ENVIRONMENTAL TRACERS IN SUBSURFACE HYDROLOGY

ENVIRONMENTAL TRACERS IN SUBSURFACE HYDROLOGY

Edited by

Peter G. Cook and Andrew L. Herczeg

CSIRO Land and Water, Glen Osmond, Australia

~.

" Springer Science+Business Media, LLC

Library of Congress Cataloging-in-Publication Data

Environmental tracers in subsurface hydrology I edited by Peter G. Cook and Andrew L. Herczeg

p.em. Ineludes bibliographieal referenees. ISBN 978-1-4613-7057-4 ISBN 978-1-4615-4557-6 (eBook) DOI 10.1007/978-1-4615-4557-6

1. Radioactive tracers in hydrogeology. 2. Groundwater traeers. 1. Cook, Peter G. (Peter Gordon), 1965- II. Herczeg, Andrew Leslie

GB1001.72.R34 E58 1999 577' .49'0285--de21 99-048102

Copyright © 2000 Springer Science+Business Media New York Origina11y published by Kluwer Academic Publishers in 2000 Softcover reprint of the hardcover 1 st edition 2000 AII rights reserved. No part of this publication may be reproduced, stored in a retrieval system or transmitted in any form or by any means, mechanical, photo­copying, recording, or otherwise, without the prior written permission of the publisher, Springer Science+Business Media, LLC.

Printed on acid-free pa per.

Contents

List of Contributors Preface Acknowledgements

1. Determining Timescales for Groundwater Flow and Solute Transport Peter G. Cook and John-Karl Bohlke

2.

3.

4.

5.

Inorganic Ions as Tracers Andrew L. Herczeg and W. Mike Edmunds

Isotope Engineering - Using Stable Isotopes of the Water Molecule to Solve Practical Problems Tyler B. Coplen, Andrew L. Herczeg and Chris Barnes

Radiocarbon Dating of Groundwater Systems Robert M. Kalin

U-Series Nuclides as Tracers in Groundwater Hydrology J. Kenneth Osmond and James B. Cowart

6. Radon-222

7.

8.

9.

10.

11.

12.

L. DeWayne Cecil and Jaromy R. Green

Sulphur and Oxygen Isotopes in Sulphate H. Roy Krouse and Bernhard Mayer

Strontium Isotopes Robert H. McNutt

Nitrate Isotopes in Groundwater Systems Carol Kendall and Ramon Aravena

Chlorine-36 Fred M. Phillips

Atmospheric Noble Gases Martin Stute and Peter Schlosser

Noble Gas Radioisotopes: 37 Ar, 85 Kr, 39 Ar, 81 Kr Heinz H. Loosli, Bernhard E. Lehmann and William M. Smethie, Jr.

vii xiii

xv

31

79

111

145

175

195

233

261

299

349

379

VI

13.

14.

15.

16.

3H and 3He D. Kip Solomon and Peter G. Cook

4He in Groundwater D. Kip Solomon

Chlorofluorocarbons L. Niel Plummer and Eurybiades Busenberg

8 II B, Rare Earth Elements, 8 37 Cl, 32 Si, 35 S, 1291 Avner Vengosh, Arthur J. Spivack, Kevin J. Johannesson, W. Berry Lyons, Tamie R. Weaver, Uwe Morgenstern, Robert L. Michel, June Fabryka-Martin

Appendix 1: Stable Isotope Notation and Fractionation

Appendix 2: Decay Constants and Half-Lives of Radioactive Isotopes

Appendix 3: Solubilities of Environmental Gas Tracers

Appendix 4: Liquid and Gas-Phase Diffusion Coefficients

Index

397

425

441

479

511

517

519

521

523

List of Contributors

Ramon Aravena Department of Earth Sciences University of Waterloo Waterloo, Ontario N2L 3Gl, Canada roaraven@sciborg.uwaterloo.ca

Chris Barnes Faculty of Engineering and Information Technology Australian National University Canberra, ACT 0200, Australia Chris.Barnes@fareng.anu.edu.au

John-Karl Bohlke US Geological Survey 431 National Center Reston, VA 20192, USA jkbohlke@usgs.gov

Eurybiades Busenberg US Geological Survey 432 National Center Reston, VA 20192, USA ebusenbe@usgs.gov

L. DeWayne Cecil US Geological Survey 900 N. Skyline Drive, Suite C Idaho Falls, ID 83402, USA Idcecil@usgs.gov

Peter G. Cook CSIRO Land and Water Private Mail Bag No.2 Glen Osmond, SA 5064, Australia Peter.Cook@adl.c1w.csiro.au

