
Reijuders. 1982. Soil acidification ammonium sulfate
in forest canopy throughfall. Nature 299:548-550.
Vermont Department of Water Resources and Environmental
Engineering. 1983. Vermont acid precipitation
program--long-term lake monitoring. Vermont Department
of Water Resources and Environmental Engineering,
Montpelier.
Wagner, D. P., D. S. Fanning, J. E. Foss, M. S.
Patterson, and P. A. Snow. 1982. Morphological and
mineralogical features related to sulfide oxidation
under natural and disturbed land surfaces in Maryland.
Chapter 7 of Acid Sulfate Weathering, J. A. Kittrick,
D. S. Fanning, and L. R. Hossner, eds. SSSA Special
publication 10. Soil Society of America, Madison, Wisc
Warfel, H. E. 1939. Biological survey of the Connecticut
watershed. New Hampshire Fish and Game Commission,
Concord.
Watt, W. D., D. Scott, and S. Ray. 1979. Acidification
and other chemical changes in Halifax County lakeS
after 21 years. Limnol. Oceanogr. 24:1154-1161.
Wright, R. F. 1983. Predicting Acidification of North
American Lakes. Norwegian Institute for Water Research
(NIVA) report 4/1983. Oslo, Norway. 165 pp.
Wright, R. F. 1984. Regional pattern of sulfate
concentrations in lakes in Eastern North America.
Paper submitted to Committee on Monitoring and
Assessment of Trends in Eastern North America,
National Research Council. May 1984.
.
OCR for page 299
299
Wright, R. F., and E. T. Gjessing. 1976. Acid
precipitation: changes in the chemical composition of
lakes. Ambio 5:219-223.
Zimmerman, A. P., and H. H. Harvey. 1979. Sensitivity
to acidification of waters of Ontario and neighboring
states. Final report to Ontario Hydro. University of
Toronto, Ontario. 118 pp.
Representative terms from entire chapter:
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