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ACID
DEPOSITION
Long-Term
Trends
Committee on Monitoring and Assessment of
Trencis in Acid Deposition
Environmental Studies Board
Commission on Physical Sciences,
Mathematics, and Resources
National Research Council
NATIONAL ACADEMY PRESS
Washington, D.C. 1986
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NATIONAL ACADEMY PRESS 2101 Constitution Avenue, NW Washington, DC 20418
NOTICE: The project that is the subject of this report was approved by the Governing
Board of the National Research Council, whose members are drawn from the Councils of
the National Academy of Sciences, the National Academy of Engineering, and the
Institute of Medicine. The members of the committee responsible for the report were
chosen for their special competences and with regard for appropriate balance.
This report has been reviewed by a group other than the authors according to
procedures approved by a Report Review Committee consisting of members of the
National Academy of Sciences, the National Academy of Engineering, and the Institute
of Medicine.
The National Research Council was established by the National Academy of Sciences
in 1916 to associate the broad community of science and technology with the Academy's
purposes of furthering knowledge and of advising the federal government. The Council
operates in accordance with general policies determined by the Academy under the
authority of its congressional charter of 1863, which establishes the Academy as a
private, nonprofit, self-governing membership corporation. The Council has become the
principal operating agency of both the National Academy of Sciences and the National
Academy of Engineering in the conduct of their services to the government, the public,
and the scientific and engineering communities. It is administered jointly by both
Academies and the Institute of Medicine. The National Academy of Engineering and the
Institute of Medicine were established in 1964 and 1970, respectively, under the charter
of the National Academy of Sciences.
Although the information in this publication has been funded in part by the U.S.
Environmental Protection Agency under Assistance Agreement No. CR-811626-01-0 and
the U.S. Geological Survey under Grant No. 14-08-0001-G-954 to the National Academy
of Sciences, it may not necessarily reflect the views of these agencies, and no official
endorsement should be inferred.
Library of Congress Catalog Card Number 86-70311
International Standard Book Number 0-309-03647-X
Printed in the United States of America
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Committee on Monitoring and Assessment
of Trends in Acid Deposition
JAMES H. GIBSON, Colorado State University, Chairman
ANDERS W. ANDREN, University of Wisconsin
RAYMOND S. BRADLEY, University of Massachusetts
DONALD F. CHARLES, Indiana University
TERRY A. HAINES, University of Maine
RUDOLF B. HUSAR, Washington University
ARTHUR H. JOHNSON, University of Pennsylvania
JAMES R. KRAMER, McMaster University
SAMUEL B. MCLAUGHLIN, Oak Ridge National Laboratory
STEPHEN A. NORTON, University of Maine
GARY OEHLERT, University of Minnesota
GARY J. STENSLAND, Illinois State Water Survey
JOHN TRI]ONIS, Santa Fe Research Corporation
DOUGLAS M. WHELPDALE, Atmospheric Environment Service,
Canada
Staff
WILLIAM M. STIGLIANI, Staff Officer
JOYCE E. FOWLER, Administrative Secretary
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Environmental Studies Board
STANLEY I. AUERBACH, Oak Ridge National Laboratory, Chairman
WILLIAM E. COOPER, Michigan State University
J. CLARENCE DAVIES, The Conservation Foundation
JOHN W. FARRINGTON, Woods Hole Oceanographic Institution
BENJAMIN G. FERRIS, JR., Harvard School of Public Health
GEORGE M. HIDY, Desert Research Institute
WILLIAM G. HUNTER, University of Wisconsin
RAYMOND C. LOEHR, University of Texas
ROGER A. MINEAR, University of Illinois
PHILIP A. PALMER, E.I. DuPont de Nemours & Company
CLIFFORD RUSSELL, Vanderbilt University
WILLIAM H. RODGERS, University of Washington
Staff
MYRON F. UMAN, Staff Director
WILLIAM M. STIGLIANI, Staff Officer
RUTH S. DEFRIES, Staff Officer
JANET A. STOLL, Staff Assistant
JOYCE E. FOWLER, Administrative Secretary
CAROLYN STEWART, Administrative Secretary
lo
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Commission on Physical Sciences,
Mathematics, and Resources
HERBERT FRIEDMAN, National Research Council, Chairman
CLARENCE R. ALLEN, California Institute of Technology
THOMAS D. BARROW, Standard Oil Company, Ohio (retired)
ELKAN R. BLOUT, Harvard Medical School
BERNARD F. BURKE, Massachusetts Institute of Technology
GEORGE F. CARRIER, Harvard University
CHARLES L. DRAKE, Dartmouth College
MILDRED S. DRESSELHAUS, Massachusetts Institute of Technology
JOSEPH L. FISHER, Office of the Governor, Commonwealth of
Virginia
JAMES C. FLETCHER, University of Pittsburgh
WILLIAM A. FOWLER, California Institute of Technology
GERHART FRIEDLANDER, Brookhaven National Laboratory
EDWARD D. GOLDBERG, Scripps Institution of Oceanography
MARY L. GOOD, Signal Research Center
J. ROSS MACDONALD, University of North Carolina
THOMAS F. MALONE, Saint Joseph College
CHARLES J. MANKIN, Oklahoma Geological Survey
PERRY L. MCCARTY, Stanford University
WILLIAM D. PHILLIPS, Mallinckrodt, Inc.
