Table Of ContentNATO ASI Series
Advanced Science Institutes Series
A series presenting the results of activities sponsored by the NA TO Science
Committee, which aims at the dissemination of advanced scientific and
technological knowledge, with a view to strengthening links between
scientific communities.
The Series is published by an international board of publishers in
conjunction with the NATO Scientific Affairs Division
A Life Sciences Plenum Publishing Corporation
B Physics London and New York
C Mathematical and Kluwer Academic Publishers
Physical Sciences Dordrecht, Boston and London
o Behavioural and
Social Sciences
E Applied Sciences
F Computer and Springer-Verlag
Systems Sciences Berlin Heidelberg New York
G Ecological Sciences London Paris Tokyo Hong Kong
H Cell Biology Barcelona Budapest
I Global Environmental
Change
NATo-pea DATABASE
The electronic index to the NATO ASI Series provides full bibliographical
references (with keywords and/or abstracts) to more than 30000
contributions from international scientists published in all sections of the
NATO ASI Series. Access to the NATO-PCO DATABASE compiled by the
NATO Publication Coordination Office is possible in two ways:
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Series I: Global Environmental Change, Vol. 13
The ASI Series Books Published as a Result of
Activities of the Special Programme on
Global Environmental Change
This book contains the proceedings of a NATO Advanced Research
Workshop held within the activities of the NATO Special Programme on
Global Environmental Change, which started in 1991 under the auspices
of the NATO Science Committee.
The volumes published as a result of the activities of the Special Programme
are:
Vol. 1: Global Environmental Change.
Edited by R. W. Corell and P. A. Anderson. 1991.
Vol. 2: The Last Deglaciation: Absolute and Radiocarbon Chronologies.
Edited by E. Bard and W. S. Broecker. 1992.
Vol. 3: Start of a Glacial. Edited by G. J. Kukla and E. Went. 1992.
Vol. 4: Interactions of C, N, P and S Biogeochemical Cycles and Global
Change. Edited by R. Wollast, F. T. Mackenzie and L. Chou. 1993.
Vol. 5: Energy and Water Cycles in the Climate System.
Edited by E. Raschke and D. Jacob. 1993.
Vol. 6: Prediction of Interannual Climate Variations.
Edited by J. Shukla. 1993.
Vol. 7: The Tropospheric Chemistry of Ozone in the Polar Regions.
Edited by H. Niki and K. H. Becker. 1993.
Vol. 8: The Role of the Stratosphere in Global Change.
Edited by M.-L. Chanin. 1993.
Vol. 9: High Spectral Resolution Infrared Remote Sensing for Earth's
Weather and Climate Studies.
Edited by A. Chedin, M.T. Chahine and NA Scott. 1993.
Vol. 10:Towards a Model of Ocean Biogeochemical Processes.
Edited by G. T. Evans and M.J. R. Fasham. 1993.
Vol. 11: Modelling Oceanic Climate Interactions.
Edited by J. Willebrand and D. L.T. Anderson. 1993.
Vol. 12: Ice in the Climate System. Edited by W. Richard Peltier. 1993.
Vol. 13: Atmospheric Methane: Sources, Sinks, and Role in Global
Change. Edited by M. A. K. Khalil. 1993.
Vol. 14: The Role of Regional Organizations in the Context of Climate
Change. Edited by M. H. Glantz. 1993.
Vol. 15: The Global Carbon Cycle.
Edited by M. Heimann. 1993.
Vol. 16: Interacting Stresses on Plants in a Changing Climate.
Edited by M. B. Jackson and C. R. Black. 1993.
Atmospheric Methane:
Sources, Sinks, and Role in
Global Change
Edited by
M. A. K. Khalil
Oregon Graduate Institute
P. O. Box 91000
Portland, Oregon 97291
USA
Springer-Verlag
Berlin Heidelberg New York London Paris Tokyo
Hong Kong Barcelona Budapest
Published in cooperation with NATO Scientific Affairs Division
Proceedings of the NATO Advanced Research Workshop on the Atmospheric
Methane Cycle: Sources, Sinks, Distributions, and Role in Global Change, held
at Mt. Hood near Portland, OR, USA, October 7-11, 1991
ISBN-13: 978-3-642-84607-6 e-ISBN-13:978-3-642-84605-2
001: 10.1007/978-3-642-84605-2
Library of Congress Cataloging-in-Publication Data
Atmospheric methane: sources, sinks, and role in global change / edited by MAK. Khalil. p. cm. -
(NATO ASI series. Series I, Global environmental change; vol. 13)
"Published in cooperation with NATO Scientific Affairs Division."
"Proceedings of the NATO Advanced Research Workshop on the Atmospheric Methane Cycle:
Sources, Sinks, Distributions, and Role in Global Change, held at Mt. Hood near Portland, OR, USA,
October 7-11,1991" - T.p. verso.
