FWS/OBS-80/40.18 Air Pollution and Acid Rain
October 1984 Report No. 18
EFFECTS OF ACIDIC PRECIPITATION
ON ATLANTIC SALMON RIVERS
IN NEW ENGLAND
Office of Research and Development
U. S. Environmental Protection Agency
Fish and Wildlife Service
U. S. Department of the Interior
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REPORTS ISSUED
FWS/QBS-80/4Q.1
FWS/OBS-80/40.2
FWS/OBS-80/40.3
FWS/OBS-
FWS/OBS-
FWS/OBS'
FWS/OBS'
FWS/OBS'
FWS/OBS
FWS/OBS'
FWS/OBS
80/40.4
80/40.5
-80/40.6
-80/40.7
-80/40.8
-80/40.9
-80/40,10
-80/40.11
FWS/OBS-80/40.12
FWS/OBS-80/40.13
FWS/OBS-80/4Q.14
FWS/OBS-80/40.15
FWS/OBS-80/40.16
FWS/OBS-80/40.17
FWS/OBS-80/40.18
Effects of Air Emissions on Wildlife Resources
Potential Impacts of Low pH on Fish and Fish Populations
The Effects of Air Pollution and Acid Rain on Fish,
Wildlife, and Their Habitats: Introduction
: Lakes
: Rivers and Streams
: Forests
: Grasslands
: Tundra and Alpine Meadows
: Deserts and Steppes
: Urban Ecosystems
Critical Habitats of
Threatened and Endangered Species
Effects of Acid Precipitation on Aquatic Resources:
Results of Modeling Workshops
Liming of Acidified Waters: A Review of Methods and
Effects on Aquatic Ecosystems
The Liming of Acidified Waters: Issues and Research -
A Report of the International Liming Workshop
A Regional Survey of Chemistry of Headwater Lakes and
Streams in New England: Vulnerability to Acidification
Comparative Analyses of Fish Populations in Naturally
Acidic and Circumneutral Lakes in Northern Wisconsin
Rocky Mountain Acidification Study
Effects of Acidic Precipitation on Atlantic Salmon
Rivers in New England
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UNITED STATES
DEPARTMENT OF THE INTERIOR
FISH AND WILDLIFE SERVICE
EASTERN ENERGY AND LAND USE TEAM
Route 3, Box 44
Keameysville, West Virginia 25430
Dear Colleague:
The Eastern Energy and Land Use Team (EELUT) is pleased to provide you
this report on the effects of acidic precipitation on Atlantic salmon
rivers in New England. This report is the eighteenth in our series
dealing with air pollution and acid rain. Other reports previously
issued are listed on the inside front cover.
This report describes the results of a water chemistry survey conducted
in eight rivers in Maine (Narraguagus, Sinclair, Machias, Kerwin, Holmes,
Old Stream, Bowles, and Harmon) and one in Vermont (White). All rivers
contain actual or potential Atlantic salmon spawning and nursery habitat
and the Maine rivers currently have native populations. The White River
is undergoing restoration of its population. Results of the survey indicate
pH and aluminum concentrations in second and third order streams are
within safe limits for Atlantic salmon but first order streams can reach
concentrations that may be toxic to sensitive early life stages or during
smoltification. These first order streams constitute 20-40% of the
available habitat.
Your comments and suggestions on this report are welcomed.
Sincerely,
R. Kent Schreiber
Acting Team Leader, EELUT
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FWS/OBS-80/40.18 Air Pollution and Acid Rain
October 1984 Report 18
EFFECTS OF ACIDIC PRECIPITATION ON ATLANTIC
SALMON RIVERS IN NEW ENGLAND
by
Terry A. Haines and John J. Akielaszek
U.S. Fish and Wildlife Service
Columbia National Fisheries Research Laboratory
Field Research Station
Zoology Department, University of Maine
Orono, Maine 04469
Project Officers
R. Kent Schreiber/Paul Rago
Eastern Energy and Land Use Team
U. S. Fish and Wildlife Service
Route 3, Box 44
Kearneysville, WV 25430
Performed for:
Eastern Energy and Land Use Team
Division of Biological Services
Research and Development
Fish and Wildlife Service
U.S. Department of the Interior
Washington, D.C. 20240
Fish and Wildlife Service
U.S. Department of the Interior
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DISCLAIMER
Although the research described in this report has been funded wholly
or in part by the U.S. Environmental Protection Agency through Interagency
Agreement'No. EPA-82-D-X0581 to the U.S. Fish and Wildlife Service, it has
not been subjected to the Agency's required peer and policy review and
therefore does not necessarily reflect the views of the Agency. Mention of
trade names or commercial products does not constitute endorsement or
recommendation for use by the Federal Govrernment.
This report should be cited as:
Haines, T.A. and J.J. Akielaszek. 1984. Effects of acidic precipitation
on Atlantic salmon river in New England. U.S. Fish and Wildlife
Service, Eastern Energy and Land Use Team, FWS/OBS-80/40.18. 108 pp.
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Executive Summary
_A water chemistry survey was conducted in nine Atlantic salmon rivers
in New England. Eight rivers are in Maine and contain native Atlantic
salmon populations. One river^is in Vermont and is undergoing restoration
of the Atlantic salmon population. The rivers ranged in size from first
order tributary streams to third order main stem rivers. All contained
actual or potential Atlantic salmon spawning and nursery habitat.
The chemistry of the Maine rivers was similar to that reported for
other rivers located in areas where bedrock is low in acid neutralizing
capacity and where precipitation is similarly acidic. The major cation was
calcium in all rivers; the major anion was sulfate in all except a few high
order streams where bicarbonate concentrations slightly exceeded sulfate.
The Vermont river had much higher concentrations of all ions except
aluminum and hydrogen than the Maine rivers, especially calcium, magnesium,
and bicarbonate, indicating the presence of carbonate mineral in the
watershed of this river.
All rivers exhibited a seasonal pattern of chemical change, although
changes were relatively small in the Vermont river. River pH, alkalinity,
and calcium, magnesium, sodium, and potassium concentrations decreased
during periods of high discharge in the spring and fall. Aluminum
concentrations increased during high discharge, and sulfate and nitrate
concentrations peaked at snowmelt, preceeding peak discharge. High
discharge periods resulted from snowmelt and increased precipitation in the
spring, and increased precipitation in the fall. The decrease in cations
and alkalinity was the result of dilution of base flow by runoff. The
decrease in pH (increase in hydrogen ion) probably results from dilution of
alkalinity by runoff, and the increase in sulfate and nitrate probably
results from the higher concentrations of these ions in snow and runoff
than in base flow. Increased aluminum concentrations may result from
increased solubility of aluminum in soil and sediment at reduced pH.
The net discharge of total ions from the watersheds exceeds the input
of ions from precipitation. The discharge of aluminum and part of the base
cations can be accounted for by input of hydrogen ion that is neutralized
by ion exchange and weathering reactions in the watershed. The discharge
of bicarbonate and the remainder of the base cations cannot be thus
accounted for and must therefore reflect internal hydrogen ion generation
in the watersheds, probably by dissociation of carbonic acid.
The pH and aluminum concentrations in second and third order streams
were well within safe limits for Atlantic salmon, even during periods of
high discharge. First order streams, however, reached levels of pH and
aluminum concentration that may be toxic to sensitive early life stages of
Atlantic salmon, or during smoltification, although conditions were not as
severe as those reported for Atlantic salmon streams in southern Norway or
southwestern Nova Scotia, where Atlantic salmon populations have declined
or disappeared apparently as a result of acidification.
Comparisons of chemical data from two rivers in this study with data
for 1969 indicated that conditions were very similar. Slight differences
in a few ions could be accounted for by differences in discharge. However,
iii
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aluminum concentrations were much higher in the present study. More acidic
deposition could have leached more aluminum from the watershed into the
streams, or the difference may result from differences in methodology.
present chemical conditions in high order streams are not critical
for Xtlantic salmon survival. However, first order streams, which
constitute 20-40% of the available habitat, now approach such conditions,?
and continued or increased deposition of acid may further degrade J
conditions in these streams.
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Table of Contents
Executive Summary H]
List of Figures vi
List of Tables i*
Li st of Abbrevi ati ons and Symbols x
Acknowledgements xl
I nt roduct ion 1
Methods 2
Selection of Sampling Sites 2
Sample Collection Procedure 2
Open Water Sampl es 2
Intragravel Samples 2
Analytical Methods 5
Field Procedures 5
Laboratory Procedures 5
Resul ts 7
Quality Assurance '
Precipitation and Discharge 7
Chemical Factors 7
pH, Alkalinity, and Conductance 7
Color 24
Al umi num 24
Cati ons 24
Ani ons 36
Ion Correlations 36
Ion Discharge 36
Intragravel Water 48
Comparisons with Previous Data 55
Di scussi on 64
Quality Assurance 64
Chemical Factors 64
pH, Alkalinity, and Conductance 64
Col or 65
Al umi num 65
Cati ons 66
Ani ons 66
Ion Correlations 68
Ion Discharge 68
Intragravel Water 74
Comparisons with Previous Data 75
Potential Effects on Atlantic Salmon 76
Conclusions 77
References 78
Appendi ces 83
A. Water Chemistry Data , 83
B. Salmon Redd Excavation 108
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List of Figures
Number
1. Map showing locations of Maine rivers 3
2. Calculated versus measured specific conductance 10
3. Sum of cations versus sum of anions 11
4. Discharge of the White and Narraguagus Rivers 13
5. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for the Narraguagus River. 14
6. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for Sinclair Brook 15
7. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for the Machias River 16
8. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for Kerwin Brook 17
9. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for Holmes Brook 18
10. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for Old Stream 19
11. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for Bowles Brook 20
12. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for Harmon Brook 21
13. Variation of pH, alkalinity, specific conductance,
color, and aluminum over time for the White Rive 22
14. Regression of log aluminum on pH 25
15. Variation of total concentrations of base cations
over time for the Narraguagus River 27
16. Variations of total concentrations of base
cations over time for Sinclair Brook 28
17. Variations of total concentrations of base
cations over time for the Machias River 29
18. Variations of total concentrations of base
cations over time for Kerwin Brook 30
VI
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19. Variations of total concentrations of base
cations over time for Holmes Brook ...................... 31
20. Variations of total concentrations of base
cations over time for Old Stream ........................ 32
21. Variations of total concentrations of base
cations over time for Bowles Brook ...................... 33
22. Variations of total concentrations of base
cations over time for Harmon Brook ...................... 34
23. Variations of total concentrations of base
cations over time for the White River ................... 35
24. Variations of total concentrations of major
anions over time for the Narraguagus River .............. 3/
25. Variations of total concentrations of major
anions over time for Sinclair Brook ..................... 38
26. Variations of total concentrations of major
anions over time for the Machias River .................. 39
27. Variations of total concentrations of major
anions over time for Kerwin Brook ....................... 40
28. Variations of total concentrations of major
anions over time for Holmes Brook ....................... 41
29. Variations of total concentrations of major
anions over time for Old Stream ......................... 4Z
30. Variations of total concentrations of major
anions over time for Bowles Brook ....................... 43
31. Variations of total concentrations of major
anions over time for Harmon Brook ....................... 44
32. Variations of total concentrations of major
anions over time for the White River .................... 45
33. Comparison of pH of ambient and intragravel stream
water over time for Bowles Brook and Old Stream ......... W
34. Comparison of alkalinity of ambient and intragravel
stream water over time for Bowles Brook and
01 d Stream
35. Comparison of specific conductance of ambient and
intragravel stream water over time for Bowles Brook
and Old Stream ............................. ............ 51
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36. Comparison of calcium concentration of ambient and
intragravel stream water over time for Bowles Brook
and Old Stream 52
37. Comparison of aluminum concentration of ambient and
intragravel stream water over time for Bowles Brook
and Old Stream 53
38. Comparison of sulfate concentration of ambient and
intragravel stream water over time for Bowles Brook
and Old Stream 54
39. Comparison of recent and previous pH for the
Narraguagus Ri ver 56
40. Comparison of recent and previous pH for the
Machias River 57
41. Comparison of recent and previous alkalinity for the
Narraguagus Ri ver 58
42. Comparison of recent and previous alkalinity for
the Machias River 59
43. Comparison of recent and previous specific
conductance for the Narraguagus River 60
44. Comparison of recent and previous specific
conductance for the Machias River 61
45. Comparison of recent and previous aluminum
concentration for the Narraguagus River 62
46. Comparison of recent and previous aluminum
concentration for the Machias River 63
vm
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List of Tables
Number
1. Physical characteristics of the streams selected
for study
2. Results of analysis of EPA Water Pollution Quality
Control Samples for Minerals
3. Results of analysis of EPA Water Pollution Quality
Control Samples for Trace Metals
4. Mean monthly precipitation and snow depth during
the study period ........................................ 12
5. Pearson product moment correlations of physical and
chemical factors with discharge ......................... 23
6. Mean chemical concentrations for the period of
measurement for all streams ............................. 26
7. Number and direction of significant correlation
coefficients among the ions measured .................... 46
8. Precipitation input, discharge output, and net retention
of ions for the Narraguagus and White rivers ............ 47
9. Mean concentrations of major ions in streams located
in areas where bedrock is resistant to weathering
and precipitation is acidic ............................. 67
10. Precipitation input, discharge output and net retention
of ions for watersheds located in glaciated areas of
North America and Europe ................................ 70
11. Comparison of various parameters assumed to reflect
acid deposition or cation discharge ..................... 72
12. Cation denudation rate and hydrogen ion deposition
rate for various watersheds ............................. 73
IX
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List of Abbreviations and Symbols
Abbreviations
AAS
ANC
CDR
FEP
1C
IP
mg/1
ueq/1
wg/1
z anions
i cations
Symbol s
AT
Ca
Cl
F
H
HCOo
K 6
Mg
Na
NOo
so43
Atomic absorption spectrophotometry
Acid neutralizing capacity
Cation denudation rate
Fixed end point
Ion chromatography
Inflection point
Milligrams per liter
Microequivalents per liter
Micrograms per liter
Sum of anions
Sum of cations
Aluminum
Calcium
Chlorine
Fluorine
Hydrogen
Bicarbonate
Potassium
Magnesium
Sodium
Nitrate
Sulfate
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Acknowledgements
Collection of water samples and measurement of temperature, pH,
alkalinity, and specific conductance for the White River, Vermont, was
performed by T. King, White River National Fish Hatchery, Bethel, Vermont.
M. Morrison and G. Blake conducted the cation and anion analyses. C.H.
Jagoe assisted with some chemical analyses. K.F. Beland, Maine Atlantic
Sea-Run Salmon Commission, assisted with site selection, collection of
intragravel water samples, and excavation of Atlantic salmon redds.
Precipitation chemistry data were supplied by T. Potter, Maine Dept. of
Environmental Protection, and J. Hornbeck, U.S. Forest Service. Discharge
data for the Narraguagus River were supplied by R. Haskell, U.S. Geological
Survey, Augusta, Maine.
XI
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Introduction
Atlantic salmon constitute an anadromous fishery resource of high
value. In the United States, Atlantic salmon formerly inhabited major
coastal rivers from Maine to Connecticut (Elson and Hord undated). They
entered at least 28 rivers and are estimated to have numbered around
300,000 fish (U.S. Fish and Wildlife Service 1983). A combination of
low-head dams without fish passage facilities, municipal and industrial
pollution of spawning rivers, and overharvest resulted in the extirpation
of the species from most of its range by the late 1800s.
Presently, self-sustaining Atlantic salmon populations exist in the
Dennys, East Machias, Machias, Narraguagus, Pleasant, and Sheepscot rivers
in Maine, and number around 2,000 fish (U.S. Fish and Wildlife Service
1983). Small, self-sustaining populations also exist in a number of small
coastal drainage systems (e.g., Ducktrap, Passagassawaukeag, Tunk, and
Hobart Stream drainages), and intermittent spawning occurs in additional
streams (Beland 1983). Hatchery assisted populations are being developed
in the Penobscot, St. Croix, and Union Rivers in Maine, the Merrimack River
in New Hampshire, the Connecticut River in Connecticut, Massachusetts,
Vermont, and New Hampshire, and the Pawcatuck River in Rhode Island. The
hatchery assisted populations number around 4,000 fish (U.S. Fish and
Wildlife Service 1983).
The present and historical range of the Atlantic salmon in the United
States receives precipitation that is highly acidic, with a mean annual
volume weighted pH of 4.2-4.4 (National Atmospheric Deposition Program
1983.) This area is also characterized by low alkalinity surface waters
that are vulnerable to acidification (Omernik and Powers 1982). Acidic
precipitation has caused acidification of Atlantic salmon spawning rivers
and resulted in reduction or elimination of fish populations in southern
Norway (Overrein et^ a^L 1980), and southwestern Nova Scotia (Watt et al.
1983). A survey of chemistry of headwater lakes and streams in New England
identified a number of Atlantic salmon spawning and nursery streams that
were very low in alkalinity (Haines and Akielaszek 1983). Inasmuch as
these streams were sampled at summer base flow the pH minima could not be
determined.
This study was conducted to determine whether some of .the Atlantic
salmon resources in New England are at risk from acidification as a
consequence of acidic precipitation. We selected nine Atlantic salmon
streams for an intensive water chemistry survey. Eight of these were in
Maine and presently support major naturally reproducing populations of
Atlantic salmon; one was in Vermont and is receiving hatchery
introductions. An effort was made to locate previous water chemistry data
that could be compared to the present data.
