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Atmosphere- Biosphere Interactions: Toward a Better Understanding of the Ecological Consequences of Fossil Fuel Combustion A Report Prepared by the Committee on the Atmosphere and the Biosphere Board on Agriculture and Renewable Resources Commission on Natural Resources National Research Council NATIONAL ACADEMY PRESS Washington, D.C. 1981

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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. This study was supported by the U.S. Environmental Protection Agency, the Forest Service of the U.S. Department of Agriculture, and the Fish and Wildlife Service and National Park Service of the U.S. Department of the Interior. Because of the timely nature of its content and widespread requests for its early release, this report has been reproduced directly from the typescript. Library of Congress Catalog Card Number 81-84469 International Standard Book Number 0-309-03196-6 Available from: NATIONAL ACADEMY PRESS 2101 Constitution Ave., N.W. Washington, D.C. 20418 Printed in the United States of America

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COMMITTEE ON THE ATMOSPHERE AND THE BIOSPHERE David W. Schindler (Chairman), Freshwater Institute, Winnipeg, Manitoba Martin Alexander, Cornell University Edward D. Goldberg, Scripps Institution of Oceanography Eville Gorham, University of Minnesota Daniel Grosjean, Environmental Research and Technology, Inc., Westlake Village, California Halstead Harrison, University of Washington Walter W. Heck, USDA/SEA and Botany Department, North Carolina State University Rudolph B. Husar, Washington University Thomas C. Hutchinson, University of Toronto Svante Oden, Swedish University of Agricultural Sciences, Uppsala Gerald T. Orlob, University of California, Davis Lars Overrein, Norwegian Water Research Institute, Oslo Douglas M. Whelpdale, Atmosphere Environment Service, Downsview, Ontario Liaison Robert C. Harriss, NASA Langley Research Center Staff l James Tavare s, Pro j ect Staf f Of f icer Jef frey Brotnov, Associate Stat f Of f icer Catherine lino, Editor Carole B. Carstater, Secretary Sheridan E. Caldwell, Secretary iii

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BOARD ON AGRICULTURE AND RENEWABLE RESOURCES George K. Davis (Chairman), University of Florida, retired Neville P. Clarke (Vice Chairman), Texas Agricultural Experiment Station, College Station William L. Brown, Pioneer Hi-Bred International, Inc. Robert O. Herrmann, Pennsylvania State University Minoru Hironaka, University of Idaho Laurence R. Jahn, Wildlife Management Institute Bernard S. Schweigert, University of California, Davis E. Wayne Shell, Auburn University George R. Staebler, Weyerhaeuser Co., retired Champ B. Tanner, University of Wisconsin John F. Timmons, Iowa State University Paul E. Waggoner, Connecticut Agricultural Experiment Station, New Haven Philip Ross, Executive Secretary COMMISSION ON NATURAL RESOURCES Robert M. White (Chairman), University Corporation for Atmospheric Research Timothy Atkeson, Steptoe & Johnson Stanley I. Auerbach, Oak Ridge National Laboratory Neville P. Clarke, Texas Agricultural Experiment Station, College Station Norman A. Copeland, E.I. du Pont de Nemours & Co., retired George K. Davis, University of Florida, retired Joseph L. Fisher, The Wilderness Society Edward D. Goldberg, Scripps Institution of Oceanography Charles J. Mankin, Oklahoma Geological Survey Norton Nelson, New York University Medical Center Daniel A. Okun, University of North Carolina David Pimentel, Cornell University John E. Tilton, Pennsylvania State University E. Bright Wilson, Harvard University; ex officio Wallace D. Bowman, Executive Director iv

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ACKNOWLEDGMENTS The Committee gratefully acknowledges the leadership of Ellis B. Cowling in initiating this study and in chairing the planning session that developed its scope. Thanks are also due to Barbara D. Brown and Raymond Her rmann of the National Park Service, Leon Dochinger and Donald Boelter of the U.S. Forest Service, Kent Schreiber of the U.S. Fish and Wildlife Service, and Dennis Tirpak of the U.S. Environmental Protection Agency. Their liaison role contributed richly to committee discussions and kept us informed of their agency's interests as they related to our study. We also thank G.J. Brunskill and J.H. Klaverkamp who reviewed the text and provided numerous references. The interaction with the NRC Report Review Committee was rewarding and beneficial to the report. The Committee owes a special debt of gratitude to Robert Harriss, who contributed so generously of his time and thinking and helped in the writing of the report. Finally, we thank the NRC staff members whose unflagging efforts and genuine interest made service on the Committee the enjoyable and successful experience that it was. v