Tyler B. Coplen US Geological Survey 431 National Center Reston, VA 20192, USA tbcoplen@usgs.gov

viii

James B Cowart Florida State University Department of Geology Tallahassee, FL 32306-3026, USA jcowart@gly.fsu.edu

W. Mike Edmunds Hydrology Group British Geological Survey Crowmarsh Gifford Wallingford,Oxon OXlO 8BB, UK wyndham.m.edmunds@bgs.ac.uk

June Fabryka-Martin Los Alamos National Laboratory E-ET Mail Stop J514 Los Alamos, NM 87545, USA fabryka@ Ian!. gov

J aromy R. Green US Geological Survey 900 N. Skyline Drive, Suite C Idaho Falls, ID 83402, USA jrgreen@usgs.gov

Andrew L. Herczeg CSIRO Land and Water Private Mail Bag No.2 Glen Osmond, SA 5064, Australia Andrew.Herczeg@ad!.c1w.csiro.au

Kevin H. Johannesson Old Dominion University Department of Ocean, Earth, and Atmospheric Sciences 4600 Elkhorn A venue Norfolk, VA 23529, USA kjohanne@odu.edu

Robert M. Kalin Environmental Engineering Research Centre School of Civil Engineering The Queen's University of Belfast Belfast, BT9 SAG N. Ireland, UK r.kalin@gub.ac.uk

Carol Kendall US Geological Survey Mail Stop 434 345 Middlefield Road Menlo Park, CA 94025, USA ckendall@usgs.gov

H. Roy Krouse Department of Physics and Astronomy University of Calgary 2500 University Drive Calgary, Alberta T2N IN4, Canada roy@earth.geo.ucalgary.ca

Bernhard E. Lehmann Physics Institute University of Bern Sidlerstr.5 CH-3012 Bern, Switzerland lehmann@climate.unibe.ch

Heinz H. Loosli Physics Institute University of Bern Sidlerstr.5 CH-3012 Bern, Switzerland loosli@climate.unibe.ch

w. Berry Lyons Department of Geology University of Alabama Tuscaloosa, AL 35487-0338, USA blyons@wgs.geo.us.edu

Robert H. McNutt University of Toronto at Mississauga Erindale College 3359 Mississauga Road North Mississauga, Ontario L5L lC6, Canada rmcnutt@credit.erin.utoronto.ca

ix

x

Bernhard Mayer Department of Physics and Astronomy, and Department of Geology and Geophysics University of Calgary 2500 University Drive NW Calgary, Alberta T2N IN4, Canada bernhard@earth.geo.ucalgary.ca

Robert L. Michel US Geological survey Mail Stop 434 345 Middlefield Road Menlo Park, CA 94025, USA rlmiche1@usgs.gov

Uwe Morgenstern Institute of Geological and Nuclear Sciences 41 Bell Road South Lower Hutt, New Zealand U .Morgenstern@gns.cri.nz

J. Kenneth Osmond Florida State University Department of Geology Tallahassee, FL 32306-3026, USA osmond@gly.fsu.edu

L. Nie1 Plummer US Geological Survey 432 National Center Reston, VA 20192, USA nplummer@usgs.gov

Fred M. Phillips Department of Earth and Environmental Science New Mexico Tech Socorro, NM 87801, USA phillips@nmt.edu

Peter Schlosser Lamont-Doherty Earth Observatory Columbia University PO Box 1000 Palisades, NY 10964-1000, USA peters@ldeo.columbia.edu

William M. Smethie, Jf. Lamont-Doherty Earth Observatory Columbia University PO Box 1000 Palisades, NY 10964-1000, USA bsmeth@ldeo.columbia.edu

D. Kip Solomon Department of Geology and Geophysics 717 WBB University of Utah Salt Lake City, UT 84112-1183, USA ksolomon@mines.utah.edu

Arthur J. Spivack Center for Marine Science Research University of North Carolina at Wilmington 7205 Wrightsville Ave. Wilmington, NC 28403, USA spi vacka@uncwil.edu

Martin Stute Lamont-Doherty Earth Observatory Columbia University PO Box 1000 Palisades, NY 10964-8000, USA martins@ldeo.columbia.edu

A vner Vengosh Department of Geological and Environmental Sciences Ben Gurion University at the Negev PO Box 653 Beer Sheva 84105, Israel A vnerv@vms.huji.ac.il

Tamie Weaver School of Earth Sciences University of Melbourne Parkville VIC. 3052, Australia t. weaver@earthsci.unimelb.edu.au