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Methods
Selection of Sampling Sites
The eight streams in Maine (Figure 1) were selected to be
representative of first, second, and third order Atlantic salmon spawning
and nursery streams in the state. Additional criteria for selection
included^relatively low color (dissolved organic carbon), low ionic
strength," lack of direct human disturbance (roads, logging, etc.),
availability of previous chemistry data, and winter access. The White
River, Vermont, was also selected for study. The primary criterion was
availablity of personnel at the White River National Fish Hatchery to
collect, analyze, and ship samples. A secondary consideration was the
importance of this river in the restoration plans for the Connecticut River
system. The sampling station was located at the White River National Fish
Hatchery, Bethel, Vermont. Physical characteristics of the sampling sites
are given in Table 1.
Sample Collection Procedure
Open Water Samples
Open water samples were collected by dipping water directly into
sample containers at approximately mid-channel. Sample containers were
linear polyethylene bottles with polyseal caps. The bottles were
acid-washed, distilled water rinsed, and stored filled with deionized,
distilled water (specific conductance <2 uS/cm). The bottles were rinsed
with sample water three times before being filled. Each set of samples
consisted of three bottles one 500 ml for pH, alkalinity, specific
conductance, and color; one 250 ml for anions; and one 125 ml for cations.
The cation sample was preserved with 6.25 ml of 4 N ultrapure nitric acid;
the remaining samples were placed on ice until analyzed. During winter
months if the stream was completely ice covered a hole was cut through the
ice with a 20 cm diameter auger. Ice chips were removed and the sample was
then dipped from the hole.
Samples were collected from most streams from about November 1, 1981,
to June 1, 1982. The White River was sampled once weekly. The Maine
rivers were sampled at various intervals ranging from twice weekly to once
every three weeks. Generally, samples were collected more frequently
during spring and fall, when chemical conditions were changing rapidly.
Intragravel Samples
Intragravel water samples were collected from two sites, Bowles Brook
and Old Stream, in the vicinity of naturally spawned redds. A standpipe
was constructed generally similar to the Mark VI groundwater standpipe
described by Terhune (1958), except that the pipe used was plastic, annular
grooves were omitted, and an oak driving point was cemented into the bottom
end. The standpipe was driven into the gravel so that the inlet holes were
25 cm below the gravel surface. A water sampling apparatus was constructed
as described in Koo (1964), and was used to pump water from the standpipe
into the sample bottles. Samples were then handled as described for open
water samples.
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Kerwin Bk
MACHJAS RIVER
N
ATLANTIC OCEAN
Figure 1. Map showing locations of Maine rivers.
3
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Table 1. Physical characteristics of the streams selected for study.
Drainage Order
River Basin
Narraguagus Narraguagus 3
Sinclair Narraguagus 2
Machias Machias 3
Kerwin Machias 1
Holmes Machias 1
Old Stream Machias 3
Bowles Machias 2
Harmon E. Machias 1
White Connecticut 3
Drainage Bedrock
Area Class
(km ) (percent)
581 1 (80%)
2 (10%)
3 (10%)
11 3 (100%)
1,173 1 (30%)
2 (40%)
3 (30%)
11 1 (100%)
31 1 (75%)
2 (15%)
3 (10%)
274 1 (50%)
3 (50%)
14 1 (100%)
10 2 (10%)
3 (90%)
1,823 2 (60%)
3 (40%)
Soil Mean
Class Color
(percent) (Pt/Co unit
SSI (70%)
SS2 (30%)
SSI (60%)
SS2 (40%)
SSI (25%)
SS2 (75%)
SSI (40%)
SS2 (60%)
SSI (60%)
SS2 (40%)
SSI (30%)
SS2 (70%)
SSI (50%)
SS2 (50%)
SS2 (100%)
NS (100%)
65
42
75
94
92
81
90
54
0
Drainage area at the mouth of the river, except for the Narraguagus River at Cherryfie
Maine, and the Machias River at Whitneyville, Maine.
1 = low to no buffering capacity (granite, gneiss, quartz, sandstone), 2 = medium/low
buffering capacity (sandstones, shale, metamorphic felsic to intermediate volcanic rock:
3 = medium/high buffering capacity (slightly calcareous, low grade intermediate to mafi
volcanic rocks). After Hendrey et^ a/[. (1980).
NS = mostly non-sensitive soils, soils are calcareous or subject to frequent flooding,
cation exchange capacity (CEC) >15.4 meq/lOOg; SSI = slightly sensitive soils dominate,
CEC - 6.2 to 15.4 meq/lOOg; SS2 = slightly sensitive soils significant but cover less t
50% of the area. After McFee (1980).
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Analytical Methods
Field Procedures
Analyses of pH, alkalinity, specific conductance, and color were
performed at field locations. Within 8 hours after sampling, and as soon
as possible, the 500 ml bottle was removed from ice and warmed to room
temperature. Two 100 ml aliquots were removed for determination of pH and
alkalinity. The pH was measured with a portable meter (Fisher model 107 or
Cole Parmer DigiSense) equipped with a plastic-body, gel filled,
combination electrode. The meter was standardized with pH 7.00 and 4.01
NBS certified buffers, and electrode response was verified by measuring the
pH of dilute sulfuric acid solutions of theoretical pH 4.00. If measured
values deviated from expected values by more than 0.1 pH units the
electrode was discarded. The electrode was rinsed thoroughly with
distilled water, blotted dry, and soaked in the sample for 15 minutes or
longer -- until three successive readings at 1 minute intervals were
identical and pH was recorded.
Alkalinity was determined by titrating each of the 100 ml sample
aliquots with 0.0200 N sulfuric acid to pH <4. Acid was added in 0.10 ml
portions using a micro syringe until pH 5 was reached, then in 0.05 ml
portions to pH <4. The pH was recorded after equilibration following each
addition of acid. Alkalinity was calculated by two methods. Inflection
point alkalinity was determined by the method of Gran (Stumm and Morgan
1981), and fixed endpoint (pH 4.5) alkalinity was determined as described
in American Public Health Association e_t aj_. (1975). Inflection point
results were used for all analyses and comparisons except for those using
previous data, where fixed endpoint data were used.
Two 50 ml aliquots of sample were measured and used for determination
of specific conductance and color. Specific conductance was measured with
a calibrated meter (Markson Scientific Company model 10), and apparent
color was determined by comparison of unfiltered samples with platinum
cobalt standard solution (LaMotte Chemical Company, Chestertown, Maryland).
Stream discharge data for the Narraguagus and White rivers were obtained
from the U.S. Geological Survey. Precipitation chemistry data for the
Acadia National Park, Maine, and Hubbard Brook, New Hampshire, sites were
obtained from the National Atmospheric Deposition Program. Data for amount
of precipitation in the study areas were obtained from various U.S. Weather
Bureau sites.
Laboratory Procedures
The remaining water samples were kept on ice, returned to the
laboratory, and kept refrigerated until analyzed. The acidified sample was
analyzed for cations. Sodium and potassium were determined by
air-acetylene flame atomic absorption spectrophotometry (AAS; Perkin Elmer
model 703), calcium and magnesium were determined by nitrous
oxide-acetylene flame AAS, and aluminum by graphite furnace AAS. Samples
were not filtered. The unacidified samples were filtered through Whatman
42 ashless filters and analyzed for chloride, nitrate, sulfate, and
fluoride by ion chromatography (Dionex model 16) following the
manufacturer's recommended procedures. Organic anions were estimated by
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first estimating dissolved organic carbon (DOC) from color measurements
using a linear regression equation derived previously (Haines and
Akielaszek 1983), then multiplying DOC by the factor 0.6 to obtain Peq/1 of
organic anions (A. Henriksen, Norwegian Institute of Water Research,
personal communication). Where necessary, ions were corrected for marine
aerosol input by assuming that all chloride resulted from marine aerosols
and that the ratio of other ions to chloride was the same in marine
aerosols as in sea water. Non-marine ion concentrations were obtained by
subtracting estimated marine contributions from total ion concentrations.
Because all sampling sites were upstream from roads, and all except the
White River were remote from any road, the influence of deicing salt on
chloride concentrations was expected to be minimal.
Quality assurance of analytical procedures was performed as specified
in a quality assurance project plan filed with the U.S. Environmental
Protection Agency. Analytical instruments were maintained and serviced
regularly, and precision was determined by analysis of U.S. Environmental
Protection Agency Water Pollution Quality Control Samples for Trace Metals,
and Minerals (EPA Environmental Monitoring and Support Laboratory,
Cincinnati, Ohio). Ionic balance and calculated (theoretical) versus
measured specific conductance also were used as a check on analytical
accuracy and data coding errors. Theoretical specific conductance was
calculated by multiplying ion concentrations by equivalent conductance
values (Weast 1978).
Most previous water chemistry data located for the rivers studied
consisted largely of single grab samples, or samples collected at i
infrequent intervals. The most useful data were very complete chemical
analysis of monthly water samples from the Narraguagus and Machias Rivers,
collected in 1969. These data were located in an unpublished report
(intended as a Master of Science thesis but never defended) in the files of
the Maine Cooperative Fishery Research Unit, University of Maine.
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Results
Quality Assurance
The laboratory analyses of EPA Water Pollution Quality Control Samples
for Minerals (Table 2), and Trace Metals (Table 3) gave acceptable
precision. The precision we obtained equalled or exceeded that of the
laboratories reported by EPA in all cases. The bias for mineral analyses
was less than 10%, but bias for aluminum and manganese frequently exceeded
10%. Bias was generally lowest for the highest concentrations. No
correction for bias was applied to the results presented later.
A further check on data quality was made by comparing measured and
calculated specific conductance (Figure 2). The intercept of the
regression is slightly less than zero and the slope is somewhat greater
than one. This indicates that the calculated values exceed measured values
at high concentrations. Additionally, cations and anions were summed
separately for each sample, and total cations were plotted against total
anions (Figure 3), which gave very similar results.
Precipitation and Discharge
The mean monthly precipitation received, and mean monthly depth of
snow on the ground at the nearest weather bureau station for the Maine
rivers and the White River are shown in Table 4. Precipitation is
considerably higher in Maine than in Vermont. Precipitation is higher in
s||rin§ and fall than in summer and winter in both areas, but the timing of
the precipitation maxima shifts from year to year. Both areas generally
have snow on the ground from November to April, but snow depth is greater
in Vermont.
/ Two of the rivers, Narraguagus and White, contain hydrologic gauges
operated by the U.S. Geological Survey. Daily discharge for each sample
date for these rivers (Figure 4) is highly variable but tends to be highest
in spring and fall, and lowest in summer and winter. Intense precipitation
events can increase discharge at any time of year. The 1981 water year was
characterized by multiple discharge peaks.
Chemical Factors
pH, Alkalinity, and Conductance
The pH, alkalinity, and conductance values followed similar temporal
patterns in all rivers (Figures 5-13) and were negatively correlated with
discharge (except for pH in the White River; Table 5). The general pattern
was relatively high values during winter, a sharp decline at spring peak
discharge, increasing values during summer, a decline in autumn, and an
increase in winter. This pattern was clear for 1980 and 1982 in the
Narraguagus, Machias, and Kerwin streams, but was obscured during 1981. In
the remaining streams pH, alkalinity, and conductance increased from autumn
to winter, were relatively high and stable during winter, declined at
spring peak discharge, and increased during summer. Higher order streams
had higher pH, alkalinity, and conductance values at all times of the year
than did lower order streams.
-------
Table 2. Results of Analysis of EPA Water Pollution Quality Control
Sample for Minerals. Mean Values of pH were Computed from Hydrogen Ion
Concentrations.
EPA Sample
Number Factor
3 pH
(units)
Calcium
(mg/1)
Magnesium
(mg/1)
Potassium
(mg/1)
Sodium
(mg/1)
Sulfate
(mg/1)
Chloride
(mg/1)
4 pH
(units)
Calcium
(mg/1)
Magnesium
(mg/1)
Potassium
(mg/1)
Sodium
(mg/1)
True
Value
7.4
6.7
2.4
1.7
7.0
12.0
20.5
8.6
32.0
7.1
7.2
40.0
X
(H-3)
7.54
6.8
2.4
1.6
7.2
12.0
20.3
8.56
34.8
7.1
7.5
40.1
Laboratory
S.D.
0.01
0.2
0.05
0.06
0.06
0.08
0
0.02
0.2
0.1
0.06
0.1
Results
Precision
+0.3%
±5.9%
±4.2%
±7.5%
±1.7%
±1.3%
IP
±0.5%
±1.2%
±2.8%
±1.6%
+0.5%
Bias
+1.9%
+1.5%
0
-5.9%
+2.8%
0
-1.0%
-0.5%
+8.8%
0
+4.2%
+0.3%
8
-------
Table 3. Results of Analysis of EPA Water Quality Control Samples for Trace Metals. All units are ug/1
EPA Sample Trace
Number Metal
1 Al
Mn
2 Al
Mn
3 Al
Mn
True
Value
350
55
50
11
700
350
Laboratory
X
(N=3)
424.3
62.3
68.3
13.7
726.7
387.5
S.D.
29.9
2.6
5.5
0.6
46.2
6.5
Results
Precision
±14.1%
± 8.3%
+16.1%
+ 8.8%
±12.7%
± 3.4%
Bias
+21.2%
+13.3%
+36.6%
+24.5%
+ 3.8%
+10.7%
X
369
54.8
74.9
11.0
712
348
EPA
S.D.
41.7
5.7
24.3
3.8
62.1
18.6
Recovery
F'recision
±22.6%
±20.8%
±64.9%
±69.1%
±17.4%
±10.7%
Bias
+ 5.4%
- 0.4%
+49.8%
0
+ 1.7%
- 0.6%
-------
80-1
70-
60-1
C
fl 50-
L
C
U 40-
L
fl
T 30-
E
D
20-
10-
0-
T
10 20 30 40 50 60 70
MEflSURED
80
Figure 2. Calculated versus measured specific conductance. Regression
equation: Calculated = -5 + 1.11 Measured (r_2 = 0.99, £ = 0.0001, N :
10
-------
S 700-
U
M
600J
0
F
500
C
fl
T 400-
I
0
N 300
U 200
E
Q
/ 100
L
0-
100 200 300 1400 500 600 700
SUM OF ONIONS UEQ/L
800
Figure 3. Sum of cations versus sum of anions. Regression
equation: cations = -16 + 1.04 anions (r2- = 0.97,
£ <0.0001, N = 173).
1]
-------
Table 4. Mean monthly precipitation, 30 year average precipitation (1931-1960), and mean monthly snow
depth, in mm, for Oonesboro, Maine, and Montpelier, Vermont, during the study period.
ro
Precipitation
Month
Jan
Feb
Mar
Apr
May
Jun
Jul
Aug
Sep
Oct
Nov
Dec
Total
1980
39
56
157
130
23
91
89
36
110
159
175
84
1,149
1981
47
70
59
174
109
126
183
91
126
121
113
217
1,436
1982
158
91
86
121
20
122
93
108
67
49
115
58
1,087
Jonesboro
Depth of Snow
30 yr
Avg 1980 1981 1982
123 22 373 325
107 126 52 469
107 86 87 293
104 2 31
90
95
86
79
113
104
134 34 2
114 180 55 47
1,255
Montpelier
Precipitation Depth of Snow
1981
5
159
16
66
143
92
91
83
146
79
39
59
979
1982
75
46
70
47
42
170
27
58
52
41
77
38
719
30 yr
Avg 1981
91 127
77 53
98 109
99
101
102
105
89
100
86
104 8
89 437
1,142
1982
630
663
434
41
3
16
-------
NARRAGUAGUS
120-1
OCT
1980
MAR AUG
1981
JAN OUN
1982
WHITE
150-
0 125-
I
S
C
H 100-
H
n
G
E 75-
H
3
/ 50-
S
25-
0-
i. m». 1.1. IH..,.....MI.I....I.|III.'.."|."'" ni|iiiiiii»i M
OCT DEC FEB APR
1981 1982
JUN
Figure 4. Discharge of the White and Narraguagus rivers,
13
-------
p
H
U
N
I
T
S
7.5-
7.0-
6.5-
6.0-
5.5-
250-
200-
U 150-
E
Q 100^
/
L 50H
0-
50-1
U «iC
S
C 30-
M
20^
C
0 125-j
L
0
R
75^
U
N
I
T
S
300-
250-
U 200-
G
/ 150H
L
100-
50-
111111111111111111111
10
15
20
Figure 5. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for the
Narraguagus River.
14
-------
p
H
U
N
I
T
S
6.5-
6.0-
5.5-
5.0-
U.5-
50-
U
E
Q
/
L
-10-
30-
U 25-
S
/
C 2
M
15-
100-
80
c
0
L
0
R
20-
UOO-
300-
U
G 200^
L 100^
0-
1 1
OCT
" -
l l
DEC
1
FEE
_ - '
1 1 1
APR
JUN
1981
1982
Figure 6. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for Sinclair
Brook.
15
-------
7.0-
P
H 6.5-
U 6.0-
N
I 5.5J
T
S 5.0-
125-
100-
U 75-
E
Q 50H
L 25-
0-
U 30-
S
/
C 2
M
200-
160-
C
0
0 80-
R
«iOO-
300-
U
G 20CH
L 100
0^
P"1
DEC
M ' ' ' ' ' I
|iini|i in i|in |'I
i i i i i i i i I i i i i i
MAR JUN
1980
SEP DEC MAR
a
I ' " " I
' I' " " I I i i i i | r
JUN SEP DEC MAR JUN
1981
1982
Figure 7. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for the
Machias River.