ROBERT E. SIEVERS, University of Colorado
JOHN D. SPENGLER, Harvard School of Public Health
GEORGE W. WETHERILL, Carnegie Institution of Washington
IRVING WLADAWSKY-BERGER, IBM Corporation
Staff
RAPHAEL G. KASPER, Executive Director
LAWRENCE E. MCCRAY, Associate Executive Director
v
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Preface
Recognizing that deposition of chemical pollutants from the
atmosphere constitutes one of the more significant environmental
issues of our time, both nationally and internationally, the National
Research Council has undertaken a series of studies designed to
summarize what is known about this complex phenomenon and to
correct many of the misunderstandings surrounding it. A central
objective of this activity has been to delineate more clearly the role of
our industrial society in contributing to the chemical composition of
the atmosphere as well as the consequences for the environment of the
ultimate return of the pollutants to the Earth's surface.
The first report in the series Atmosphere-Biosphere Interactions:
Toward a Better Understanding of the Consequences of Fossil Fuel Combustion
(1981) provides a comprehensive synthesis of our knowledge of the
aquatic and terrestrial effects of the deposition of substances derived
from fossil fuel combustion. The second report—Acid Deposition:
Atmospheric Processes in Eastern North America (1983) addressed the
relationships between average rates of emission of sulfur oxides and
deposition of acid sulfate. The third report—Acid Deposition: Processes of
Lake Acidification (1984)—reviewed alternative hypotheses regarding
geochemical processes in watersheds responding to acid inputs from
the atmosphere. Another report—Acid Deposition: Effects on Geochemical
Cycling and Biological Availability of Trace Elements (1985) was prepared
jointly with the Royal Society of Canada (RSC) and the Mexican
Academy of Scientific Research (AIC). It examined the influences of
atmospheric deposition on biogeochemical processes involving trace
elements.
The current report addresses another dimension of the relationships
among emissions, deposition, and environmental effects. If industrial
activity is implicated in atmospheric deposition, then the phenomenon
is a relatively recent one and should be related to changes in the levels
and kinds of such activity. It is logical, then, to seek historical data or
. .
All
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other reliable information that may be available to assess whether
emissions, deposition, and effects are temporally linked over the
period since the beginning of industrialization (or over a portion of the
period), thus suggesting possible cause-effect relationships. The
original suggestion for the study came from the Tri-Academy
Committee on Acid Deposition, a joint activity of the NAS, RSC, and
AIC.
The Committee on Monitoring and Assessment of Trends in Acid
Deposition was organized by the National Research Council to carry
out the study. The committee, comprising experts in the disciplines of
atmospheric chemistry, visibility, environmental monitoring,
analytical chemistry, aquatic chemistry, geochemistry, geology,
forestry, fisheries resources, climatology, and statistics, conducted its
work under the auspices of the Council's Environmental Studies
Board. The committee reviewed and summarized the available
literature and data on historical trends in phenomena related to the
emission and deposition of acidic materials. Other chemical substances
are recognized to play an important role in certain effects, but
insufficient information existed to incorporate their assessment in this
report.
In the process of reviewing the literature and available data, the
committee found that a number of the potentially informative sets of
data that exist had previously not been analyzed for this purpose. We
concluded that in order to conduct a comprehensive study, it would be
necessary for us to obtain and analyze these data. The report therefore
contains not only our review of the literature but also original analyses
of a number of data sets. The analyses were prepared by members of
the committee, often with the assistance of consultants and colleagues,
and are contained in the respective chapters of the report. Members of
the committee and their colleagues who prepared the respective
chapters are identified. The analyses, which commanded considerable
commitments of time and energy from the members, permitted us to
assess the implications of findings for a number of diverse phenomena
together, which greatly enhances the strength of our conclusions.
The committee is indebted to its colleagues and consultants for their
contributions and to the reviewers for their helpful comments and
suggestions. We are particularly indebted to Richard A. Smith and
Richard B. Alexander of the U.S. Geological Survey for their significant
contributions to the analysis of surface water chemistry data and to the
preparation of Chapter 7. We wish to single out for special recognition
William M. Stigliani, professional staff officer for the project; without
his tireless work, this complex and difficult project could not have been
. . .
v'~z
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accomplished. Other members of the NRC staff also made important
contributions to the effort, including Myron F. Uman, staff director of
the Environmental Studies Board, who provided administrative
leadership; Joyce Fowler and Carolyn Stewart, project secretaries;
Roseanne Price and Joanne B. Sprehe, editors; and the manuscript
processing unit headed by Estelle Miller.
The report required an unusual level of effort and commitment by
members of the committee. It is not possible to commend them
adequately for their enthusiasm, dedication, and cooperation. They
were presented with the difficult challenge and, in performing original
analyses, undertook more than most NRC committees are asked to do.