Xl

Preface

The idea for this book grew out of the 1996 Western Pacific Geophysics Meeting of the American Geophysical Union, Brisbane, July 1996, at which the editors convened a special session on environmental tracers. After being approached by Kluwer to put together a volume, we only decided to proceed when our suggestion received an enthusiastic response by the authors of the following chapters. We insisted that the book would not be simply a proceedings of the conference, but rather we 'head-hunted' experts in the various fields of environmental tracers. In the early years, much of the research on environmental tracers appeared in proceedings of conferences and specialist meetings held at regular intervals by the International Atomic Energy Agency. However, the field has been expanding greatly within the past decade, and studies incorporating environmental tracers have become more common in the mainstream literature. There have also been large advances in a number of areas since publication of the major review work of Fritz and Fontes (1980, 1986). Since we began compiling this manuscript, two new publications have appeared. Kendall and McDonnell (1998) provides a comprehensive overview ofthe role of isotope tracers in catchment studies. The book considers mainly environmental tracers, but also including some discussion of applied isotopes. Clark and Fritz (1997) includes a much more detailed discussion of theoretical issues than Kendall and McDonnell (1998), and focuses on the more widely used isotopes (especially 180, 2H and 14C). Our publication focusses on subsurface hydrology, and attempts to provide a comprehensive look at each of the tracers, with particular emphasis on their use in integrated studies.

Environmental tracers can be used for determining sources of contaminants and other solutes; for determining solute transport, reaction and degradation pathways and rates; and, in the case of the more conservative tracers, for determining water flow rates. Many of the environmental tracers (e.g., 14C, 222Rn, 36CI, 81 Kr, 85Kr, 39Ar, 3H, 3He, 4He, 35S, 32si, 1291, CFCs) can be used to determine! groundwater 'ages' or 'travel times', and some of the issues related to the use of these tracers are discussed in Chapter 1. In particular, the development of 3HPHe and CFC dating within the past 1 ° years has led to exciting opportunities to combine groundwater dating methods with groundwater contamination studies. In some cases, these studies have been combined with stable isotope studies to determine not only sources of contaminants, but also contaminant input histories, transport rates and degradation rates. Clearly, environmental tracers have a role in all aspects of subsurface hydrology.

Chapters 2 through 15 discuss the applications of each of the more commonly used environmental tracers. Tracers which are currently most widely used (e.g., 14C, 180, 2H) are given equal weight with newer techniques (e.g., 3HPHe, CFCs). Too often, investigators use techniques that they are familiar with, even though they may not necessarily be the most suitable for the task at hand. Hopefully, a book such as this one will introduce investigators to new techniques, and help to overcome this problem. Each chapter begins with an outline of the essential principles of the use of the tracer, followed by a discussion of applications and examples. Analytical and

XIV

sampling methods are referenced, but not discussed in detail. (It is assumed that the reader will consult the papers that are cited for more information here). While more thorough reviews of several of these tracer methods are available elsewhere, our aim was to bring this information together in the one volume, while at the same time keeping the volume to a manageable size. Readers are still encouraged to consult the other sources for more detailed discussions of various aspects of the different techniques. The final chapter contains shorter discussions of some lesser-used techniques, including some which might still be regarded as developmental (e.g., 35S, 32Si).

Peter Cook

Andrew Herczeg

References

Clark I. and Fritz P. (1997) Environmental Isotopes in Hydrogeology. Lewis, Boca Raton, 328pp.

Fritz P. and Fontes 1.-Ch. (1980) Handbook of Environmental Isotope Geochemistry. Vol I. The Terrestrial Environment, A. Elsevier, Amsterdam, 545pp.

Fritz P. and Fontes J.-Ch. (1986) Handbook of Environmental Isotope Geochemistry. Vol 2. The Terrestrial Environment, B. Elsevier, Amsterdam, 557pp.

Kendall C. and McDonnell J.1. (1998) Isotope Tracers in Catchment Hydrology. Elsevier, Amsterdam, 839pp.

Acknowledgements

Firstly, the editors would like to thank the authors of the chapters that comprise this book, who collectively did a lot more work than we did. Thanks also go to the reviewers of the various chapters: Simon Bottrell, Tom Bullen, Ian Clark, Jordan Clark, Richard Cresswell, George Darling, Peter Folger, Mel Gascoyne, Andrew Love, Berry Lyons, Gavin McNeill, Emanuel Mazor, Niel Plummer, Kazimir Rozanski, Pauline Smedley, Martin Stute, Claude Taylor, Tom Torgersen, Herb Veeh, Glen Walker, Len Wassenaar, Warren Wood and Yuecil Yurtsever. Particular thanks are also due to Tricia Williams for formatting this book, Fiona Cahill for administrative and organisational support, Greg Rinder and Bob Schuster for drafting many of the figures, and Glen Harrington for assistance with indexing. The authors would like to acknowledge the financial support provided by CSIRO Land and Water, and South Australian Department of Environment, Heritage and Aboriginal Affairs.