16
-------
p
H
U
N
I
T
S
6.5-
6.0-
5.5-
5.0-
11.5-
75-
50-
25-
0-
-25-
35-
30-
U
S 25-
C 20-
M
300-j
C
0 250-^
L
0 200H
R
U
N
I
T
S
50-
U50-
350-
U
G 250-^
L 150-
50-
DEC
a
MAR
JUN
1980
SEP
DEC
MAR
JUN
1981
SEP
DEC
1 1 1 ..... 1 1
MAR JUN
Figure 8. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for Kerwin Brook
17
-------
6.5H
H 6.0-
U
N 5.5-
I
T
S 5.0-
75'-
U 50-
E
Q
/ '
-------
7. OH
p
H 6.5-1
U
N 6.0-
I
T
S 5.5-
150H
U 100-
E
Q
/ 50H
L
0-
35-
30-
U
S 25-
C 20-
M
15-
125H
[III II II ll|lll II Illl |l
C 100-
0
L
0 7
R
50-
200-1
150-
U
G
/ 100-1
L
OCT DEC
1981
FEB
APR
JUN
1982
Figure 10. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for Old Stream.
19
-------
p
H
U
N
I
T
S
6.5-
6.0--
5.5-
5.0-
>4.5-
100-
75-
50-
25-
-25-
30-
U
S
/
C
H
15H
150-
C
a
L
0
R
U
N
I
T 50-1
U
G
«IOO-
300H
200-\
100-
OCT
T~
DEC
a
iiu n| 11
I"
FEB
APR
JUN
1981
1982
Figure 11. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for Bowles Brook,
20
-------
p
H
U
N
I
T
S
7.0-
6.5
6.0-j
5.5-
125-
100-
75-
50-
25-
0-
30H
U 25H
S
/
C 20-]
H
15-
a
c
0
L
0
R 50^
U
N
I
T
S
0-
Ill|lllllllll[
l|lllll Illl[i
300H
U
G
/
L
0-
e
OCT
I
DEC
I
FEB
APR
JUN
1981
1982
Figure 12. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for Harmon Brook.
21
-------
7.5H
P
H 7.OH
U
N 6.5-
I
T
S 6.0-
a
u 300-
E
Q
/ 200^
L
100-
80-1
U
3
/
C
H
40-
II Mil II [III llll II|MIII I III [111 II II ll|l II I I 1111)11111 II 11)11111 II !.[.... |.
5-
C
0
L
0
R 0-
250-
200-
U 150-
G
/ 100-
L
0-J
T
OCT
r~
1981
T~
DEC
FEB
APR
JUN
e
1982
Figure 13. Variation of pH (a), alkalinity (b), specific conductance
(c), color (d), and aluminum (e) over time for the White River,
22
-------
Table 5. Pearson product moment correlations of physical
and chemical factors with discharge for the two gauged
streams.
Factor
pH
Alkalinity
Specific Conductance
Color
Calcium
Magnesium
Sodium
Potassium
Aluminum
a
Sum of cations
Sulfate
Nitrate
Chloride
Fluoride
Sum of anions
White R.
-0.15
**
-0.82
**
-0.82
*
0.47
**
-0.85
**
-0.55
*
-0.47
-0.51*
**
0.83
**
-0.77
**
-0.80
0.35
-0.31
-0.17
**
-0.81
Narraguagus R.
-0.62
-0.67
-0.48
0.04
-0.62
-0.51
**
-0.37
0.02
0.45
-0.61
-0.16
-0.02
-0.24
-0.50
-0.80
^Excluding aluminum.
^Significant at £ £0.05.
Significant at £ <0.01.
23
-------
Color
The White River was virtually colorless; the Maine rivers were
moderately colored, ranging from 20 to nearly 300 units and averaging 30-40
units (Figures 5-13). Color changed seasonally, being lowest from late
winter to early summer and highest from late summer to early fall.
However, color was not correlated with discharge (Table 5). Color appeared
to decline in winter, when discharge was low, and did not increase until
summer, when discharge was also low.
Aluminum
Aluminum concentration exhibits a seasonal cycle that is the inverse
of that for pH and alkalinity (Figures 5-13). Concentrations are highest
when pH is lowest and alkalinity is lowest. Aluminum is significantly
positively correlated with discharge in the two gauged rivers (Table 5),
and with pH in all rivers combined (Figure 14). Aluminum concentrations
are generally higher in lower order streams, which are also lower in pH
than higher order streams. A linear regression of aluminum with color
yielded significant regressions in three of eight rivers. Regression was
not performed for the White River as color was zero for all but one sample
date. The significanto(p_ <0.0001) regressions were for Bowles Brook(jr =
0.73), Holmes Brook (_r = 0.73), and Harmon Brook (r_ = 0.77). Aluminum
may have been bound to dissolved to organic compounds in these streams. We
measured only total aluminum in this study.
Cations
Mean cation concentrations for the period of measurement are given in
Table 6, and temporal trends are shown in Figures 15-23. Cation
concentrations were generally higher in the higher order streams. Calcium
was the most abundant cation in all third order streams. Sodium exceeded
calcium in all first and second order streams except Harmon Brook, where
calcium was most abundant. Sodium was nearly as abundant as calcium in all
Maine rivers, but was much lower than calcium in the White River.
Magnesium was intermediate and potassium was lowest in concentration in all
streams.
Potassium concentrations were nearly constant over time with no
apparent temporal pattern. Magnesium was relatively constant over most of
the year but concentrations generally declined in spring during the period
of snow melt and high discharge. This occurred in April in 1980 and 1982,
but multiple discharge peaks occurred in 1981 (December 1980, March, May,
July, and August 1981). Snow cover disappeared in February and March in
1981.
Calcium and sodium had similar seasonal patterns of concentration.
Concentrations were highest in August and lowest in April in 1980 and 1982.
Again, 1981 was characterized by multiple cycles. Sodium concentrations in
the Narraguagus River were different from calcium in 1980, but were similar
thereafter. All cations were negatively correlated with discharge (Table
5), except potassium in the Narraguagus River.
24
-------
3.OH
D D DUD D
PH
Figure 14. Linear regressions of log^o total aluminum concentration on pH.
Regression equation; Logic Al = 3.97 - 0.31 pH (_r2 = 0.36,
£ <0.0001, N = 333).
-------
Table 6. Mean chemical concentrations, for the period of measurement in the nine streams, organized by
watershed and order. Units are ueq/1 except as noted.
ro
Watershed Order
and Site
MaAAa.gua.gui>
Sinclair Bk.
Narraguagus R.
Kerwin Bk.
Holmes Bk.
Bowles Bk.
Old Str.
Machias R.
E. Mac/tou
Harmon Bk.
Connectccot
White R.
1
3
1
1
2
3
3
1
3
PH
5.56
6.33
5.31
5.52
5.36
6.19
6.09
5.95
6.83
Color
65
42
75
94
92
81
90
54
-------
n n
ro
200-
175-
ISO-
125-
U
E 100-
Q
L 75^
25-
0-
DEC
_ Na
APR AUG
1980
DEC
APR AUG
1981
DEC
APR
1982
AUG
Figure 15. Variation of total concentrations of base cations over time
for the Narraguagus River.
-------
ro
oo
70-
60-
U 50-
E
Q
/ HO-
L
30^
20-
OCT
DEC
FEB
APR
JUN
1981
1982
Figure 16. Variations of total concentrations of base cations over time
for Sinclair Brook.
-------
ro
i-O
150
140
120-
100-
U
E 80-
Q
0-
D- D Ca
DEC
+-+ K
APR AUG
1980
DEC
APR AUG
1981
DEC
APR AUG
1982
Figure 17. Variations of total concentrations of base cations over
time for the Machias River.
-------
150-1
125-
100-
u
E 75^
Q
50-1
25-
0-
Da c»
Mg
Na
-+ K
DEC APR AUG DEC
1980
APR AUG
1981
DEC APR AUG
1982
Figure 18. Variations of total concentrations of base cations over
time for Kerwin Brook.
-------
100-1
75
U
E 50-
Q
0-
I I I I I 11 11 I 111 11 I 11 I 11 I I 111 I I I 11
OCT DEC
1981
"I"
FEB
APR
JUN
1982
Figure 19. Variations of total concentrations of base cations
over time for Holmes Brook.
-------
co
ro
150-
140-J
120-
u
E
Q
L 60-
20-:
0-
II I I
4-M-
1 -H '
II I *- I
FEB APR JUN AUG OCT
1981
DEC FEB APR
1982
JUN
Figure 20. Variations of total concentration of base cations over
time for Old Stream.
-------
GO
co
U
E
Q
/
L
100-1
75-
50-
0-
H 1
1 1 1 ii ii ii ijii 1 1 1 n 1 1| 1 1 MI i M i| i
OCT DEC
1981
11111111111111 >f T 111111111111111111 [ 11111111111111111111
FEB
APR
JUN
1982
Figure 21. Variations of total concentrations of base cations over
time for Bowles Brook.
-------
CO
100-]
u
E
Q
75-
50-
25-
0-
OCT
DEC
1981
"I"
FEB
APR
JUN
1982
Figure 22. Variations of total concentrations of base cations over
time for Harmon Brook.
-------
CO
01
50CM
400-
300
U
E
Q
/ 200
L
100-
0-
1M 1 'I 4 II I III II i I I I1H-+
1111IIIII[IIIIIII11[ 11 111 111 n IIIIIIII1111
OCT DEC FEB
1981
..... ii 1 1 1 ii i
APR
M I I MI I|I I I I I II I I |
JUN
1982
Figure 23. Variations of total concentrations of base cations over
time for the White River.
-------
Anions
The most abundant anions in all streams were bicarbonate, sulfate, and
chloride (Table 6). Organic anions were intermediate in concentration in
all streams except the White River, where they were very low. Nitrate was
low in all streams except the White River, where it was intermediate.
Fluoride was very low in all streams.
Few anions other than alkalinity (bicarbonate) were correlated with
discharge (Table 5), although the sum of all anions was negatively
correlated. Both sulfate and nitrate (Figures 24-32) showed a tendency to
reach a peak concentration in March of 1981, proceeding the discharge peak
in April (Figure 4) and coinciding with the period of snowmelt (Table 4).
The nitrate peak was variable, sometimes sharp and sometimes broad. The
timing of the nitrate peak was somewhat later in the White River.
Chloride concentrations were highly variable. Generally there were
multiple chloride peaks, usually in the fall and again in late spring,
after peak discharge. Chloride concentrations were often stable during
winter. Organic anions usually reached their maximum concentration in
fall. There often also was a small peak coinciding with peak discharge in
April. Organic anions were very low and stable in the White River.
Fluoride concentrations were low and stable in all streams.
Ion Correlations
Simple product moment correlations were calculated for pH, alkalinity,
and all cations and anions. The number of significant (p _<0.05)
correlations out of the nine correlations for each pair, and the direction
of these correlations, were charted as an index of the overall significance
of each possible correlation (Table 7). Five or more significant
correlations of the same direction were judged indicative of a strong
relationship. There were 13 such strong relationships out of 66 possible.
Alkalinity was positively related to calcium, magnesium, and sodium, and
negatively related to aluminum. The relationships for pH were positive
with alkalinity and sodium, and negative with aluminum. Calcium was
positively related to magnesium and sodium. There were four other strong
relationships, all positive: magnesium with sodium, sodium with fluoride,
chloride with sulfate, and aluminum with organic anions.
Ion Discharge
Two rivers studied (Narraguagus and White) were gauged and discharge
records were available to enable calculation of discharge of major ions.
Precipitation input data for major ions were also available from National
Atmospheric Deposition Program stations at Acadia National Park, Maine,
(47 km from Narraguagus River) and Hubbard Brook, New Hampshire (76 km from
White River). The input and output of total ions were calculated on an
areal basis (Table 8). Total ions input from precipitation were estimated
by multiplying wet deposition by 1.5 (Wright and Johannessen 1980). Both
river systems discharged more calcium and magnesium than were input from
precipitation, but less hydrogen ion. Potassium was nearly balanced at
both sites, with input approximately the same as output. Sodium was nearly
balanced in the Narraguagus but there was an excess of discharge in the
36
-------
125
100-
75-
U
E
Q
50-
to
25-
0-
I I I I I I I I I 1 I I I I I I II I I I I II I I I I I I I I I I I I I I I I I I I I [ M I I I I I I 1 I I I I I I I M I I I I I I I I I I I I
OCT DEC FEB APR JUN
1980 1981
Figure 24. Variations of total concentrations of major anions over
time for the Narraguagus River.
-------
125-
100-
CO
00
75-
U
E
Q
/ 50-
L
25-
0-
OCT
DEC
r
I I I I I I I I I I I I I I I I I I I I I I I I I I I 1 II |T IT I I I If It
' I '
FEB
1980
11
1981
APR
JUN
Figure 25. Variations of total concentrations of major anions over
time for Sinclair Brook.
-------
CO
50-
U
E
Q
25-
I I I I I I I I
OCT
DEC
nj ii
FEB
APR
JUN
1980
1981
Figure 26. Variations of total concentrations of major anions over
time for the Machias River.
-------
.p.
o
100-1
u
E
Q
75
50-
25-
0-
OCT
I I I I I I I I
DEC
I I I I I I I
FEB
I I I I I I I I TI TIIIIlTIIIIIIII
APR
1980
1981
JUN
Figure 27. Variations of total concentrations of major anions over
time for Kerwin Brook.
-------
100-
u
E
Q
75-
50-
25-
0-
OCT
A
-H4
DEC
FEB
1 ' ' I "
APR
1980
1981
11
JUN
Figure 28. Variations of total concentrations of major anions over
time for Holmes Brook.
-------
100-J
75-
U
E 50-
Q
0-
I I 111 I» I
ITTi i i r I I i 1 I I I
OCT
DEC
FEB
APR
i i i i I
JUN
1980
1981
Figure 29. Variations of total concentrations of major anions over
time for Old Stream.
-------
100-1
75-
to
U
E 50
Q
25-
0-
A*.
I I M I I I I I I | I I ' I I I I I I | I ........ | I I I I I I I I I | I I I I I I I M pi I I
OCT DEC FEB
1980 1981
I I I M | I I I I II I I I | I I ....... |
APR JUN
Figure 30. Variations of total concentrations of major anions over
time for Bowles Brook.
-------
DD
A A
80-1
60-
u
E 40-1
Q
20-1
0-
S04
N03
Organic
Cl
F
-e-
^\ V
ff~^-A
i i 3* -^
I I I I I I I I I I | I I I I I M I I | I I I I I I I I I | I I I I I I I I I | I I I I
OCT DEC FEB
1980
I II I I | I I I I I I I M | I I I I I I H I | I I I I I I I I I |
APR
JUN
1981
Figure 31. Variations of total concentrations of major anions over
time for Harmon Brook.
-------
en
200-
150-
U
E 100-
Q
50-
0-
OCT
1980
DEC
I '
I I I II I rri I I I FT
FEB
1981
i 11 i 11 11 i
APR
i i i i i i i I
JUN
Figure 32. Variations of total concentrations of major anions over
time for the White River.
-------
Table 7. Number and direction of significant (£ <0.05) correlation
coefficients among the ions measured.
pH
alkalinity
calcium
magnesium
sodium
potassium
chloride
nitrate
sulfate
aluminum
fluoride
.? 1
c E -
i-31/l
-r- Q)
-o
tl
o
3
14-
1 +
3+
2+
2+
5+
1-
2+
0
0
1-
v
organic
anions
3-
3-
2+
4+
2+
2-
0
2-
2-
9+
1+
46
-------
Table 8. Precipitation input, discharge output, and net retention (input-output) of major ions for the
Narraguagus and White rivers. Units are meq/m /year except as noted.
Narraquaqus R.
p re c i p i t a t i on
Ca
Mg
Na
K
H
£ cations
HC03
so4
N03
Cl
Organic anion
z anions
water (mm)
wet
7
16
61
2
33
119
0
44
15
72
0
130
total
11
24
92
3
50
179
0
66
23
108
0
195
1,048
discharge
130
46
88
18
^1
284
87
81
10
61
59
298
768
net
retention
-119
-22
4
-15
49
-105
-87
-15
13
47
-59
-103
-280
White R.
precipitation
wet
5
3
3
0
34
45
0
33
21
4
0
58
total
8
5
5
0
51
68
0
50
32
6
0
87
886
discharge
182
67
86
8
<1
343
162
106
35
99
<1
403
626
net
retention
-174
-62
-81
-8
51
-275
-162
-56
-3
-93
%0
-316
-256
-------
White River. Inputs were relatively similar at the two sites for calcium,
magnesium, and hydrogen ion, but sodium and potassium were much higher at
the Narraguagus. Discharge of calcium, magnesium, and sodium were highest
in the White River.
Discharge of sulfate and chloride were higher than precipitation input
for the White River. The Narraguagus River retained chloride, and sulfate
was nearly balanced. Nitrate was nearly balanced in both rivers.
Bicarbonate discharge exceeds precipitation input, which is negligible for
this ion, for both rivers. Discharge of all anions, including nitrate, was
higher in the White River than in the Narraguagus River. Precipitation
input of chloride was highest in the Narraguagus River. Sulfate input was
also higher in the Narraguagus River, as was hydrogen ion, but nitrate
input was lower.
The ionic balance of both discharge output and precipitation input was
reasonably good. The cation denudation rate (CDR) for each of the gauged
rivers, defined as the discharge of non-marine cations excluding hydrogen
ion per unit watershed area, was 215 meq/m /yr for the Narraguagus River
and 232 meq/m /yr for the White River. The contribution of cations from
precipitation is negligible, except for hydrogen ion. The CDR model of
Thompson (1982) predicts a pH of 6.27 for the Narraguagus River and 6.51
for the White River. The CDR model as presented ignores nitrate, which was
significant in the White River. If nitrate is included in the model the
predicted pHs are 6.24 and 6.39 respectively. The actual volume weighted
mean pH was 6.02 for the Narraguagus River and 6.92 for the White River.