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CONTENTS List of Figures. List of Tables . . CHAPTER 1: INTRODUCTION AND OVERVIEW. The Fossil Fuel Scenario: The Probability of a Crisis in the Biosphere. . . . . . This Report. . . . . . . Conclusions and Recommendations. . . . . . . . . . . . . . . . . . . 7 CHAPTER 2: SCIENTIFIC UNDERSTANDING OF ATMOSPHERE-BIOSPHERE INTERACTIONS: A HISTORICAL OVERVIEW. . . . . . . . . . . . . . . 9 . . . . . . . . . . .13 i. ~,.,~, . . . ~ , · — Energy and Air Pollution . . . ~ . . . . . . . . . . . . . . . . . .19 Hymn Al P=r=timn~ of the Atmosphere. . CHAPTER 3: BIOGENIC EMISSIONS TO THE ATMOSPHERE . . . . . . . . . . Nitrogen . . . . . . . . . . . . . . . . . . . ~ ~ Terrestrial Ecosystems . . . . . . . . . . . . . . . . . . . . . Aquatic Ecosystems . . . . . . . . . . . . . . . . . . . . . . . Sulfur . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Terrestrial Ecosystems . . . . . . . . . . . . . . . . . . . . . Aquatic Ecosystems . . . . . . . . . . . . . . . . . . . . . . . Trace Metals ........................... Atmospheric Emissions from Burning of Natural Biomass. . . . . . . Natural Organic Products . . . . . . . . . . . . . . . . . . . . . Summary. . . . . . . . . CHAPTER 4: ANTHROPOGENIC SOURCES OF ATMOSPHERIC SUBSTANCES. . . . . .22 .22 .22 .25 .26 .26 .27 .28 .30 .32 .32 .35 Patterns of Fossil Fuel Use. . . . . . . . . . . . . . . . . . . . .36 Atmospheric Emissions from Fossil Fuel Burning . . . . . . . . . . .38 Oxides of Sulfur and Nitrogen. . . . . . . . . . . . . . . . . . .41 · . V11

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Trace Metals Organic Compounds . Sununary . a47 5 4 e ~ ~ ~ ~ ~ e ~ ~ ~ ~ 56 CHAPTER 5: ATMOSPHERIC TRANSPORT, TRANSFORMATION, AND DEPOSITION PROCESSES . . . . . . . . . . . . . . . . . . . . . . . . e Transport and Dif fusion. . . . . . . . . . . . . . . . Transformat ions. . . . . e ~ ~ ~ ~ ~ ~ ~ e e e Oxidation Reactions in the Atmosphere .57 .59 . .60 —~ __ _ . . . . . . . . . . . . . . 6 2 Reduction Reactions in the Biosphere . . . . . . . . . . . he Organ ic Compound s . . . . . Deposition . . . . . . We t Deposi t ion Processe s new no; a; ~^ DO - ~_,z~.=_~___~lĒ~V-C=~=·············· - Residence Times for Substances in the Atmosoher~ Monitoring and Data Needs....... Summa ry . . . . . ~ . . . . . .70 __ _ . . . . . . . . 74 . . . . . . . . . . . . . 7 7 . . . . . . . . . . . . . .84 CHAPTER 6: BIOLOGICAL ACCUMULATION AND EFFECT OF ATMOSPHERIC CONTAMINANTS . . .87 Accumulation in Terrestrial Ecosystems 87 Accumulation in Aquatic Ecosystems 88 Accumulation in Soils and Aquatic Sediments. . . . . . . . . . . . .93 Aquatic Sediments a s Hi star ical Records . ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ ~ . 9 5 Transformations in Soils and Waters. . . . . . . . . . . . . . . . .95 Transfer of Substances from Terrestrial to Aquatic Ecosystems. . . .99 Pollutants and Individual Organisms. . . . . . . . . . . . . . . . 101 Toxicity of Deposited Substances to Organisms. . . . . . . . . . 104 Interactions Among Pollutants or Between Pollutants and Other Stresses . . . . . . . . . . . . . . . . . . . . . . . . 108 Resistance to Pollutants 114 Past Ef forts to Predict Wide F;Or-~ ~ HEY i - Off feed ~ i, c CHAPTER 7: STUDYING THE EFFECTS OF ATMOSPHERIC DEPOSITION ON ECOSYSTEMS. Predicting Anthropogenic Effects on Ecosystems 121 Highly Sensitive Organisms as Early Indicators . . . . . . . . ] OR Colon Responses of Ecosvstems to.~tr-.~ , ~ , , . . . . . . . . . . . 1 2 9 Natural Records of Pollution e ~ ~ ,.20 Monitoring Large-Scale Pollution - Summary . CHAPTER 8: ACID PRECIPITATION . Causes of Ac id Precipitation . . . . . . . . Extent of the Problem . ., 133 ............. 139 ............. 140 . ....... 140 ~ , , ~ . . . . . . . . . ~ ~ ~ . 1 ~ ~ Ef fects of Acid on the Biosphere . ........ ~ 149 V111

