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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 reportAcid 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 reportAcid Deposition: Processes of Lake Acidification (1984)reviewed alternative hypotheses regarding geochemical processes in watersheds responding to acid inputs from the atmosphere. Another reportAcid 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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