Intragravel Water
Intragravel water samples were very difficult to collect under the
conditions experienced. The standpipes froze, were dislodged by moving
ice, and filled with silt. The vacuum tubing froze and the pump
clogged with silt. Consequently, few water samples of adequate quality
were obtained for analysis: four samples from Bowles Brook and six from
Old Stream.
Intragravel pH (Figure 33), alkalinity (Figure 34), and specific
conductance (Figure 35) were generally higher than stream values for the
same sample dates. Both the stream and intragravel values follow similar
seasonal patterns, with no apparent time lag for the intragravel values.
Values for Old Stream almost always exceeded those of Bowles Brook. The
differences between the two sets of values were smallest during the period
of high discharge in April.
Intragravel values of calcium (Figure 36) and aluminum (Figure 37)
also generally exceeded stream values. The maximum aluminum concentrations
reached in intragravel water samples were as much as 40 times higher than
in stream water samples. Sulfate concentrations are slightly higher in the
stream than in intragravel water and are slightly higher in Bowles Brook
than in Old Stream (Figure 38).
48
-------
7.0-
6.5-
6.0-
5.5-
5.0-
14.5-
P
H "A.0-1
U 3.5
N
I 3.U-I
T
S 2.5-1
2.0-
1.5-
1.0-
0.5-
0.0-
T
DEC
1981
Bowles ambient
O---Q Bowles intragravel
Old Stream ambient
Old Stream intragravel
I
JAN
FEB
MAR
APR
MAY
1982
Figure 33. Comparison of pH of ambient and intragravel stream
water over time for Bowles Brook and Old Stream.
-------
en
o
R
I
K
fl
I
I
N
I
T
Y
U
E
Q
150-
125-
-* »
I
100-
owlet ambitnt
Q--D Bowlti intragravtl
JkA Old Stream ambient
AA Old Stream intragravei
0
APR
MAY
1982
Figure 34. Comparison of alkalinity of ambient and intragravei
stream water over time for Bowles Brook and Old Stream,
-------
HO-I
(Ji
30-
20-
c
0
N
D
U
C
T
R
N
C
E
U
s
/ 10-
c
M
Bowles ambient
Q-O Bowles intragravel
Old Stream ambient
Old Stream intragravel
0-
T
DEC
1981
JAN
FEB
MAR
I
APR
MAY
1982
Figure 35. Comparison of specific conductance of ambient and intragravel
stream water over time for Bowles Brook and Old Stream.
-------
tn
ro
C
R
L
C
I
U
M
U
E
Q
/
L
175H
150
125-
100-
75-=
50^
25-
0
Bowles ambient
Q---O Bowles intragravel
Old Stream ambient
Old Stream intragravel
DEC
1981
JAN
FEB
MAR
APR
MAY
1982
Figure 36. Comparison of calcium concentration of ambient and intragravel
stream water over time for Bowles Brook and Old Stream.
-------
CJ1
fl
L
U
M
I
N
U
M
U
G
L
HQOQ-
-
.
-
3000-
m
m
-
"
-
2000-
*"
"
\
-
1000-
-
«
m
-
*
0-
9
Bowles ambient / 1
i i
OQ Bowles intragravel / ,
i «
A A Old Stream ambient ' ',
i »
£s~-& Old Stream intragravel '
i »
j »
i i
i t
i i
i t
i i
* <
i »
i
'.
X 1
x' 1
1
s \
" \
f \
s t
X ^*~ \ |
' ««» N
/ ..--- \ 1
X N I
---"*" Xl
S^»~~"~~ \ *"'^,
f^2k i *Jk
f">"x \
qfel_ u ^ m
1 " "*
1 1 1 1 1 1
DEC JAN FEB MAR APR MAY
1981 1982
Figure 37. Comparison of aluminum concentration of ambient and intragravel
stream water over time for Bowles Brook and Old Stream.
-------
en
70-1
60-
50-
140-
5
U
L
F
F)
T
E
30-
U
E
Q
/ 20-
10-
0-
1
DEC
1981
Bowie* ambient
Q--D Bowles intragravel
Old Stream ambient
Old Stream intragravel
I
JAN
I
FEB
MAR
APR
MAY
1982
Figure 38. Comparison of sulfate concentration of ambient and intragravel
stream water over time for Bowles Brook and Old Stream.
-------
Comparisons with Previous Data
Previous chemistry data were available for the Narraguagus and Machias
rivers. Data were available for 10 samples collected nearly monthly from
February 1969 to January 1970 (Taylor 1973). The discharge of the
Narraguagus River on sample dates in 1969 was similar to that during our
sampling3period. The mean sample date discharge was 18 m /sec in 1969,
and 20/m /sec in 1981-82. Comparison of pH and alkalinity data from
1980-82 to those of 1969 (Figures 39-42) reveals no apparent differences.
The timing of annual cycles is similar and the maxima and minima are also
similar. The alkalinity data plotted for 1980-82 are fixed endpoint data,
which is what was measured in 1969. Specific conductance (Figures 43-44)
appears to have been slightly higher in 1980-82 than in 1969.
The only chemical factor that is markedly different between the
historical and recent data is aluminum (Figures 45-46). Total aluminum
concentrations were considerably higher for 1980-82, but seasonal patterns
were similar. Concentrations in 1980-82 appeared to be higher than in 1969
during periods of high discharge but similar to those in 1969 during
periods of low discharge.
55
-------
7.0-
P 6.5-
H
en
6.0-
5.5-
JAN MAR MAY JUL SEP
MONTH
NOV
JAN
Figure 39. Comparison of recent and previous pH for the Narraguagus River.
-------
en
7.0-1
6.5-
P 6.0-
H
5.5-
5.0-
A
o
X
1969
I960
198 1
1982
JAN MAR MAY
JUL SEP
MONTH
NOV
JAN
Figure 40. Comparison of recent and previous pH for the Machias River.
-------
en
CO
250-4
200H
R
L
K
R
L 150
I
N
I
Y
U
E
Q
100-
50-
0-
JAN MAR MAY
JUL SEP NOV
MONTH
JAN
Figure 41. Comparison of recent and previous alkalinity for the
Narraguagus River.
-------
en
15CH
125-
P
L
K 100-
R
L
I
N
I 75-
T
Y
U
E 50-
Q
0-
JAN
1
MAR
MAY
JUL
MONTH
SEP
NOV
JAN
Figure 42. Comparison of recent and previous alkalinity for the Machias River.
-------
50-1
UO-
C
0
N
0
U 30-
C
T
fl
N
C
E 20-
U
S
/
C
M 10-
0-
JAN
MAR
MAY
JUL
MONTH
SEP
NOV
JAN
Figure 43. Comparison of recent and previous specific conductance for
the Narraguagus River.
-------
uo-l
C 30-
0
N
D
U
C
T
fl 20
N
C
E
U
S
/ 10-1
C
M
0-
JAN
MAR
MAY
JUL
MONTH
SEP
NOV
JAN
Figure 44. Comparison of recent and previous specific conductance for
the Machias River.
-------
rto
fl
L
U
M
I
N
U
M
30CH
250-
200-
150-
U
G 100-
50-
0-
11111
i 11 11 i
JAN
MAR
MAY
JUL
MONTH
SEP
NOV
JAN
Figure 45. Comparison of recent and previous aluminum concentration for
the Narraguagus River.
-------
en
to
fl
L
U
M
I
N
U
M
U
G
350-1
300-
250-
200-
150-
100-
50-
0-
A
o
X
1969
1980
1981
1982
1 1 1 1 1 1
JAN
T-r i i | i i i i
MAR
MAY
1 ' ' ' i
JUL
MONTH
' i
SEP
1 ' ' ' ' TT "' ' '
NOV
JAN
Figure 46. Comparison of recent and previous aluminum concentration
for the Machias River.
-------
Discussion
Quality Assurance
Precision was high and bias was generally low for major ions, but were
variable and less satisfactory for aluminum and manganese. We believe that
the results are generally acceptable, however. The regressions of measured
on calculated specific conductance and sum of cations on sum of anions
indicate that there are no major measurement or coding errors in the data
set.
Chemical Factors
pH. Alkalinity, and Conductance
The seasonal pattern of change in these three factors is apparently
related to periods of high precipitation and increased discharge. The
magnitude and timing of the declines that we observed were similar to those
observed in other low order streams that are located in resistant bedrock
and that receive precipitation of similar chemistry (Jeffries et_ a]_. 1979;
Martin 1979;' Christophersen and Wright 1980; Colquhoun et_ al_. 1981; Webb
1982). These declines are associated with high precipitation and peak
stream discharge, and follow snowmelt. However, Watt et_ aU (1983) found
that the annual minimum pH and alkalinity occurred before the peak
discharge in Nova Scotia rivers. They attributed this to the fact that
snow was higher in pH than rain in this area so that snowmelt water did not
depress stream pH or alkalinity. In the White River, pH and alkalinity are
buffered by carbonate minerals in the watershed and show little
relationship to precipitation or discharge.
The fall pH, alkalinity, and conductance declines are also associated
with increased discharge that accompanies increased precipitation occurring
as rain, before soils freeze and a snowpack forms. Similar declines have
been observed in Norway (Webb 1982), Ontario (Jeffries et aJL 1979), Nova
Scotia (Watt et^ aj_. 1983), and New Hampshire (Martin 1977). Additional
declines occurred in our streams during the summer of 1981, following
intense precipitation events and again associated with increased discharge.
The summer declines may be enhanced by the fact that precipitation is more
acidic during summer than at other times of the year (National Atmospheric
Deposition Program 1983). During periods of high precipitation water may
enter streams via overland flow rather than percolation through soil.
In contrast to the above, Likens et_ al_. (1977) reported that stream ptt
in the Hubbard Brook Experimental Forest was very stable seasonally, which
was attributed to buffering by the terrestrial ecosystem. The stream pH
was chronically depressed below 5.0.
There appeared to be a general relationship between bedrock geology
class and soil sensitivity class in the watershed and stream pH,
alkalinity, and conductance. Streams that were lowest in pH and alkalinity
generally drained watersheds that had a high proportion of low sensitivity
bedrock, soil, or both (e.g., Kerwin Brook, Narraguagus River), whereas
streams that were highest in pH and alkalinity drained watersheds with a
preponderance of non-sensitive materials (e.g., Harmon Brook, White River).
64
-------
All rivers in Maine were located in areas with moderately sensitive soils
(McFee 1980), and all were lower in pH, alkalinity, and conductance than
the White River, which was located entirely in a non-sensitive soil area.
The lower pH, alkalinity, and conductance values in smaller, lower order
streams may also result from the smaller watersheds of these streams, which
provide less opportunity for precipitation water to percolate through soil.
The degree to which influent water passed through inorganic soil horizons
was found to be the critical factor governing lake pH and alkalinity in the
Adirondack Mountain region of New York (Chen et_ aU 1983). Small streams
also tend to have less diverse geology and soil types in their watersheds,
offering less opportunity for buffering from incursions of higher buffering
materials in the watershed. Johnson (1979) found that stream pH was highly
correlated with order for small streams in the Hubbard Brook, New
Hampshire, watershed. Low order streams had lower pH than higher order
streams in the same watershed, even though ionic strength was the same. He
attributed the neutralization of hydrogen ion to dissolution of preexisting
aluminum hydroxide compounds in the upper soil horizons.
Other authors, however, believe that hydrogen ion from precipitation
increases weathering reactions and is exchanged for base cations (Fisher et^
al. 1968; Martin 1979; Webb 1982). For example, Martin (1979) found that
pH~, alkalinity, and base cations increased from a headwater to a downstream
site in a watershed in New Hampshire. In our streams aluminum
concentration is highest in low order streams. As stream order increases
aluminum concentration declines but conductivity and alkalinity increase.
It appears that reduced pH increases aluminum solubilization initially.
Later, the hydrogen ion is exchanged for base cations, pH increases, and
aluminum is precipitated out of solution.
Color
Color is moderate to high in the Maine rivers, and virtually absent in
the White River. Color was highest from late summer to early fall and may
result from leaching of organic compounds from decaying vegetation at this
time. Color was lowest during spring when discharge was highest and pH was
lowest. Therefore the pH depression at high discharge cannot be attributed
to increases in organic acids.
Aluminum
The increase in aluminum concentration at periods of high discharge
probably results from increased aluminum dissolved from terrestrial rocks
and soils and aquatic sediments by the increased hydrogen ion, especially
considering that other cations decrease at this time. Many authors have
shown that lake aluminum is highly correlated with pH (Wright and 6jessing
1976; Dickson 1980; Wright and Henriksen 1980; Schofield 1982; Haines and
Alielaszek 1983), and this is consistent with the relationship between
stream pH and aluminum hypothesized by Johnson (1979).
Inasmuch as we did not filter our samples or fractionate aluminum
compounds, our data represent only total aluminum. Recent comparisons of
filtered and unfiltered samples in our laboratory show little or no
difference in aluminum concentration. We conclude that particulate
aluminum is very low in these streams. Color is appreciable in the Maine
65
-------
streams, and much of the aluminum may have been present as an organic
complex. Aluminum concentration was positively correlated with organic
anion concentration in all nine streams.
Cations
The concentrations of cations in the first order streams in Maine were
similar to those from comparable (similar order, bedrock and soil types,
and precipitation chemistry) streams reported elsewhere (Table 9). The
slightly higher sodium concentrations in our streams probably reflect the
proximity to the ocean; concentrations were even higher at Birkenes.
Higher order Maine streams had higher calcium concentrations, but other
cations were little, if any, higher than in first order streams. The White
River had much higher cation concentrations than third order Maine rivers,
reflecting the presence of more soluble bedrock and higher concentrations
of exchangable soil cations in this area. Calcium was the dominant cation
in all streams, as it generally is in surface waters world-wide
(Livingstone 1963).
The seasonal cycles of cation concentrations in our streams are
similar to those reported for New Hampshire streams (Likens et^ a]_. 1977;
Martin 1979). The spring and fall declines in cations result from dilution
of base flow by precipitation runoff and snowmelt. However, in Sweden
(Calles 1983) and Norway (Webb 1982), base cations, primarily calcium,
increase at spring snowmelt and high discharge, and decline in summer.
This is attributed to leaching of base cations by hydrogen ion. In our
streams hydrogen ion and aluminum increase at spring snowmelt and high
discharge. Increases in base cations occur at downstream locations in
higher order streams concomitant with decreases in hydrogen ion and
aluminum.
Anions
The most abundant anion in the low order streams was sulfate, and in
the higher order streams bicarbonate. Bicarbonate is the most abundant
anion in surface waters world-wide (Livingstone 1963). In acidified
surface waters sulfate replaces bicarbonate (Wright and Henriksen 1983).
Sulfate concentrations were not highly related to stream order in the Maine
streams, being only slightly lower in higher order streams (Table 9), but
sulfate was considerably higher in the White River than any Maine river,
even though the White River is not acidified. This may simply be a
reflection of the much higher concentration of all ions in this river,
inasmuch as bicarbonate far exceeds sulfate. Bicarbonate was higher in
third order than in first or second order streams in similar geological and
soil regions in Maine, possibly as a result of weathering reactions.
Nitrate was generally present at very low concentrations in the Maine
rivers. This is expected because of the high biological uptake rates for
this important nutrient. The intermediate nitrate concentration in
Sinclair Brook is unexplained. Nitrate was consistently elevated in all
samples and good ionic balance is achieved, ruling out analytical error.
Nitrate was relatively high in the White River, probably as a result of
agricultural and urban runoff in this more developed river basin. Nitrate
concentrations in the Maine streams were comparable to Sweden (Calles 1983)
66
-------
cr>
Table 9. Mean concentrations of major ions in streams located in areas where bedrock is resistant
to weathering and precipitation is acidic (pH <4.5). Concentrations are inyeq/1.
Location
Maine, first order3
Maine, third order9
New Hampshire
New Hampshire0
New Hampshire
Sweden6
N orway
N orway^
Ca
66
107
100
120
83
100-400
50
67
Mg
37
37
25
29
31
15
40
Na
72
76
44
57
38
40-90
50-80
123
Ion
K H Al
10 3.0 18
12 0.6 13
15 1.6
15 0.4
6 12.6
7
7 33 71
so4
59
54
94
82
130
60-200
80-90
152
N03
3
5
37
40
31
-------
and Norway (Webb 1982), but much lower than in New Hampshire. Likens et^
al. (1977) report nitrate concentrations averaging about 30 ueq/1 in the
HUbbard Brook system, and Martin (1979) found that nitrate concentrations
averaged 37-40 ieq/1 in The Bowl natural area. Both these areas have
deciduous forest vegetation, whereas forests are primarily coniferous in
our study area.
The seasonal pattern of bicarbonate concentration is similar to that
of cations in all streams, for the same reason. Sulfate concentrations
were highest at the time of high discharge, when pH was lowest. Nitrate
concentrations were relatively constant, but there generally was a small
increase coinciding with snowmelt and proceeding peak discharge. This may
result because snow is relatively high in nitrate, and biological activity
is relatively low at this time. Galloway and Dillon (1983) found that
nitrate increased in lakes and streams following snowmelt, and Gallway et^
al. (1983) observed that sulfate was relatively constant but nitrate
Increased during spring snowmelt in three watersheds in New York. These
results coincide with our findings. Both sulfate and nitrate tended to be
lowest during summer base flow, when biological activity was highest, and
gradually increased during fall and winter, when biological activity
declined. Calles (1983) found that sulfate increased at peak runoff in one
stream in Sweden, nitrate increased in a second stream, and neither
increased in a third stream. The pH of these streams was not reported.