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Aquatic Ecosystems . . Terrestrial Ecosystems . . . . Assessment of Ecological Ef feats Amelioration . . . . . . Summary. . . . . . . . . APPENDIX Biographical Sketches of Committee Members REFERENCES . INDEX . . . . . 149 . 0 167 . 181 . 181 . 182 1X . 183 . 187 . .233

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FIGURES Projected cadmium concentrations in Lake Michigan for various rates of increase in the annual input rate. . . . . . . . . . 2.1 Chemical composition of rain in the British Isles reported in 1872 3.1 The biological cycle for mercury and arsenic. . . . . . 4.1 World energy production from primary sources, 1950-1977 4.2 Global market shares of primary energy forms. . . . . . 4.3 World energy flux density expressed as kilograms of coal per square kilometer per year, 1970 . . . . . . . . . . 4.4 Coal consumption in the United States . . . . 4.5 Sulfur oxide emissions in the United States by source, 1940-1975 43 4.6 Net emissions of nitrogen oxides and sulfur oxides for the United States by source for 1975 and projections for 1990 . . . 44 4.7 Nitrogen oxide emission density in the United States by county. 45 4.8 Nitrogen chemistry in the troposphere . . . . . . . . . . . . . 46 5.1 Dispersion of pollutants introduced into the atmosphere as determined by residence time. . . . . . . . . . . . . . . . . 5.2 Tracing from ERTS photograph, showing the outline of a plume from the 381-m nickel smelter stack at Sudbury, Ontario, crossing Georgian Bay . . . . . . . . . . . . e · · · · 5.3a Simplified photooxidation mechanisms for e-butane . . . . . .5 · . . 16 . 31 . 37 . 37 . 39 . 40

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5.3b Simplified photooxidation mechanisms for isopren e . . . 5.3c Simplified photooxidation mechanisms for toluene. . . . . . . . 68 5.3d Simplified photooxidation mechanisms for monoterpenes . . . . The effects of wet and dry leaf surfaces and light and dark on the deposition velocity of SO2 in wind tunnel experiments for three tree species. . . . . . . . . . . . . . . . . . . 5.5 Velocity of deposition of particles onto short grass. . . 5.6 Resistance to dry deposition of pollutant gases in a cereal crop ......................... 5.7 Atmospheric lifetimes of gaseous organic compounds. . . . . Mean annual pH of precipitation in the United States and Canada, 1979-1980 . . . . . . . . . . . . . . . . . . . . . . 69 . . 71 . . 73 e 75 . . 80 . . 81 5.9 Average lead deposition by precipitation over the continental United States, September 1966 to March 1967 . . . . . . . . . . 82 5.10 Average zinc deposition by precipitation over the continental United States, September 1966 to March 1967 . . . . . . . . . 5~11 Median concentrations of metals in precipitation in remote, rural, and urban areas relative to organism toxicity levels. . . . . . . . . . . ~ ~ - . ~ ~ 6.1 Electrical analog of pollutant exchange between leaf and surrounding air ...................... . 82 . . 89 6.2 Seasonal changes of pH of lake water taken from the outlet of Little Moose Lake, Adirondacks, New York, and from a 3-m deep pipe in the lake . . . . . . . . . . . . . . ~ e ~ ~ ~ ~ ~ 9 2 6.3 Nomogram used to predict changes in the acidity of lakes as the acidity of precipitation changes . . . . . . . . . . . . 102 6.4 Thresholds for the death of plants, foliar lesions, and metabolic or growth effects as related to the nitrogen dioxide concentration and the duration of exposure. . . . . . . . . . . 106 Interactive effects of pollutants . . . . . . . . . . . . . 6.6 A model for tolerance limits of Asellus aquaticus toward low water hardness and low pH . . . . . . . . . . . . . . . . 110 . . . 112 Models of interactions in the atmosphere-biosphere system . . . 123 Charcoal (elemental carbon) concentration as a function of depth in the Lake Michigan core . . . . . . . . . . . . . · ~ X11 . . ~ 134