Although assisted by staff, colleagues, and consultants, and having
the benefit of helpful comments from more than 30 anonymous
reviewers, the committee bears full responsibility for the report.
Finally, the project would not have been possible without the
generous support of its sponsors, the U.S. Environmental Protection
Agency, the U.S. Geological Survey, and a consortium of private
foundations: the Carnegie Corporation of New York, the Charles E.
Culpepper Foundation, Inc., the William and Flora Hewlett
Foundation, the John D. and Kathryn T. MacArthur Foundation, the
Andrew W. Mellon Foundation, the Rockefeller Foundation, and the
Alfred P. Sloan Foundation.
J. H. GIBSON, Chairman
lX
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Contents
I. SUMMARY AND SYNTHESIS
Findings and Conclusions, 6; Methods, 9; Mechanisms,
11; Spatial Patterns and Temporal Trends, 21; References,
46
2. EMISSIONS OF SULFUR DIOXIDE AND NITROGEN OXIDES
AND TRENDS FOR EASTERN NORTH AMERICA .........
Rudolf B. Husar
Introduction, 48; Production and Consumption of Fuels
and Metals, 53; Sulfur Emission Trends, 78; Regional
Trends in Emissions of Nitrogen Oxides, 82; Comparisons
with Other Trend Estimates, 86; Summary, 89;
References, 91
3. UNCERTAINTIES IN TRENDS IN ACID DEPOSITION: THE
ROLE OF CLIMATIC FLUCTUATIONS ...................
Raymond! S. Bradley
Introduction, 93; Cyclone Tracks, 94; Precipitation and
Drought, 95; Air Stagnation Episodes, 101; Temperature,
103; Summary, 107; References, 107
4. PATTERNS AND TRENDS IN DATA FOR ATMOSPHERIC
SULFATES AND VISIBILITY ..........................
. .. .
fonn Tryon~s
Introduction, 109; Description of Data Bases, 110;
Geographical Distribution, 112; Historical Trends, 114;
Conclusions, 124; References, 125
5. PRECIPITATION CHEMISTRY ......................
Gary J StensZand, Douglas M. Whelpdlale, and Gary
OehZert
Introduction, 128; Data Evaluation, 132; Geographical
Distribution, 142; Time-Trend Information, 159;
Conclusions and Recommendations, 193; References, 196
Xl
.. 48
93
109
... 128
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6. THE NATURE AND TIMING OF THE DETERIORATION OF
RED SPRUCE IN THE NORTHERN APPALACHIAN
MOUNTAINS ..............................
Arthur H. Johnson and Samuel B. McLaughlin
Introduction, 200; High-Elevation Coniferous Forests of
the Appalachians, 201; Deposition of Acidic Substances
and Heavy Metals in Northern Appalachian Forests, 203;
Characteristics of Red Spruce in High-Elevation
Coniferous Forests, 208; Summary of Possible Causes,
221; References, 226
7. STREAMS AND LAKES .............................
James R. Kramer, Anders W. Andren, Richard A.
Smith, Arthur H. Johnson, Richard B. Alexander,
and Gary Oehiert
Introduction, 231; Sulfate Fluxes in Precipitation and
Lakes, 236; Trends in the Chemistry of Headwater
Streams over the Past 15 to 20 Years, 243; Protolytic
Chemistry of Surface Waters of New Hampshire, New
York, and Wisconsin, 260; Summary, 287; References, 290
S. FISH POPULATION TRENDS IN RESPONSE TO SURFACE
WATER ACIDIFICATION ........................
Terry A. Haines
Introduction, 300; Laboratory Investigations, 301; Field
Experiments, 301; Spatial Associations, 304; Temporal
Associations, 310; Summary, 327; References, 329
9. PALEOLIMNOLOGICAL EVIDENCE FOR TRENDS IN
ATMOSPHERIC DEPOSITION OF ACIDS AND METALS
Donald F. Charles and Stephen A. Norton
. .
Introduction, 335; Diatom and Chrysophyte Sediment
Assemblages, 337; Assessment of Recent Lake
Acidification Trends in Eastern North America, 349;
Uncertainties in the Interpretation of Sediment Diatom
and Chrysophyte Assemblage Data and
Recommendations for Further Research, 363; The
Chemical Stratigraphy of Lake Sediments, 369; The
Sediment Record, 374; The Chemical Stratigraphy of Peat
Bog Deposition, 392; Direct Comparison of Diatom and
Chemical Data, 402; Conclusions, 409; References, 411
. .
All
...... 200
231
.... 300
... 335
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APPENDIXES
A. Methods for Sampling and Analysis of
Red Spruce Data ...........................
B. Input Sulfate Fluxes to Lakes from Wet-Only
Deposition and Output Sulfate Fluxes
from Takes: Data Sources and Methods ........
C. Characteristics of Bench-Mark Streams ....
D. Historical Correction Factors for Alkalinity
and Acid Status of Surface Waters .............
E. Physical and Chemical Characteristics of Some
Lakes in North America for Which
Sediment-Diatom Data Exist ...............
. . .
x~'
. . . —
. 435
... 441
445
471
. 482
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