Webb (1982) reported a general increase in sulfate and decrease in nitrate
during the peak discharge period for the Tovdal River, Norway. At this
time, river pH declined from 5.0 to 4.6.
Ion Correlations
In our streams, pH was most highly correlated to discharge and to
alkalinity. There were significant correlations for all streams tested.
There were significant correlations with organic anions in three streams
(negative), with nitrate in one stream (negative), and with sulfate in one
stream (positive). The positive correlation with sulfate is probably
spurious. Thus the pH decline at peak discharge probably results from
dilution of base flow with low alkalinity runoff water, rather than from an
increase in sulfate or nitrate.
Ion Discharge
Ion discharge from a watershed is a function of the chemistry of
precipitation and the interaction of the chemicals in precipitation with
those in the terrestrial components of the watershed. Among the
interactions that may take place are the following:
uptake and release by vegetation
cation exchange reactions
weathering reactions
oxidation/reduction reactions, including those mediated by microbes
accumulation and depletion from watershed reservoirs
formation and dissociation of carbonic acid
dissolution of organic and other weak acids
Along with the above interactions, the chemical nature of the rocks, soil,
68
-------
and till in the watershed, the type of vegetation, and hydrological
characteristics that affect contact time between precipitation and
watershed components will ultimately control the chemistry of water
discharged from a watershed.
All watersheds located in glaciated areas for which ion discharge data
were available had a net loss of all cations except hydrogen (Table 10).
Net loss was generally highest for calcium, intermediate for magnesium and
sodium, and lowest for potassium. The White River had the highest net
output of cations, probably as the result of carbonate weathering reactions
(Johnson 1979). Wright and Johannessen (1980) reported that cation output
far exceeded acid input in non-granitic watersheds, probably because of
carbonation reactions. The net output of cations was lowest in the Rawson
Lake watershed, which is granitic and does not receive acidic precipitation
(Schindler et^ al_. 1976). Although Johnson et^ aK (1972) believed that the
cation discharge from Hubbard Brook was low as compared to regional or
world-wide averages, the net loss of cations for this watershed is higher
than that for acidified areas in Scandinavia.
The net output of cations was higher in higher order streams. Martin
(1979) found higher cation discharge at downstream as compared to upstream
locations. Both the Narraguagus and White rivers are third order streams
and cation concentrations are relatively high as compared to the other
streams in Table 10, most of which are first order streams. Johnson (1979)
found that ionic strength increased with stream order as strong acids were
neutralized, allowing carbonic acid to ionize and carbonation reactions to
occur. There was also an exchange of aluminum compounds for base cations
in higher order streams. Galloway et^ a_K (1983) found that depth of soil
and till were also important factors in determining discharge of base
cations from watersheds in New York. Generally higher order streams will
have larger watersheds, lower gradients, and thicker soils, all of which
contribute to increased contact of precipitation with soil particles, which
in turn promotes weathering reactions. An examination of Table 10 strongly
suggests that some factor or factors other than acid deposition alone are
responsible for the differences in cation discharge among the watersheds
listed. Rather minor differences in the chemistry of bedrock or soils, in
addition to differences in soil contact time, could appreciably affect the
chemistry of the precipitation as it passes through the system.
Some authors have attempted to quantitatively relate the deposition of
acid to the discharge of cations. Fisher et^ aj[. (1968) assumed that H ion
input approximated cation output. Their data supported this assumption,
but they did not consider precipitation inputs of other cations. Dillon gt
al. (1980) estimated the input of acid as the net retention of H ion and
ML ion in the watershed plus the loss of HCO- ion from the watershed, and
output of ions mobilized by acid as the sum of cations lost plus NO-
retained. In practice, NH. and NO., ion are roughly equivalent, canceling
each other, and ma^y be ignored. Wright and Henriksen (1983) calculated two
functions -- g(Ca + Mg ) and SA ~ and related these funjtions^to S04
resulting from atmospheric deposition. Tfce function g(Ca + Mg ) is
empirically derived and is 0.93 (Ca + Mg ) -14, where the asterisk
signifies correction for marine aerosols. This is an estimate of major
cations in the absence of acid deposition. The function SA is defined as
H + Al - HC03 and represents strong acid. Net S04 is computed by
69
-------
Table 10. Precipitation input, discharge output, and net retention (input - output) of ions for a
number of watersheds located in glaciated areas in North America and Europe. Units are
meq/m2/year.
Ca
Maine4
Vermont*
Norway6
Norway0
Swedend
New Hampshire6
New Hampsh1ref
New Hampshire9
Ontario11
Ontario1
In out
11 130
8 182
7 35
21 72
19 66
16 115
16 132
11 68
14 22
net In
-119 16
-174 5
-28 3
-51 29
-47 6
-99 6
-116 6
-57 5
-55
-8 7
Mt|
out
46
67
12
43
30
28
31
26
15
net
-22
-62
-9
-14
-24
-22
-25
-21
-34
-8
In
92
5
10
123
12
6
6
7
4
Na
out
88
86
16
133
23
44
57
32
12
net
4
-81
-6
-10
-11
-38
-51
-25
-7
-8
1n
3
0
3
8
3
6
6
2
2
K
out net
18 -15
8 -8
3 0
8 0
4 -1
15 -9
18 -12
5 -3
-3
3 -1
In
50
51
59
127
97
70
8
Ion
H
out
0.95
0.12
16
36
10
3
3
net
49
34
43
91
87
67
5
Al
In out net In
0 20 -20 0
07-70
0 16 -16 0
0 77 -77 0
0
0
08 -38 -0 13
HCO,
out net
87 -87
162 -162
0 0
0 0
29 -29
69 -69
-13 80
-32
In
66
50
63
164
49
112
112
112
6
SO,
out
81
106
50
164
29
101
90
-32
7
net
-15
-56
13
0
20
11
22
32
-1
in
23
32
25
84
3
43
43
28
51
NO.
out '
10
35
1
8
0.3
47
47
4
6
)
net
13
-3
24
76
3
-4
-4
20
32
45
Cl
In out net
108 61 47
6 99 -93
11 11 0
133 133 0
770
14 6
6 1 5
"This study. Langtjern watershed (Wright 1983). cB1rkenes, South Norway (Wright and Johannessen 1980). Tentral Sweden, average for three
watersheds (Calles 1983). eThe Bowl, headwater site (Martin, 1979). TThe Bowl, downstream site (Martin 1979). ^ubbard Brook (Likens et a].. 1977).
Muskoka-Hal1burton area, Harp Lake (Dillon et al... 1980). Rawson Lk., Ontario, average for three streams (Schlndler et al_. 1976).
-------
subtracting*estima.ted natural, or ^background," SO. from measured SO. .
Then: 9(Ca + Mg ) + SA = net S04 . * H
Comparison of these various methods for watersheds that have data
available (Table 11) indicates that the discharge of cations far exceeds H
ion deposition for all watersheds except Langtjern, Norway. The question
arising, then, is how are cations mobilized from a watershed if not by H
ion in precipitation. The apparent explanation is that there is
considerable internal H ion generation from ionization of carbonic acid,
which could be appreciable where mineral acid inputs are neutralized by ion
exchange reactions in the watershed (Johnson 1979; Wright and Johannessen
1980). Although wet deposition measurements probably underestimate H ion
deposition by a factor of one third, even making this correction does not
account for the discrepancy in our data.
The net retention of H ion plus HCO^ lost generally provides a better
approximation of the sum of cations lost from the watersheds. This
relationship presumes that the output of HCO, results from acid
neutralization reactions in the watershed, including internally generated
acids. The neutralization process plus other weathering reactions that
consume H ion results in the release of cations, including both aluminum
and base cations.
The function g(Ca + Mg ) + SA of Wright and Henriksen (1983)
represents H ion that passes through the system unneutralized plus that
which is neutralized and results in the release of Al and HCO^. Internally
generated H ion is assumed to be responsible for the estimated normal (or
"background") sum of major cations in watershed discharge, as well as part
of the HCO-, ion. These two quantities should approximate SO^ correction
for normal ("background") SO, and that resulting from marine aerosols. The
agreement is fair. In a previous study we found that this relationship
also generally held true for lakes in New England (Haines and Akielaszek
1983). The strength of this relationship is that it allows calculation of
surface water pH if acid deposition should change (Wright and Henriksen
1983). Watt et_ aj_. (1983) compared recent and historical water chemistry
for rivers in Nova Scotia. They concluded that increased acid deposition
had resulted in increased sulfate, aluminum, and H ion and decreased HCO,
in these ri vers.
Thompson (1982) proposed that the sum of non-marine base cations --
CDR -- would reflect leaching of cations by acid deposition. Among
watersheds for which such data were located (Table 12) there seems to be
little relationship between acid deposition and CDR. The chemistry of
bedrock and soil, watershed characteristics such as size, depth of soil and
till, etc., and the deposition of cations are more likely explanations of
differences in CDR.
It is nearly universal that watersheds have a net loss of bicarbonate,
providing only that the pH of the drainage water is sufficiently high for
bicarbonate ion to exist (Table 10). There is essentially no bicarbonate
ion in precipitation. The source of bicarbonate in these noncalcareous
systems is apparently dissociation of carbonic acid. The largest
bicarbonate loss was from the White River, which was the largest river and
71
-------
Table 11. Comparison of various parameters assumed to reflect acid
deposition or cation discharge. All units are meq/m /year.
Location
Maineb
Vermont
Norway0
Norway
New Hampshire6
Ontari o
Ontario9
cati ons
lost
21
339
59
152
144
99
25a
H ion
input
50
51
59
127
97
70
8
H ion retained
+ HCQ 1 ost
136
213
43
91
100
99
-
g(Ca* + Mg*)
+ SA
71
40
60
176
105
-
-
net S0*4
25
46
34
136
61
-
-
aNot including Al. bThis study. cLangtjern (Wright 1983). dBerkenesf
(Wright and Johannessen 1980). eHubbard Brook (Likens et Jl. 1977). Harp
Lake (Dillcn^t^L 1980). 9Rawson Lake (Schindler ^t a\_. 1976).
72
-------
Table 12. Cation Denudation Rate, and H ion deposition,
meq/m /year, for various watersheds.
Location
Narraguagus R.c
White R.c
New Hampshire (The Bowl, headwater) d
New Hampshire (The Bowl, downstream)d
New Hampshire (Hubbard Brook)6
North Carolina (hardwoods )f
New England (upper drainage basins)9
Northeastern U.S. 9
Oregon (S. Cascade Glacier)h
Ontario (mean of 3 streams)1
Newfoundland (mean of 10 streams)-}
Nova Scotia (mean of 11 streams)-3
Norway (Langtjern)1
Norway (Birkenes)"1
Sweden (mean of 3 streams)"
Great Britain0
World average"
CDR
215
343
202
238
115
116
220
680
930
51
124
106
53
125
116
78
390
H ion
50a
5ia
158
158
97
_b
b
b
b
10
20
40
59
127
b
10
b
aWet deposition only. bNot measured. cThis study. dMartin
jf!979). 6Likens et al. (1977). fJohnson and Swank (1973).
"Johnson et al_. (T972T- "Reynolds and Johnson (1972).
iSchindler et al. (1976). ^Thompson (1982). ^Thompson et al_.
(1980). IwTTght (1983). Bright and Johannessen (1980).
"Calles (1983). °Cryer (1976).
73
-------
had the highest alkalinity concentration. This river also probably has
carbonate minerals in the watershed. Johnson et^ aK (1972) found that
alkalinity increased as stream size increased, and Galloway £L il- (1983)
found that the largest loss of bicarbonate was from the watershed where
alkalinity was highest.
Nitrate is generally strongly retained by watersheds. The only
exception noted in the literature was one stream in New Hampshire (Martin
1979). This loss was small and may represent a net balance in a mature,
undisturbed watershed. In our data the White River had a large net loss of
nitrate, possibly as the result of agricultural and urban runoff.
Mechanisms of nitrate retention include uptake by vegetation, accumulation
in soil organic matter, loss of volatile nitrogen compounds such as nitric
oxide, or dissimilatory reduction such as denitrification or ammonification
(Calles 1983; Galloway and Dillon 1983).
Sulfate discharge was quite variable among rivers ranging from net
loss to balance to net retention. A net loss of sulfate may indicate a
source of sulfate in the watershed other than precipitation (Galloway et^
al. 1983), or an underestimation of sulfate input because of failure to
account for-dry deposition or gaseous sulfur dioxide (Dillon et al. 1982).
The data from Sweden (Calles 1983), New Hampshire (Martin 197UJ, and
Ontario (Schindler et_ al_. 1976) are bulk deposition, which underestimates
sulfate deposition. Both the Narraguagus and White rivers had net losses
of sulfate, even though deposition estimates were adjusted to include dry
deposition. A net retention of sulfate could result from accumulation of
sulfur in soil organic matter, release of volatile sulfur compounds such as
methyl sulfide, or sulfate reduction to form sulfide minerals (Calles 1983;
Wright 1983). A balance of sulfate input and output does not necessarily
mean that sulfate does not enter into any significant reaction pathways.
In fact, sulfate may function as a "mobile anion" (Christophersen et al.
1982) resulting in net loss of base cations.
Chloride is generally conserved and is geochemically unimportant. It
should therefore be in balance for input and discharge. In some cases this
is assumed, and any discrepancy is assumed to result from measurement
errors and ion deposition is adjusted to result in balance (Calles 1983;
Wright 1983). Streams in New Hampshire (Likens et^ al_. 1977) and Ontario
(Schindler _e_t a_K 1976) have a net retention of chloride. In our data the
Narraguagus had a net retention and the White had a net loss. Road deicing
salt may contribute to the net loss for the White River. Chloride
deposition measurements are much higher for the Narraguagus River because
of the proximity to the ocean. The precipitation station was much closer
to the ocean than was the water chemistry station.
Intragravel Water
Intragravel water was similar to, but slightly more alkaline than,
stream water. Inasmuch as both stream and intragravel water exhibited
similar temporal chemistry patterns, the exchange between the two types
must be relatively rapid. The slightly higher pH, alkalinity, calcium, and
specific conductance in intragravel water may result from very fine
particles of substrate that exert a minor neutralizing effect. In New
Brunswick and Nova Scotia streams intragravel pH was slightly higher than
74
-------
stream water for streams with pH <5.5, but slightly lower for streams with
pH >5.5 (6. Lacroix, Fisheries and Oceans, St. Andrews, New Brunswick,
personal communication). Williams and Hynes (1974) found that pH declined
from 7.8-8.2 at the water-substrate interface to 7.4-7.6 at 20 cm depth in
the substrate in the Speed River, Ontario. Water chemistry within
gravel-filled hatching boxes placed in two lakes was measured by Gunn and
Keller (1980). They found slightly higher pH, alkalinity, calcium, and
specific conductance in intragravel water from mixed noncalcareous gravel
placed in acidic (pH 5.2) Lake George. However, there was no difference
between ambient lake and intragravel water from a circumneutral lake (pH
6.7).
Intragravel water from our streams was extremely high in aluminum.
These high concentrations may have resulted from clay particles washed from
the sediment. However, aluminum was highest in the intragravel water with
the lowest pH, and intragravel aluminum concentrations followed temporal
patterns similar to stream water aluminum. If this difference is real,
elevated aluminum could constitute a threat to salmonid reproduction in
these streams. Because of the small number of samples and the lack of
filtering, these results should be interpreted cautiously.
Comparisons with Previous Data
Except for aluminum, there was little or no difference between water
chemistry factors measured in 1969 and those in our study. This is not too
surprising considering the time interval between measurements was only 12
years. Precipitation chemistry has probably changed little during this
time. We expected that continued acid deposition would increase leaching
of base cations or decrease alkalinity, but neither seems to have occurred.
In contrast to this, Thompson et_ _al_. (1980) found a significant decline in
pH and calcium in three Nova Scotia rivers between 1954-55 and 1973, and
substantial pH declines from 1965 to 1973, but no such declines in three
Newfoundland rivers. The Nova Scotia rivers?had mean annual pHs ranging
from 4.4 to 6.2, and CDRs of 80 to 115 meq/m /year. The pHs were 4.8 to
6.0 and CDRs were 150-200 meq/m /year for the Newfoundland rivers.
However, Watt et^ al_. (1983) found no change in calcium, magnesium, sodium,
or potassium between 1954-55 and 1980-81 in four Nova Scotia rivers. They
did find a significant decrease in bicarbonate and increase in hydrogen
ion, aluminum, and sulfate. We previously found that lakes in Maine
located near the rivers studied here had declined in pH and alkalinity
(Haines and Akielaszek 1983).
We did find an increase in aluminum concentration as compared to the
historical values, even though hydrogen ion concentration of the rivers was
not different. It is possible that the increase represents an improvement
in methodology. Aluminum is an analytically difficult element, and
quantification methods have improved greatly in recent years.
Historical comparisons in streams are subject to error because of
differences in discharge, vegetation, and climatic conditions. These
factors also affect lakes, but to a lesser extent than in streams. We were
fortunate to have relatively similar discharge levels in our data sets, and
to locate historical data that were collected over an annual cycle. A much
75
-------
longer series of data would be required to accurately assess historical
chemical changes in these rivers.