ISBN-13: 978-3-642-84607-6
1. Atmospheric methane-Congresses. 2. Sinks (Atmospheric chemistry)-Congresses. 3. Methane-
Environmental aspects-Congresses. I. Khalil, M. A. (Muhammad Ahsan Khan), 1950- . II. North
American Treaty Association. Scientific Affairs Division. III. NATO Advanced Research Workshop on
the Atmospheric Methane Cycle: Sources, Sinks, Distributions, and Role in Global Change (1991 :
Portland, Or.) IV. Serie:;. QC879.85.A78 1993 551.5'112-dc20 93-31890
This work is subject to copyright. All rights are reserved, whether the whole or part of the material is
concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broadcast-
ing, reproduction on microfilm or in any other way, and storage in data banks. Duplication of this
publication or parts thereof is permitted only under the provisions of the German Copyright Law of
September 9, 1965, in its current version, and permission for use must always be obtained from
Springer-Verlag. Violations are liable for prosecution under the German Copyright Law.
© Springer-Verlag Berlin Heidelberg 1993
Softcover reprint of the hardcover 1st edition 1993
Typesetting: Camera ready by authors
31/3145 - 5 43210 - Printed on acid-free paper
Preface
Atmospheric methane is thought to be the most important trace gas
involved in man-made climate change. It may be second only to carbon dioxide
in causing global warming. Methane affects also the oxidizing capacity of the
atmosphere by controlling tropospheric OH radicals and creating 0 3, and it
affects the ozone layer in the stratosphere by contributing water vapor and
removing chlorine atoms. In the long term, methane is a natural product of life
on earth, reaching high concentrations during warm and biologically productive
epochs. Yet the scientific understanding of atmospheric methane has evolved
mostly during the past decade after it was shown that concentrations were rapidly
rising.
Because of the environmental importance of methane, North Atlantic
Treaty Organization's Scientific and Environmental Affairs Division
commissioned an Advanced Research Workshop. This book is the result of such
a conference held during the week of 6 October 1991 at Timberline Lodge on
Mount Hood near Portland, Oregon. About 100 scientists were invited, or
accepted as participants, in recognition of their significant scientific achievements
or potential for leading new developments.
Review lectures on the main topics were presented to the entire assembly
by those who had been invited to write the chapters in this book. Specialist
subgroups met during the next three days, coordinated by session chairs who
documented the discussions in the working group reports included in this volume.
The meeting was extremely active with discussions that continued late into the
nights.
This book began in 1990 when the framework was conceived and writers
were invited. Drafts of most chapters were available at the meeting. After the
meeting, session chairs and other participants met to decide whether there were
gaps in the existing material. Several new chapters were identified and
commissioned. My own writings for the book are in the areas for which I could
not find writers or where there were gaps. During most of 1992 we reviewed,
edited, and refined each chapter. We abandoned the pursuit of perfection early
on, but we sought completeness.
VI
My approach was to define the areas that constitute the current
understanding of methane with a chapter devoted to each subject. Above all, the
book was not to be a collection of specialized research articles but of definitive
and critical reviews that formed a coordinated whole. Research results, I believe,
belong in peer-reviewed journals. Accordingly, it was announced before the
meeting that papers dealing with original research would be considered for
publication in the journal as a companion volume to the book. This allowed
formal presentation and debate on current research results. Much of the
research presented in the journal special issue was discussed in the specialty
working groups, and some papers that were more complete are referenced by the
session chairs in the working group reports. In the end, 55 technical papers were
published in Chemosphere, 26 #s 1-4 (1993) with 814 pages written by 125 authors
from all over the world (see Appendix 2 for a Table of Contents of the journal
special issue).
In putting together this book, I was fortunate to have the support of my
family, of many friends and colleagues, and of generous sponsors. I especially
want to thank Martha J. Shearer and Francis Moraes who, as members of the
technical review team, contributed significantly to editing, reviewing, and
correcting each chapter. I thank Edie Taylor who copy-edited the entire book
and produced the final photo-ready version. I received much valuable advice,
encouragement, and major contributions from the organizing committee, which
consisted of Paul Crutzen, Robert Harriss, Rei Rasmussen, Dominique Raynaud,
and Wolfgang Seiler. Major financial support from NATO's Scientific and
Environmental Affairs Division was the foundation for this work and is gratefully
acknowledged. The critical involvement of scientists from many non-NATO
countries and the excess of U.S. scientists was supported by supplementary grants
from the National Science Foundation (ATM-9120070) and the United States
Environmental Protection Agency (Order No.1-W-1085-NASA). Both these
grants were given to Andarz Company which provided additional support.