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7.3 Metal concentrations (by dry weight) as a function of depth in the Lake Michigan core 135 Monthly mean concentrations at Barrow, Alaska, of atmospheric sulfate and vanadium that could not be attributed to natural processes 137 7.5 Changes in pH values of a Scandinavian river. . . . . . . . . 8.1 Sulfate concentrations on a sea-salt-free basis in northwestern Greenland glacier samples. . . . . . . . . . . . . 138 . 141 8.2 The formation of sulfuric and sulfurous acids from sulfur oxide pollutants. . . . . . . . . . . . . . . . . . . . . . . . 144 8.3 The pH of levels of precipitation in Scandinavia, 1955-1975 8.4 Average stack height and tallest stack reported among power plants burning fossil fuels (bituminous coal, lignite, oil) included in biannual design surveys of new power plants, 1956 "~ ~ O70 .. 145 8.5 Titration curve for bicarbonate solution at a concentration of 100 / OCR for page R1
8.14 Concentration of silicon in relation to pH level in 20 Swedish west coast lakes, August 1978 . . . . . . . . . . . . . . . . 8.15 The pH tolerance limit for 17 widespread species of molluscs and crustaceans . . . . . . . . . . . . . . . . . . . . . . . 6 Egg Matchability of several fish species as a function of pH. 8.17 Occurrence of fish species in six or more La Cloche lakes, in relation to pH ...................... 8.18 A hypothetical model of the effect of acid precipitation upon the nitrogen cycle in forests . . . . . . . . . . . . . . . . 8.19 Loss of nutrients by weathering and mineralization. . . . 8.20 Distribution of adsorbed 35SO42- sulfur in soil profiles. 8.21 Effect of acidity upon the leaching of heavy metals from spruce humus layers, normalized to pH 4.2 . . . . . . . . . . Correlation between denitrification rates and soil pH . . . . · — xiv e 162 166 171 . 174 . . . 175 . 177 . 178

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TABLES 3.1 Emissions of major pollutants from residential wood combustion. 33 3.2 4.1 4.2 Natural sources of organic carbon . . . . . . . . . . . . Atmospheric sulfur budget for eastern North America . . . Total U.S. NOX emissions for the years 1950 and 1975. . . . . 4.3 Range in estimates of anthropogenic mercury emissions to the global atmosphere 49 4.4 Amounts of elements mobilized into the atmosphere as a result of weathering processes and the combustion of fossil fuels. . . 51 Worldwide anthropogenic and natural emissions of trace metals during 1975. . . . . . . . . . . . . . . . . . . . . . . 52 4.6 Emissions of volatile oxides from the production of cement. . . 53 4.7 Estimates of global primary particulate organic carbon (POC) emissions from anthropogenic sources, 1973-1974 . . . . . . 5.1 Dry deposition of atmospheric and gaseous sulfur and nitrogen compounds. . . . . . . . . . . . . . . . . . . 5.2 Residence times of metals in the atmosphere at La Jolla and Ensenada. e.~-~-~-~---- . . . 34 42 · · — . 48 5.3 Average residence times in the atmosphere of substances not given in Table 5.2. ea.--~--~--~--- 5.4 Major studies of atmospheric transport and deposition currently under way in the United States. . . . . . . 6.1 Types of interactions of gases with plant surfaces. . xv . . 55 · · —

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6.2 Effects on native vegetation of SO2 in combination with other pollutants. . . . . . . . . - - . Plant processes and characteristics that may increase tolerance to acid precipitation . . . . . . . . . . . . . . 7.1 Major factors to be determined in an assessment of the ecological effects of a pollutant . . . . . . . . . . 8.1 Factors affecting the vulnerability of an ecosystem to acid rain . . . . Results of recent experiments on effects of simulated acidic precipitation on crops grown under greenhouse conditions. . 8.3 Results of recent experiments on effects of simulated acidic precipitation on field-grown crops. . . . . . . . . . . . . xvi - - . . .109 . .116 . . .126 . .143 . .168 . .169