Potential Effects on Atlantic Salmon
Reduction or elimination of native Atlantic salmon populations has
been reported for acidic rivers in southern Norway and Nova Scotia. In
Norway, Atlantic salmon have disappeared from seven rivers with a mean pH
of 5.12 (Leivestad et^ aJL 1976). Mortality of naturally produced presmolts
has been observed in rivers at pH 5.15-5.50 and labile aluminum
concentrations of 30-55 wj/1 (Hesthagen and Skogheim 1983). Labile
aluminum usually constitutes 60 to 98% of total aluminum in Norwegian
rivers (Skogheim et^ al_. 1983). In Nova Scotia, Atlantic salmon populations
have been severely reduced or eliminated from 10 rivers with annual mean pH
5.0 or less (Watt et^ al_. 1983). Rivers with mean pH above 5.0 had no
declines in fish populations.
The difference in the pH at which Atlantic salmon are affected in
Norwegian versus Nova Scotian rivers is most likely the result of different
amounts of color (= dissolved organic matter) in the rivers of these two
regions. The increased dissolved organic matter chelates proportionally
more of the aluminum, rendering it non-toxic to fish (Driscoll et al.
1980). Color is very low in the Norwegian rivers (<5 color units;
Hesthagen and Skogheim 1983), and ranges from 30 to >100 color units in
Nova Scotia rivers (Watt et^ al_. 1983).
The pH and aluminum concentrations in some of the first and second
order streams in Maine (Table 6) are similar to those of Norwegian rivers
where Atlantic salmon mortalities have recently been reported. However,
inasmuch as the color levels of the Maine rivers are similar to those of
Nova Scotia rivers, such severe mortalities may not occur in the Maine
rivers at the present pH and aluminum conditions. Only total aluminum was
measured in Nova Scotia and Maine rivers, but it is probable that only half
the aluminum or less is present in the labile, toxic form. The conditions
of the most acidic Maine rivers appear to be marginally toxic to sensitive
life stages of Atlantic salmon. Although marked population declines may
not yet occur, low levels of mortality may result and prevent the full
utilization of available spawning and nursery habitat.
Surveys indicate that tributaries contribute about 34% of the total
spawning habitat in the Machias River, about 19% in the Narraguagus River,
and about 30-40% in the East Machias River (Bryant 1952; E. Baum and K.
Beland, Atlantic Sea Run Salmon Commission, personal communication).
Therefore tributaries constitute a significant portion of available
Atlantic salmon habitat in Maine.
76
-------
Conclusions
A survey of water chemistry was conducted in nine Atlantic salmon
rivers in New England. Eight streams were located in Maine, ranged in size
from first to third order, and all contained native populations of Atlantic
salmon. One river was located in Vermont, was third order, and was being
stocked with Atlantic salmon. All streams exhibited a seasonal pattern of
change in chemical composition. At periods of high discharge, which were
associated with spring snowmelt and increased precipitation in spring and
fall, pH declined (hydrogen ion increased), base cations and alkalinity
decreased, and aluminum increased. Sulfate tended to increase with
discharge, especially during the spring high discharge period, and nitrate
generally reached a peak slightly before peak discharge. The magnitude of
the seasonal change was largest in first order streams in Maine, and
smallest in the third order stream in Vermont. The low pH and high
aluminum concentrations reached are not as severe as those in Norway and
Nova Scotia, where Atlantic salmon populations have declined as a result of
acidification.
The chemistry of these streams reflects the interaction of
precipitation chemistry, watershed hydrology, and chemistry of soils, till
and bedrock in the watersheds. First order streams with small watersheds
composed of geologic materials resistant to weathering reacted the most to
atmospheric inputs of acid, but the effects of acidification, are not yet
severe. Atmospheric deposition of acid was not sufficient to account for
all ions leached from these watersheds. The output of base cations and
aluminum, balanced by bicarbonate and sulfate, far exceeds the amount of
hydrogen ion deposited. The excess is most likely produced by internal
generation of hydrogen ion from dissociation of carbonic acid.
The present chemical conditions in the rivers surveyed are not yet
critical for Atlantic salmon survival. However, continued or increased
deposition of acid may further degrade conditions in the small tributary
streams, which constitute 20-40% of the available Atlantic salmon habitat
in these rivers.
77
-------
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substratum of a stream. Freshwat. Biol. 4: 233-256.
81
-------
Wright, R. 1983. Input-output budgets at Langtjern, a small acidified
lake in southern Norway. Hydrobiologia 101:1-12.
Wright, R., and 6. Gjessing. 1976. Acid precipitation: changes in the
chemical composition of lakes. Ambio 5: 219-223.
Wright, R., and A. Henriksen. 1980. Regional survey of lakes and streams
in southwestern Scotland, April 1979. Report IR 72/80, Acid
Precipitation - Effects on Forest and Fish Project, Aas, Norway.
Wright, R., and A. Henriksen. 1983. Restoration of Norwegian lakes by
reduction in sulfur deposition. Nature 305: 422-424.
Wright, R., and M. Johannessen. 1980. Input-output budgets of major ions
at gauged catchments in Norway. Pages 250-251 in D. Drablos and
A. Tollan, editors. Ecological Impact of Acid Precipitation. Acid
Precipitation - Effects on Forest and Fish Project, Aas, Norway.
82
-------
Appendix A
Water chemistry data collected from nine rivers in Maine and Vermont.
83
-------
Appendix A.
DATE PH
N»RR»GU»GUS RIVER
PH »LK 11.PI ALK tl.PI AlK 1F.E.P1 »LK IF.E.P) CONO
(UEO/L) (UEO/L) CUEQ/ll IUEO/LI US/CM
CONO COLOR COLOR CALCIUM SODIUM POTASSIUM MAGNESIUM
US/CM UNITS UNITS (UEO/L) IUEO/LI (UEO/L) IUEO/L)
co
12480 6.45 .
22780 6.55 6.55
32880 6.15 .
40480 6.45 .
41180 6.05 .
41880 6.25 .
42580 6.15 .
50280 6.30 .
50980 6.50 .
5168C 6.50 .
5238C 6.70 .
53080 6.75 .
60680 7.00 .
61280 7.10 .
62780 7.05 .
71180 7.20 .
81180 7.10 .
90480 7.05 .
91980 6.85 .
100280 6.50 .
101680 6.35 .
102480 6.70 .
103080 6.45 .
110680 6.55 .
111380 6.50 .
120480 5.95 .
121880 6.30 .
10981 6.15 .
11481 6.30 .
20381 6.40 .
21781 6.00 .
22681 6.35 .
31981 6.55 .
32581 6.65 .
40781 5.95 .
41681 6.20 .
42281 6.25 .
43081 6.05 .
50781 6.75 .
52181 6.15 .
60481 6.85 .
72281 6.20 .
80581 6.85 6.80
81881 5.75 5.70
82781 6.75 6. 85
90181 6.85 .
91081 6.75 6.80
92881 6.30 .
100781 6.30 6.40
101981 6.45 6.55
102981 6.05 6. 12
111081 6.30 6.36
111981 6.35 6.35
156
216
71
76
41
51
51
63
78
88
104
135
128
117
136
172
152
172
118
100
76
123
71
89
79
35
101
120
132
136
59
66
97
94
52
63
71
78
113
81
109
78
144
42
112
128
143
65
72
89
52
73
65
216
190
245
96
100
72
83
75
83
102
113
124
161
167
146
163
201
246
155
49
111
146
74
109
54
SO
71
147
158
162
fl5
93
122
120
81
90
93
96
136
112
142
104
172
89
145
158
183
94
104
120
81
95
89
188
89
149
183
106
147
94
108
102
34
26
22
23
29
27
27
24
28
32
42
28
26
25
30
28
32
29
28
34
25
28
37
30
28
26
32
32
27
24
31
42
31
33
34
33
35
41
44
27
30 30
30 30
29 29
26 26
28 28
24
25 24
31
24 26
27 27
24 24
30
40
40
50
60
50
70
60
60
50
60
50
70
50
50
100
70
110
130
100
110
70
60
80
50
60
50
40
50
50
40
30
50
40
30
40
60
70
80
140
90
130
w
,
m
120
90
80
100
90
80
.
.
.
.
.
.
.
.
^
.
.
.
.
.
.
.
.
.
\
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
^
100
150
m
80
*
100
,
100
90
80
181
102
96
82
96
98
102
106
115
121
138
129
121
137
145
144
153
153
146
132
126
121
119
119
98
124
140
140
100
95
115
120
90
105
120
120
135
120
135
145
160
145
140
140
135
115
105
95
95
90
65
84
82
70
81
90
96
119
81
102
108
152
74
73
81
78
88
90
87
81
80
80
74
78
97
102
89
*
74
70
61
57
65
91
83
83
122
100
126
122
139
78
91
65
78
83
83
70
70
87
70
70
70
14
15
14
18
17
16
15
15
14
15
17
14
13
15
14
16
16
15
12
15
14
15
13
14
12
13
*
15
13
13
13
13
15
18
15
13
10
13
10
15
13
13
15
13
13
13
13
10
13
15
13
13
51
35
33
32
34
35
35
36
37
38
41
39
37
41
43
44
46
49
47
45
43
43
40
42
38
42
41
41
33
33
33
33
33
33
41
41
41
41
41
49
49
49
41
41
41
33
33
33
33
33
33
-------
Appendix A. Continued.
l?018t 6.55 6.59 98 IOC 122 132 2fl 28 60 60 120 74 10 41
121481 6.40 6.40 74 76 99 106 26 26 60 60 110 65 10 33
123081 6.65 6.55 99 103 126 130 29 30 40 40 120 70 10 33
11982 6.10 6.22 88 84 119 117 31 31 60 60 115 71 11 35
20482 6.10 6.18 102 106 130 137 30 29 50 50 120 67 11 37
22382 «.30 6.29 110 116 139 146 32 32 60 60 130 7T 13 38
30982 6.25 6.33 107 106 137 137 31 31 50 50 135 69 13 41
31682 6.05 6.10 69 70 95 100 27 26 50 50 115 64 13 38
32482 6.40 6.45 85 82 109 116 30 30 50 50 120 82 13 39
33082 6.35 6.29 63 6<5 95 96 24 24 50 50 110 58 13 35
40182 6.05 6.05 44 47 71 71 22 21 70 60 90 47 13 32
40582 5.90 5.94 33 32 59 63 20 20 50 50 80 44 13 27
41982 6.00 5.98 30 34 59 60 22 22 60 60 65 66 12 25
42682 6.35 6.34 55 57 81 86 22 20 50 50 78 53 11 28
50682 6.55 6.60 74 82 102 117 34 33 40 40 110 125 13 35
52082 6.85 6.75 111 11! 135 139 28 28 50 50 117 68 13 35
60382 6.75 6.72 118 119 145 14S 29 28 70 70 117 69 13 38
00
cn
-------
Appendix A. Continued.
CO
cr>
DATE
12480
22780
32880
40480
41180
41880
42580
50280
50980
51680
52180
53080
60680
61280
62780
71180
81180
90480
91980
100280
101680
102480
103080
110680
111380
120480
121880
10981
11481
20381
21781
22681
31981
32581
40781
41681
42281
43081
50781
52181
60481
72281
80581
81881
82781
90181
91081
92881
100781
101981
102981
111081
111981
IRON
(UG/l)
*
110
100
80
200
130
110
100
110
120
120
120
140
140
180
180
290
200
280
230
200
190
190
230
160
160
150
200
200
100
100
100
100
100
100
70
90
100
110
150
290
340
260
240
180
170
200
200
200
200
100
100
MANGANESE
IU6/LI
,
5
20
22
47
11
10
8
11
13
15
14
13
12
17
14
11
9
13
6
n
7
9
8
5
10
7
16
7
13
8
7
4
5
7
7
12
11
12
15
7
18
42
11
11
7
14
7
10
13
7
8
ALUMINUM
IUG/L)
78
235
111
263
20?
139
154
114
101
85
124
74
92
14-)
79
130
78
164
145
168
128
159
121
141
13!
101
133
61
101
12
83
59
111
83
56
70
60
92
78
213
98
199
106
70
75
130
109
134
122
120
CHLORIDE
(UEO/L I
NITRATE
(UEO/Lt
SULFATE
(UEO/LI
FLUORTOE
(UEO/Lt
72
56
49
50
55
58
56
59
-------
Appendix A. Continued.
120181 100 4 80 37.0 4.0 49.0 4.0
121481 100 3 80 43.0 6.0 63.0 3.0
123081 100 4 60 47.4 8.8 60.2 5.0
11982 120 5 57 45.0 8.0 59.0 3.0
20482 130 7 72 50.0 11.? 62.1 4.4
22382 130 6 74 55.0 10.5 55.0 3.7
30982 160 7 78 48.5 13.7 58.7 3.0
31682 150 10 114 44.2 15.3 65.9 2.3
32482 160 8 77 73.4 1?.9 57.6 2.7
33082 200 1
-------
Appendix A. Continued.
SINCLAIR BROCK
DATE PH PH ALK II.P) ALK (I.P) ALK (F.F.PI ALK (F.E.PI COND
(UEO/L) (UEO/LI (UEO/L) (UEO/L I US/CM
00
00
102981
111081
111981
I201RI
121481
123081
11982
21182
22382
30982
315B2
32382
33082
401 R2
40582
41982
42682
50682
52082
60382
5.25
5.65
?.45
5.75
5.70
5.90
5.75
5.85
6.00
5.80
5.55
5.80
5.65
5.10
?.25
5.35
5.45
5.85
ft. 15
5.45
5.46
5.72
5.45
5.84
5.68
5. 87
5.79
5.76
5.92
5.82
5.59
5.84
5.68
5.02
5.25
5.34
5.45
5. 81
6.12
5.45
7
22
14
20
14
20
21
16
31
23
13
19
16
-I
1
2
6
15
31
16
14
20
17
23
19
23
22
22
27
24
16
24
11
-3
7
5
10
17
34
17
34
44
38
46
41
51
48
51
61
48
41
46
44
31
31
31
37
44
54
45
COND COLOR COLOR CALCIUM SODIUM POTASSIUM MAGNESIUM
US/CM UNITS UNITS tUEO/L) IUEO/L) (UEO/L) IUFO/11
41
41
41
39
38
39
37
36
39
45
44
44
44
38
36
30
29
35
37
4?
52
51
45
55
45
50
51
51
54
55
45
54
44
26
33
32
36
45
61
49
26
26
24
28
24
24
28
26
25
26
26
24
24
24
23
21
20
22
22
2!
26
26
26
26
24
24
28
24
25
26
26
24
24
24
23
20
19
21
2?
24
70
60
60
40
30
30
30
20
30
30
30
30
40
50
30
40
40
40
40
too
70
60
60
40
30
30
30
20
30
30
30
30
40
60
30
40
40
40
40
100
55
50
55
60
55
55
55
55
55
60
60
60
60
55
50
41
38
44
4R
62
78
78
74
75
70
70
71
69
72
72
67
72
67
43
51
50
51
61
70
69
15
13
13
11
11
10
12
11
11
12
13
12
14
18
15
13
12
12
14
12
-------
Appendix A. Continued.
DATE
102981
111081
111981
120181
121481
123081
11982
21182
22382
30982
31582
32382
33082
40182
40582
41982
42682
50682
52082
60382
IRON
tUG/L)
100
100
too
90
80
80
90
80
80
70
60
40
60
160
30
40
60
4C
60
140
MANGANESE
(UG/L)
22
16
18
18
IS
13
9
8
6
14
18
10
16
42
22
21
13
13
13
18
ALUMINUM
(UG/LI
149
190
95
98
70
82
81
86
112
104
95
101
342
111
113
111
115
100
113
CHLORIDE
(UEO/L)
63.0
65.0
60.0
59.0
52.0
55.1
52.7
50.7
51.8
50.1
49.2
45.1
44.6
30.0
43.1
111.0
32.6
45.0
50.0
46.0
NITRATE
19.0
18.0
23.0
25.0
26.0
27.5
27.3
26.5
28.8
24.2
29.8
30.3
32.6
34.6
25.0
15.8
13.2
14.0
7.0
e.o
SUIFUTE FLUORIDE
(UEO/L) IUFO/L)
69.0 1.0
f7.0 1.0
73.0 2.0
69.9 2.5
72.0
68.0
69. 2
*5.3
65.
-------
Appendix A. Continued.
HACHIAS RIVER
DATE PH PH ALK (l.Pt ALK 26
I 26
9 32
23
> 24
22
> 22
.
23
24
24
.
.
.
.
.
.
*
w
m
,
.
.
*
.
.
.
.
.
.
»
*
.
.
.
.
27
26
25
22
24
*
22
23
24
22
60
60
70
70
70
60
80
70
60
50
50
50
70
50
50
70
40
100
90
70
70
70
60
90
60
80
70
70
70
BO
70
60
70
40
40
80
60
80
90
200
70
100
w
60
tto
100
120
100
90
.
.
.
.
«
m
*
.
^
«
^
.
-
"
.
^
m
,
m
m
.
.
.
80
170
70
»
90
120
100
90
116
85
86
74
84
(2
81
80
ti
87
91
90
88
93
53
92
102
112
103
98
92
95
90
92
80
95
90
95
CO
80
85
80
75
70
90
85
90
70
95
115
105
120
100
95
90
75
75
75
75
75
70
90
68
64
59
67
64
61
63
64
65
67
72
71
71
77
85
85
89
82
73
70
71
70
71
64
77
70
7+
65
65
65
65
61
57
70
74
74
87
78
83
87
70
74
74
74
70
70
74
70
70
70
13
12
11
15
12
12
12
12
12
12
13
15
14
13
13
14
16
15
13
13
13
13
12
12
10
11
*
13
13
13
10
10
10
13
10
10
10
13
10
10
10
13
13
13
13
13
10
10
10
10
10
10
-------
Appendix A. Continued.