M.A.K. Khalil, Professor and Director, Global Change Research Center
Oregon Graduate Institute of Science and Technology, Portland, Oregon 97291-
1000 U.S.A.
ATMOSPHERIC METHANE:
Sources, Sinks, and Role in Global Change
CONTENTS
Preface v
Chapter 1. Introduction 1
Record of Atmospheric Methane
Chapter 2. Measurement and Research Techniques: Working
Group Report
R Conrad and RA. Rasmussen 7
Chapter 3. The Record of Atmospheric Methane
D. Raynaud and J. Chappellaz 38
Chapter 4. Isotopic Abundances in the Atmosphere and Sources
C.M. Stevens 62
Chapter 5. Atmospheric Methane Concentrations: Working
Group Report
B. Stauffer, M. Wahlen, and F. Moraes 89
Formation and Consumption of Methane
Chapter 6. Biological Formation and Consumption of Methane
D.R Boone 102
Chapter 7. Formation and Consumption of Methane: Working
Group Report
N.T. Roulet and W.S. Reeburgh 128
VIII
Sources and Sinks
Chapter 8. Stable Isotopes and Global Budgets
M.J. Whiticar 138
Chapter 9. Methane Sinks and Distributions
M.AK Khalil, M.J. Shearer, and
R.A Rasmussen 168
Chapter 10. Sources of Methane: An Overview
M.AK Khalil and M.J. Shearer 180
Methane Emissions from Individual Sources
Chapter 11. Ruminants and Other Animals
D.E. Johnson, T.M. Hill, G.M. Ward,
KA Johnson, M.E. Branine, B.R
Carmean, and D.W. Lodman 199
Chapter 12. Rice Agriculture: Emissions
M.J. Shearer and M.AK Khalil 230
Chapter 13. Rice Agriculture: Factors Controlling Emissions
H.-U. Neue and P.A Roger 254
Chapter 14. Biomass Burning
J.S. Levine, W.R Cofer, III, and J.P.
Pinto 299
Chapter 15. Wetlands
E. Matthews 314
Chapter 16. Waste Management
S.A Thorneloe, M. A Barlaz, R Peer, L.c. Huff, L.
Davis, and J. Mangino 362
Chapter 17. Industrial Sources
L.L. Beck, S.D. Piccot, and D.A Kirchgessner 399
Chapter 18. Minor Sources of Methane
AG. Judd, RH. Charlier, A Lacroix,
G. Lambert, and C. Rouland 432
IX
Chapter 19. Sources and Sinks of Methane: Working Group
Report
D. Bachelet and H.-U. Neue 457
The Environmental Role of Methane & Current Issues
Chapter 20. The Role of Methane in the Global Environment
D.J. Wuebbles and J.S. Tamaresis 469
Chapter 21. The Current and Future Environmental Role of
Atmospheric Methane: Model Studies and
Uncertainties: Working Group Report
J.P. Pinto, C.H. Bruhl, and A.M. Thompson 514
Appendices
Appendix 1. List of Participants and Photographs of Working Groups 533
Appendix 2. Contents of the Chemosphere Special Issue of
Contributed Papers 545
Index 553
Chapter 1
An Introduction to Atmospheric Methane
M.A.K. KHALIL
Global Change Research Center, Department of Environmental Science and Engineering
Oregon Graduate Institute, P.O. Box 91,000, Portland, Oregon 97291·1000 USA
I have two purposes in writing this chapter. The first is to give a brief
eyewitness report on the evolution of the current knowledge of methane trends,
and the second is to provide a guide to the logic behind this book.
The increasing trend, now so well accepted, is the single most important
reason for the current interest in methane. The trend itself is not complicated
nor is it very profound, but it is a gauge of deeper changes in the methane cycle.
Its existence is the foundation of much of the research during the past decade,
particularly on the global budget, which is tied directly to explaining why methane
is increasing.
The existence of methane in the Earth's atmosphere has been known since
1948 when Migeotte published the first measurements showing concentrations of
about 2 ppmv. It was listed under "non-variable components of atmospheric air"
by Glueckauf in 1951 and similarly in many textbooks since. Glueckauf also
pointed out in his 1951 paper that, from the isotopic analysis by F.W. Libby,
atmospheric methane appeared to be of mostly biogenic origin, and there was
evidence that the concentration was likely to be around 1200 ppbv rather than
the more commonly accepted 2 ppmv; nonetheless, he reported the higher
concentration in his table, which is used to this day (CRC, 1991). From the 1950s
to the early part of the 1980s, there was a prevalent belief that methane was a
stable gas in the Earth's atmosphere. By 1975, well before systematic
measurements could establish globally increasing trends, there were three
important published results that already told us that methane must be increasing
and that it had more than doubled over the last century, both effects due to
human activities, and pointed to the important role of methane emissions in man-
made global change, including tropospheric and stratospheric chemistry. The
three results, largely ignored at the time, were the following.
NATO AS! Series, Vol. I 13
Atmospheric Methane: Sources, Sinks. and Role
in Global Change
Edited by M. A. K. Khalil
© Springer-Verlag Berlin Heidelberg 1993