120181 6.25 6.28 61 59 81 91 23 2* 90 90 90 65 10 33
121*81 6.10 6.12 42 46 68 75 22 23 80 80 85 65 10 33
123081 6.2! 6.22 45 51 77 83 24 24 80 80 85 70 8 33
11987 5.90 6.01 46 42 71 74 26 26 80 80 85 71 9 29
20482 5.85 5.88 48 52 78 86 24 24 70 70 85 67 9 29
21182 5.90 5.89 51 50 87 85 26 26 70 70 85 72 9 29
22382 6.10 6.08 60 61 95 97 26 26 80 80 90 70 9 30
30982 6.05 6.10 58 60 89 94 26 26 80 90 100 74 11 34
31682 5.95 6.02 50 54 75 84 26 26 80 70 95 72 12 32
32482 «.15 6.26 54 6C 79 91 24 24 70 70 95 70 10 32
33082 6.20 6.15 48 51 78 80 22 2? 80 80 90 68 11 31
40182 5.85 5.85 36 35 61 60 24 20 80 80 80 57 11 28
40582 5.70 5.71 19 21 48 50 22 21 60 60 75 57 II 26
41982 5.75 5.74 21 25 51 53 18 18 BO flO 57 52 9 22
42682 5.95 5.93 25 31 58 60 18 18 70 70 58 54 9 22
50682 6.30 6.11 32 41 70 68 19 19 60 60 63 54 8 23
52082 6.45 6.45 51 52 77 78 20 20 60 60 68 60 9 25
6C382 6.40 6.34 68 67 93 92 22 22 90 90 17 67 10 28
-------
<£>
Appendix A,
DATE
12480
22780
32880
40480
41180
41B80
42580
50280
50980
51680
52380
53080
60680
61? 80
62780
71180
81180
90480
91980
100280
101680
102480
103080
110680
111380
120480
121880
10981
11481
20381
21781
22681
31981
32581
40781
41681
42281
43081
50781
52181
60481
72281
80581
81881
82781
90181
91081
92881
100781
101981
102981
111081
111981
IROK
(UG/LI
.
120
120
120
250
140
140
130
120
90
120
100
120
110
130
110
160
120
280
17C
140
120
150
120
150
140
130
,
200
200
200
200
200
200
100
100
90
100
100
100
150
350
210
330
200
170
160
200
100
100
200
100
200
Continued.
H4NGANESE
(UG/l)
6
17
15
31
16
13
13
12
14
16
16
18
15
2C
14
14
14
59
16
17
12
17
11
12
22
1«
16
13
13
13
18
10
12
10
10
7
14
41
14
46
15
12
10
17
11
14
13
9
13
«IUPINUN
(UG/U
162
272
148
344
2«!S
146
245
1«9
146
127
16t
121
124
103
76
85
47
200
141
164
130
159
117
187
150
148
II
109
1««
128
147
101
129
113
86
102
96
175
103
268
103
?72
88
66
66
154
111
10;
148
122
148
CHLORIDE
(UEQ/L)
NITR»TF
(UEC/LI
SULF*TE
(UFC/L)
FLUORIDE
(UEO/ll
47
49
44
«4
52
52
-------
Appendix A. Continued.
120181 200 7 124 38.0 6.0 53.0 4.0
121481 200 10 139 38.0 2.0 53.0 4.0
123081 200 7 114 39.0 3.0 51.0 4.0
11982 140 8 120 43.4 2.3 53.8 3.8
20482 160 10 131 49.2 3.9 54.1 4.2
21182 160 10 125 43.9 3.8 53.5 4.0
22382 150 8 102 51.2 4.0 52.5 4.0
30982 230 9 124 24.2 2.4 31.9 3.3
31682 200 12 117 49.2 5.6 58.1 3.3
32482 210 10 115 46.9 5.6 54.4 3.3
33082 220 II 116 41.8 4.5 52.9 3.7
40182 260 23 147 59.0 5.5 55.0 1.0
40582 190 9 106 44.3 3.2 51.2 3.0
41982 130 14 118 34.5 3.2 46.9 2.7
42682 120 13 98 31.5 2.6 47.8 3.0
50682 140 9 110 33.0 11.0 48.0 3.0
52082 110 9 SI 37.0 0.8 43.0 3.0
60382 190 14 110 42.0 C.8 39.0 4.0
IO
OO
-------
Appendix A. Continued.
KF.RWIN BROOK
DATE PH PH ALK ([.PI AlK (I.P» ALK (F.E.PI ALK tF.E.P) COND
(UEQ/L) 1UEO/L) tUEO/U (UFC/L) US/CP
22780
32880
40480
41180
4188C
42980
502BO
50480
91680
52380
53080
60680
61280
62780
71180
81180
9C48C
91980
10 100280
-P» 101680
102480
103080
11C680
111380
120480
12188C
20381
21781
2268t
32581
40781
41681
42281
43081
50781
52181
60481
72281
8C581
81881
827B1
9C181
91081
92881
IOCT81
101981
1029ft!
111081
111981
170181
121481
123081
1198?
6.15 .
5.45 .
5,65 .
5.05 .
5.25 .
5.35 .
5.00 .
5.10 .
5.50 .
5.80 .
5.80 .
5.85 .
6.05 .
6.20 .
6.20 .
6.15 .
6.30 .
5.35 .
5.75 .
5.35 .
5.75 .
5.25 .
5.55 .
5.20 .
4.85 .
5.60 .
6.00 .
5.15 .
5.35 .
5.95 .
5.15 .
5.20 .
5.55 .
5.25 .
5.65 .
5.15 .
5.30 .
4.95 .
5.60 5.60
4.70 4.65
5.50 5.50
5.65 .
5.65 5.65
4.90 .
5.05 5.10
5.15 5.33
4.90 5.04
5.05 5.18
5.00 5.06
5.45 5.52
*.30 5.28
5.65 5.68
5.55 5.5H
99
11
20
-3
5
8
2
5
19
33
36
27
35
66
83
94
123
15
52
26
33
14
26
5
-7
30
53
8
15
41
11
-2
7
11
34
7
19
9
55
-24
34
49
42
-8
11
12
-4
1
3
16
12
18
22
8
2
5
*
t
6
*
I
6
1
9
7
5
1
128
42
50
29
33
36
33
33
46
60
61
70
67
94
111
78
32
44
74
35
27
25
33
56
40
50
35
95
20
63
79
84
25
40
46
25
31
31
41
38
51
46
99
22
64
79
36
79
48
43
39
54
38
57
52
CONO COLOR COLOR CALCIUM SODIUM POTASSIUM MAGNESIUK
US/CK UNITS UNITS (UFC/L 1 (UEO/l I (UFO/L) (UFO/l)
39
23
21
25
26
26
25
76
25
26
76
27
26
29
31
35
35
53
41
41
36
39
33
38
33
27
25
25
25
16
25
25
25
25
25
49
33
49
33
49
33
25
25
33
25
33
33
33
25
23
21
20
20
26
20
18
21
20
20
20
20
20
28
24
26
22
24
29
26
26
32
28
32
26
26
31
25
21
23
24
20
23
26
24
20
24
21
27
28
28
25
33
24
2?
22
24
23
28
26
24
23
22
22
22
23
*
m
*
*
*
,
m
m
m
»
m
25
36
24
20
20
.
21
30
24
23
22
22
22
23
30
60
60
80
70
80
100
100
80
70
60
90
90
70
80
90
60
140
100
120
100
too
80
110
70
60
70
70
60
70
BO
70
90
90
100
100
?80
140
270
.
.
140
160
120
140
150
130
120
no
70
70
7C
*
.
m
.
*
m
m
*
,
150
700
140
110
150
no
120
BO
70
70
70
115
54
51
59
59
61
60
59
57
61
65
69
67
74
81
90
91
134
102
95
84
88
76
86
71
<1
65
60
50
55
55
50
60
70
65
130
70
125
90
120
75
70
BO
65
60
70
70
«C
60
55
50
50
50
93
66
65
50
67
65
66
64
69
74
79
66
82
88
90
96
97
102
97
92
F6
78
80
82
67
81
74
65
65
70
52
61
78
78
83
91
91
96
100
83
96
100
100
74
78
87
78
78
78
76
67
77
74
15
12
14
16
15
15
15
13
13
13
16
20
15
18
15
16
18
12
IB
17
12
11
11
11
8
10
13
13
10
10
10
10
10
8
10
10
10
8
10
ft
10
10
10
10
13
15
13
10
10
8
8
8
9
-------
Appendix A. Continued.
21182 5.60 5.56 23 22 57 55 20 20 60 60 50 75 10 21
3088? 5.75 5.79 39 38 63 70 23 23 70 70 65 74 u 27
3158? 5.45 5.56 17 24 44 57 23 24 80 70 <5 73 u 28
32382 5.70 5.74 31 37 58 68 23 23 70 70 60 74 H 26
40182 5.25 5.19 9 11 41 40 22 22 ICC 100 65 56 13 29
40582 4.90 4.98 -5 -3 20 26 22 2? 90 90 55 51 10 24
41982 5.10 5.09-1 1 28 31 18 18 90 90 39 52 9 jq
4268? 5.20 5.10 1 -1 37 29 18 18 80 RO 38 5? 8 18
5C682 5.30 5.28 2 5 34 37 18 19 f»0 BO 38 54 9 ig
52082 5.85 5.87 31 34 54 61 20 20 70 70 49 72 12 21
60382 5.20 5.25 13 19 42 50 23 23 14C 140 76 70 8 31
ID
in
-------
Appendix A. Continue
DATE
22780
32880
4048C
41180
41880
4258C
59280
50980
«168C
52380
53080
60680
61280
62780
71180
BUBO
90480
91980
100280
101680
102480
103080
vo 110680
<7) 11138C
120480
121880
2D381
21781
22681
12581
40781
416R1
422J1
43081
50781
52181
60481
72281
80581
81881
82781
90181
91081
92881
V00781
101981
102981
H1081
111981
120181
121481
123081
11982
IRON
(UG/LI
650
80
90
110
130
16C
.160
180
120
120
100
130
120
140
150
200
190
280
230
240
190
220
200
23C
200
130
100
100
too
100
100
100
5C
120
80
16C
130
340
320
320
200
160
200
200
200
200
200
20C
200
110
110
130
90
MANGANESE
-------
Appendix A. Continued.
21182 IOC 5 107 48.2 3.0 52.* 7.1
30882 90 5 1C4 45.4 2.4 53.1 7.7
31582 110 7 128 33.8 C.B 59.4 5.7
32382 110 3 116 42.0 7.9 73.9 2.0
40182 140 13 14
-------
Appendix A. Continued.
HOLMES BROOK
DATE PH PH ALK (t.P) ALK (I.PI ALK IF.F.P) ALK IF.E.Pt COND CONO COLOR COLOR CALCIUM SODIUM POTASSIUM MAGNESIU*
(UEQ/L) (UEO/L) (UEO/L) (UEQ/L) US/CC US/Cf UNITS UNITS (UFO/LI (UFO/LI (UEQ/ll (UFC/L)
102901
111081
111981
120181
171481
123081
21182
33082
40182
40982
42682
90682
92082
60382
5.15
5.50
5.25
5.95
5.80
6.09
5.90
5.70
5.25
5.05
5.75
6.02
6.45
5.35
5.34
5.65
5.35
5.96
5.80
6.07
5.83
5.71
5.20
5.05
5.70
e.is
6.44
5.43
8
21
12
33
26
45
42
30
8
4
19
39
69
29
15
26
22
42
27
51
38
28
f
-2
21
3S
70
35
41
56
46
64
51
75
73
56
38
27
56
68
92
62
61
70
55
76
59
81
75
58
31
28
48
66
98
69
28
26
25
24
22
24
22
21
20
22
18
24
21
24
28
26
25
24
22
24
21
21
20
22
18
23
21
24
150
140
140
80
70
70
50
60
60
50
70
100
60
190
150
140
140
no
70
70
50
60
60
50
70
90
60
190
85
70
80
65
55
60
60
60
50
50
42
50
63
96
78
83
83
80
74
74
75
68
*7
57
59
68
77
71
8
5
8
7
6
6
6
8
10
9
7
9
8
7
58
49
58
39
38
36
35
37
34
35
29
3?
37
57
UD
OO
-------
Appendix A. Continued.
DATE IROU MANGANESE ALUHINUH CHLORIDE NITRATE SULFATE FLUORIDE
IUG/L) »UG/tl eUG/U «UEC/LI (UEC/LI lUfO/LI (UEO/LI
102981 200 18 ?37 74.0 3.0 54.0 2.0
111081 300 11 190 73.0 0.0 «2.0 1.0
111981 300 1* 204 65.0 6.0 59.0 2.0
120181 180 7 I tit 68.0 2.0 56.0 2.0
121481 160 6 145 53.0 2.0 56.0 1.0
123081 150 4 111 53.8 5.0 52.4 2.5
21182 170 8 141 53.6 6.8 51.8
33082 180 9 141 47.7 5.3 5«.5
40182 240 2C 178 36.1 6.1 44.1
40582 140 20 140 65.5 1.6 50.0
3
.0
.0
.0
42682 120 6 132 38.2 0.0 45.7 .0
50682 190 4 176 48.0 0.8 39.0 .0
52082 190 7 l*f 51.0 C.8 38.0 2.0
60382 390 18 415 39.0 4.0 33.0 2.0
-------
Appendix A. Continued.
DATE
21781
22681
31981
32581
40781
41681
42281
43081
50781
52181
60481
72281
80581
81881
82781
90181
91081
92881
100781
101981
102981
111081
111981
120181
121481
123081
11982
20482
21182
22382
30982
31682
32482
33082
40182
40582
41982
42682
50682
57082
60382
PH PH
6.05 .
6.35 .
6.60 .
6.55 .
5.90 .
6.15 .
6.25 .
6.75 .
.65 .
.65 .
.65 .
.45 .
.65 6.55
.95 5.95
.65 6.65
6.65 .
6.70 6.75
5.95 .
6.40 6.30
6.15 .26
6.00 .20
ft. 40 .60
6.20 .17
6.50 .50
6.45 .48
6.65 .61
6.25 .28
6.10 .15
6.15 .15
6. 50 . 53
6.35 .40
6.25 .25
6.50 6.55
6.35 .36
5.75 .70
5.75 .16
5.80 .84
6.25 .18
6. !5 .65
6.80 .78
6.65 .65
ALK II. PI
tUEQ/lt
68
69
114
M4
32
74
93
74
86
96
115
36
130
56
100
120
120
56
78
57
49
86
57
101
88
119
101
88
99
130
109
82
88
86
32
32
24
43
86
126
119
OLD STREAM
ALK (I.PI ALK (F.E.Pt ALK (F.E.PI COND
(UEO/L) tUEO/L) (UEO/Lt US/CD
89
102
139
139
66
102
119
96
119
125
145
64
130 163
54 94
102 134
152
121 171
84
83 109
6! 83
66 85
89 117
55 88
96 124
97 115
122 149
101 132
89 119
98 128
134 159
111 136
81 107
88 112
85 107
31 57
32 57
27 51
47 71
88 112
127 150
124 145
CONO COLCR COLOR CALCIUM SODIUM POTASSIUM MAGNESIUM
US/CM UNITS UNITS (UEO/L) (UEO/LI IUEO/LI (UEO/ll
33
33
41
41
25
33
41
41
41
33
49
49
49
49
49
49
49
41
41
41
49
49
41
43
43
44
44
39
41
49
46
43
44
44
33
32
24
27
35
44
44
163
94
139
*
163
.
114
IOC
104
132
90
126
123
153
135
123
128
165
142
111
117
110
58
57
57
74
122
153
152
28
29
31
33
22
30
29
30
29
31
35
27
32
30
12
30
30
25
28
25
28
29
24
30
28
32
34
30
31
34
34
32
30
28
22
23
19
22
26
30
28
;
.
.
.
.
32
28
32
30
30
.
27
»
2t
29
24
30
28
32
34
30
32
34
33
32
30
28
22
23
19
21
25
30
28
60
60
50
40
70
60
50
80
80
80
100
200
120
140
.
.
100
160
110
100
110
100
uo
80
70
60
60
70
60
60
70
70
70
70
70
60
60
60
60
50
90
»
*
.
*
120
170
.
.
110
*
110
^
MO
100
MO
80
70
60
60
70
60
60
70
70
70
70
70
60
60
60
60
50
90
95
95
125
125
65
95
125
110
120
90
130
130
140
140
145
145
140
110
110
115
110
120
100
120
115
135
130
110
120
140
135
115
MS
115
75
75
105
65
98
129
MB
70
70
70
74
57
70
87
87
87
78
91
87
91
83
91
100
96
74
78
87
78
78
78
74
74
74
77
72
74
82
84
82
83
78
64
57
52
59
67
78
84
13
13
10
10
13
13
10
10
10
10
10
10
10
10
10
13
10
13
10
13
13
10
10
9
9
9
9
8
9
9
11
11
11
12
11
11
9
9
9
to
9
-------
Appendix A. Continued.
DATE
21781
22681
31981
32581
40781
41681
42281
43081
50781
52181
60481
72281
80581
81881
82781
90181
91081
92881
100781
101981
102981
111081
111981
120181
121481
123081
11982
20482
21182
22382
30982
31682
32482
33082
40182
40582
41982
42662
50682
52082
60362
IRON
tUG/L)
100
200
100
100
100
100
90
110
110
110
160
310
250
320
230
220
250
200
200
20C
200
200
200
120
120
110
120
120
120
100
190
190
200
190
190
200
90
70
90
110
180
MANGANESE
(UG/U
24
19
12
10
15
11
9
11
16
11
13
62
21
36
16
15
12
22
20
15
17
10
14
10
9
9
9
16
12
t
16
12
9
12
26
17
19
9
12
19
30
AIUPIMJM
IUG/LI
119
123
53
86
129
1C1
77
99
B6
100
97
53
127
271
149
105
167
141
137
m
106
157
121
1C1
85
75
94
97
85
132
124
103
89
147
104
106
102
85
67
138
CHLORIDE
(UEQ/L)
NITRATE
IUEO/U
SULFATE
FLUORIDE
IUEO/L)
49.0
62.0
61.0
57.0
56.0
51.0
55.0
61.5
61.5
54,3
89.2
69.6
74.6
69.6
53.2
58.8
54.5
43.1
46,0
51.0
59.0
59.0
1.0
1.0
1.0
2.0
1.0
2.0
4.0
5.0
6.3
4.5
6.1
6.8
7.3
6.5
4.5
3.2
2.4
1.6
C.8
0.8
C.8
0.8
52.0
57.0
57.0
59.0
59.0
59.0
61.0
60.2
62.1
58.7
60.6
61.2
65.0
60.6
55.9
50.6
54.3
45.7
51.0
51.0
49.0
45.0
5.0
2.0
2.0
2.0
2.0
2.0
2.0
1.9
2.4
.7
.3
.7
.7
.0
.3
.3
.3
.3
.0
.0
2.0
2.0
-------
Appendix A. Continued.
DATE
PH
PH
BOWLES BROOK
ALK (t.PI ALK (I.PI ALK (F.E.P) ALK (F.E.PI CONO
(UEQ/lt (UEQ/L) (UCQ/LI (UEO/LI US/CM
102981 4.9C 5.05
111081 5.15 5.29
111981 4.95 4.98
120181 5.95 5.89
121481 5.75 5.78
121681 5.60 5.71
123081 6.05 6.05
11982 5.95 6.01
21182 5.80 5.73
30882 5.90 5.87
31582 5.35 5.44
32382 5.85 5.86
40182 5. CO 4.96
40582 5.00 4.98
41982 5.05 5.06
42682 !.3S 5.32
50682 5.92 6.00
52082 6.55 6.55
60382 5.40 5.48
-2
7
-3
41
29
17
47
47
38
49
18
32
9
4
0
8
34
87
32
1
16
2
43
28
22
!C
4?
43
4f
20
35
-1
3
0
12
37
90
34
27
34
31
71
61
48
78
77
69
78
44
61
33
25
27
37
«6
112
57
CCNO COLOR COLOR CALCIUM SODIUM POTASSIUM MAGNESIUM
US/CM UNITS UNITS IUEQ/LI (UEQ/U (UEO/Lt (UEO/L)
41
41
33
44
39
41
44
39
48
42
42
32
30
23
26
34
90
48
49
49
35
76
64
58
82
81
73
77
53
69
27
28
28
37
71
123
66
30
28
27
26
24
24
26
28
26
27
25
26
23
24
20
18
22
26
26
30
28
26
26
24
24
26
28
25
27
27
25
23
24
20
18
22
26
26
140
130
140
80
80
70
70
70
70
70
7C
70
80
60
80
80
90
110
150
140
130
140
HO
80
70
70
70
70
70
70
70
80
60
80
80
90
110
150
75
70
CS
80
70
.
75
75
70
80
75
75
60
55
38
43
57
81
85
18
78
74
80
74
.
77
81
80
87
80
83
55
56
48
53
67
88
80
13
10
10
9
9
9
9
9
11
12
11
14
12
10
10
8
12
10
o
-------
Appendix A. Continued.
OATF
107981
111081
111981
120181
171481
121681
121081
11982
21182
30882
31582
32382
40182
40582
41982
42682
50682
52082
60382
IRON
CUG/L)
200
200
20C
140
110
.
110
100
120
150
160
16C
140
1100
100
100
100
13C
240
MANGANESE
(UG/L)
21
13
22
10
11
10
10
10
15
16
9
23
15
12
1C
9
9
2S
UUKINUN
(UG/LI
312
277
287
181
189
138
144
133
104
176
174
2oe
134
130
127
129
121
365
CHLORIDE
tUEO/U
77.0
54.8
59.0
54.0
53.2
54.0
57.7
54.3
62.7
58.1
56.1
40.4
51.8
35.3
33.7
47.0
54.0
54.0
NTTR4TE
IUEC/U
0.0
0,7
9.0
6.0
1.2
8.0
7.5
6.1
10.5
6.5
6.1
3.0
C.8
8.1
0.0
1.0
0.8
2.0
SUIF4TE
IUEC/U
65.0
«5. 5
65.0
65.0
64. 1
63.0
63.1
60.6
66.9
73.9
64.1
50.0
57.4
48.1
52.2
53.0
48.0
46.0
FLUORIDE
tUFfl/ll
2.0
2.0
2.0
1.9
?!o
2.5
2.0
2.0
1.7
1.7
1.3
1.7
1.3
1.0
2.0
3.0
2.0
o
co
-------
Appendix A. Continued.
HARMON BROOK
DATE PH
AlK II.P) «LK II.Fl ALK (F.E.PI «LK (F.E.P1 CONC
(UEQ/L) (UEO/LI (UEQ/ll (UEC/Lt US/C»
100781 6.10
102981 5.65
111081
111981
uciai
121481
123081
11982
30882
31582
32382
33082
40182
4C582
41962
.55
.75
.C5
.05
.25
.15
.10
.00
.25
.10
.55
.05
.84
.09
.83
.12
.08
.26
.19
.17
.02
.30
.12
.54
.60 5.64
.10 5.18
42682 6.00 6.00
5C682 6.25 6.26
52082 «.85 *. 75
60382 5.85 5.92
65
28
49
31
56
42
66
61
69
52
68
52
22
14
19
34
55
ill
53
59
36
5C
37
55
4f
69
69
12
53
69
4S
22
17
22
33
57
11!
98
9e
98
75
61
78
71
92
87
SB
78
92
78
;i
44
46
59
81
139
83
94
80
90
69
87
79
97
93
104
81
98
78
90
45
50
99
86
139
96
CONO COLOR COLOR CALCIUM SODIUM POTASSIUM MACNESIU*
US/CM UNITS UMTS (UEC/LJ fUEQ/ll (UEO/LI lUEC/ll
41
41
41
41
38
39
39
46
42
43
37
35
31
26
29
35
41
44
24
26
26
24
26
26
26
29
28
26
26
24
20
20
18
20
26
28
26
24
26
26
24
26
26
26
29
28
26
26
24
22
20
18
22
26
28
26
7C
40
TO
80
40
40
40
30
50
40
30
40
60
40
50
40
90
90
120
70
90
70
80
40
40
40
30
90
40
10
40
60
40
90
40
90
90
120
^
C9
79
80
(5
79
89
19
99
89
89
60
70
to
49
97
12
89
93
83
83
78
ei
77
79
79
78
74
77
«C
48
54
94
99
73
80
74
10
8
8
7
7
7
8
9
9
9
8
12
9
7
7
9
10
6
-------
Appendix A. Continued.
CATE IRON MANGANESE ALUKINUH CHLORIDE NITRATE SUIFATE FlUCRIOE
IUG/LI IUC/L) IUG/tl IUEO/L) (UEO/U (UEC/L) (UEG/LI
100781 . .
102981 200 7 197 63.0 3.0 70.0 2.0
111081 200 4 141 65.0 1.0 10.0 2.0
111981 IOC 5 176 50.0 0.0 72.0 2.0
120181 80 4 120 42.0 4.0 62.0 2.0
121481 90 4 107 49.0 3.0 73.0 2.0
123081 70 3 83 50.0 7.5 69.9 2.5
11982 70 3 81 51.0 7.0 71.0 2.0
30882 190 8 89 48.6 8.3 70.( .7
31582 140 £ 139 44.2 5.6 73.3 .3
32382 140 6 91 45.4 5.6 68.3 .3
33082 180 9 141 38.7 4.5- «9.2 .7
40182 21C 22 18C 33.3 2.4 58.0 .3
40582 110 7 SS 46.3 1.6 61.7 .3
41982 50 3 94 34.1 C.8 19.3 .7
42682 4C 2 92 31.5 C.O «3.0 .0
50682 90 7 ft 44.0 C.8 63.0 .0
52082 110 5 86 44.0 1.0 !9.0 2.0
60382 18C 13 268 34.0 0.8 45.C 2.0
O
cn
-------
Appendix A. Continued.
DATE
110581 '
111961
120181 1
120881 1
122381 1
123181 1
10882 '
11482 '
12182 1
12982
20582 -
21682 1
22682 <
31782 -
32282 <
40182
40982
41582
42382
50682
51482
52182
52782
PH
r. 16
r.25
r.2o
1.30
r.05
r.35
M5
r.oo
r.io
P. 05
r.05
r.05
i.70
r.io
..60
.80
.90
.10
.70
.35
.45
.60
.45
H ALK II. P)
IUEQ/L)
230
256
263
238
270
309
224
280
334
310
168
246
247
273
202
111
188
,
138
183
231
194
239
WHITE RIVERt VERMONT
ALK (I.P) ALK IF.F.PI ALK IF.E.P) CCNO
IUEQ/L) tUEO/L) IUEO/U US/CH
260
295
295
262
291
336
244
291
366
396
204
268
262
285
221
122
197
148
198
244
209
262
CCNO COLOR COLOR CALCIUM SODIUM POTASSIUM MAGNESIUM
US/CM UNITS UNITS IUEO/L) IUEO/LI IUEO/L) IUEO/L)
58
69
90
93
99
101
90
100
103
108
16
96
127
107
109
79
97
89
77
82
95
102
105
57
60
60
65
71
57
64
67
72
53
62
80
66
66
42
62
54
44
51
62
66
68
57
60
60
64
10
56
64
68
12
53
62
80
66
66
41
62
54
44
52
62
66
68
w
0
0
0
0
0
0
0
0
0
0
0
0
0
10
10
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
305
310
320
320
345
370
310
350
375
390
260
330
438
321
331
215
313
280
239
272
329
354
370
100
90
102
101
108
117
94
109
115
121
116
1 10
143
145
151
71
124
109
79
93
116
123
129
10
9
10
10
10
10
9
10
10
10
10
9
12
10
10
8
9
8
9
9
11
13
13
-------
Appendi
DATE
X A.
IROH
(UG/L)
110581
111981
120181
120881
1223S1
123181
10882
11482
12182
12982
20582
21682
22682
31782
32282
40182
40982
41582
42382
50682
51482
52182
52782
0
4C
30
60
20
20
30
20
10
0
70
50
60
90
270
390
0
20
150
0
20
20
20
Conclude'
MANGANESE
IUG/L»
10
3
5
9
3
3
2
2
3
0
8
3
6
15
33
59
13
15
20
14
12
5
4
ALUPINUH
IUG/LI
9
14
14
32
5
8
17
9
4
6
54
22
20
47
115
223
20
52
«3f
46
31
23
16
CHLORIDE
(UFO/LI
103.0
94.0
106.0
108.0
118.1
128.9
97.6
109.6
119.3
126.5
136.1
116.1
163.9
173.5
194.0
79.0
160.2
131.0
86.0
107.0
141.0
151.0
159.0
NITRATE
tUEO/L)
40.0
30.6
35.3
35.3
38.9
41.7
38.9
41.7
44.4
44.4
45.0
41.7
5C.O
44.2
44.4
45.0
55.6
39.0
47.0
42.0
36.0
31.0
28.0
SULFATE
IUFC/LI
143.0
134.7
136.7
138.8
140.7
140.7
134.7
142.7
140.7
140.7
120.4
134.7
148.8
132.7
134.7
118.0
132.7
126.0
118.0
122.0
128.0
130.0
132.0
FLUORIDE
CUEO/H
2.0
.3
.3
.3
.0
.3
.0
.1
.0
.1
.0
.0
2.0
2.0
2.0
1.0
-------
Appendix B
Salmon Redd Excavation
During November 1981 two naturally spawned Atlantic salmon redds were
located and mapped, one each in Old Stream and Bowles Brook. On April 26,
1982, each redd was excavated using a hooded shovel (Hatch 1957) and eggs
and fry were collected in a drift net (Jordan and Beland 1981) and
preserved for later examination. Excavation of the marked Atlantic salmon
redds was timed to occur after hatching of eggs but before emergence of
fry. There were no live, unhatched eggs among those recovered.
Stream
Bowles
Old Stream
Dead
Eggs
10
0
Dead
Fry
6
1
Live
Fry
131
46
Total
147
47
Percent
Mortality
11
2
The Bowles Brook redd had higher mortality of both eggs and fry than
did the Old Stream redd, although the total number of fish recovered was
also larger. The dead fry were partially encapsulated in the egg membrane.
Such failure to completely rupture the egg membrane has been reported
previously for Atlantic salmon embryos exposed to acid stress (Peterson et^
al. 1980). The number of fry emerging in Old Stream in 1980-81 ranged from
"9T to 109 for natural redds and 21 to 124 for artificial redds
(Gustafson-Marjanen 1982), thus the number we recovered is reasonable.
The use of naturally spawned Atlantic salmon redds precludes the
determination of total eggs deposited or total mortality. The drift net
used was large enough to ensure the collection of all eggs. Fry that were
already hatched could have migrated away from the egg pit through the
gravel and may have been missed. Eggs that died during development may
have disintegrated and would not be collected. The estimated total
survival for Atlantic salmon eggs from eyed stage to emergence from natural
redds in Old Stream during 1980-1981 was 5.8-6.4% (Gustafson-Marjanen
1982). In that study, excavation of natural redds following fry emergence
resulted in recovery of only one or two dead eggs. No dead fry were found.
We found no dead eggs and one dead fry in the Old Stream redd we excavated.
It is not possible to state conclusively that depressed pH and/or
elevated aluminum concentrations resulted in decreased Atlantic salmon
embryo and fry survival in Bowles Brook. Excavation of only one redd per
stream does not permit calculation of confidence limits or tests of
significance of mortality in the two streams. However the appearance of
the dead fry from Bowles Brook does suggest that acid stress caused the
mortality.
108
-------
50277-101
REPORT DOCUMENTATION » "EPORT NO. *.
PAGE FWS/OBS-80/40.18
Effects of Acidic Precipitation on Atlantic Salmon
Rivers in New England
7. Authord)
Haines, T.A. and J.J. Akielaszek
9. Performing Organization Nam* and Address
U.S. Fish and Wildlife Service, Columbia National
Fisheries Research Laboratory, Field Research Station,
Zoology Department, University of Maine, Orono, ME 04469
12. Sponsoring Organization Nama and Address
U.S. Department of the Interior, Fish and Wildlife Servic
Division of Biological Services, Eastern Energy and Land
Use Team, Route 3, Box 44, Kearney svi lie, WV 25430
3. Rsclplanf s Accession No.
S. Raport Data
October 1984
«.
8. Performing Organization Rapt No.
10. Prolact/Task/Work Unit No.
11. Contract(C) or GranUG) No.
(C)
(C)
13. Typa of Raport & Parlod Covered
Final
14.
15. Supplementary Notes
16. Abstract (Limit: 200 words)
A water chemistry survey was conducted in nine Atlantic salmon rivers
in New England. Eight rivers are in Maine and contain native Atlantic salmon popula-
tions. One river is in Vermont and is undergoing restoration of the Atlantic salmon
population. The rivers ranged in size from first order tributary streams to third
order main stem rivers. All contained actual or potential Atlantic salmon spawning
and nursery habitat. The chemistry of the Maine rivers was similar to that reported
for other rivers located in areas where bedrock is low in acid neutralizing capacity
and where precipitation is similarly acidic. The Vermont river had much higher con-
centrations of all ions except aluminum and hydrogen than the Maine rivers, especially
calcium, magnesium, and bicarbonate, indicating the presence of carbonate mineral in
the watershed of this river. The pH and aluminum concentrations in second and third
order streams were well within safe limits for Atlantic salmon, even during periods of
high discharge. First order streams, however, reached levels of pH and aluminum con-
centration that may be toxic to sensitive early life stages of Atlantic salmon, or
during smoltification, although conditions were not as severe as those reported for
Atlantic salmon streams in southern Norway or southwestern Nova Scotia, where Atlantic
salmon populations have declined or disappeared apparently as a result of acidification
17. Document Analysis a. Descriptors
acidification, pH, alkalinity, aluminum concentration, fisheries, water chemistry
b, Identifiers/Open-Ended Term*
Atlantic salmon, impacts, stress, metal contamination, water quality,
acid rain, acid deposition
c. COSATI Field/Group
IS. Availability Statement
unlimited
19. Security Class (This Report)
unclassified
20. Security Class (This Page)
.mrlaccifiPH
21. No. of Pages
xi + 108
22. Price
frUS. GOVERNMENT PRINTING OFFICE: 1984-781-447/9545
Dapartmant of Commerce
-------
Hawaiian Islands
"o
Headquarters. Division o( Biological
Services, Washington. DC
Eastern Energy and Land Use Team
Leetown, WV
National Coastal Ecosystems Team
Slidell. LA
Western Energy and Land Use Team
Ft Collins. CO
Locations of Regional Offices
REGION 1
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U.S. Fish and Wildlife Service
Lloyd Five Hundred Building, Suite 1692
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Regional Director
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One Gateway Center
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Regional Director
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P.O. Box 25486
Denver Federal Center
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REGION 7
Regional Director
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-------
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