Waste Forms Technology
and Performance

FINAL REPORT

Committee on Waste Forms Technology and Performance


Nuclear and Radiation Studies Board
Division of Earth and Life Studies

NATIONAL RESEARCH COUNCIL
                          OF THE NATIONAL ACADEMIES

THE NATIONAL ACADEMIES PRESS

Washington, D.C.

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Committee on Waste Forms Technology and Performance Nuclear and Radiation Studies Board Division of Earth and Life Studies

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THE NATIONAL ACADEMIES PRESS 500 Fifth Street, N.W. Washington, DC 20001 NOTICE: The project that is the subject of this report was approved by the Govern- ing Board of the National Research Council, whose members are drawn from the councils of the National Academy of Sciences, the National Academy of Engineer- ing, and the Institute of Medicine. The members of the committee responsible for the report were chosen for their special competences and with regard for appropri- ate balance. This study was supported by Contract/Grant No. DE-FC01-04EW07022 between the National Academy of Sciences and the U.S. Department of Energy. Any opin- ions, findings, conclusions, or recommendations expressed in this publication are those of the author(s) and do not necessarily reflect the views of the organizations or agencies that provided support for the project. International Standard Book Number-13: 978-0-309-18733-6 International Standard Book Number-10: 0-309-18733-8 Additional copies of this report are available from the National Academies Press, 500 Fifth Street, N.W., Lockbox 285, Washington, DC 20055; (800) 624-6242 or (202) 334-3313 (in the Washington metropolitan area); Internet, http://www.nap. edu. Copyright 2011 by the National Academy of Sciences. All rights reserved. Printed in the United States of America

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The National Academy of Sciences is a private, nonprofit, self-perpetuating society of distinguished scholars engaged in scientific and engineering research, dedicated to the furtherance of science and technology and to their use for the general welfare. Upon the authority of the charter granted to it by the Congress in 1863, the Acad- emy has a mandate that requires it to advise the federal government on scientific and technical matters. Dr. Ralph J. Cicerone is president of the National Academy of Sciences. The National Academy of Engineering was established in 1964, under the charter of the National Academy of Sciences, as a parallel organization of outstanding engi- neers. It is autonomous in its administration and in the selection of its members, sharing with the National Academy of Sciences the responsibility for advising the federal government. The National Academy of Engineering also sponsors engineer- ing programs aimed at meeting national needs, encourages education and research, and recognizes the superior achievements of engineers. Dr. Charles M. Vest is presi- dent of the National Academy of Engineering. The Institute of Medicine was established in 1970 by the National Academy of Sciences to secure the services of eminent members of appropriate professions in the examination of policy matters pertaining to the health of the public. The Insti- tute acts under the responsibility given to the National Academy of Sciences by its congressional charter to be an adviser to the federal government and, upon its own initiative, to identify issues of medical care, research, and education. Dr. Harvey V. Fineberg is president of the Institute of Medicine. The National Research Council was organized 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 advising the federal government. Functioning in accordance with general policies determined by the Academy, the Council has become the principal operating agency of both the National Academy of Sciences and the National Academy of Engineering in providing services to the government, the public, and the scientific and engineering communities. The Council is administered jointly by both Academies and the Institute of Medicine. Dr. Ralph J. Cicerone and Dr. Charles M. Vest are chair and vice chair, respectively, of the National Research Council. www.national-academies.org

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COMMITTEE ON WASTE FORMS TECHNOLOGY AND PERFORMANCE MILTON LEVENSON (Chair), Bechtel International (retired), Menlo Park, California RODNEY C. EWING (Vice Chair), University of Michigan, Ann Arbor JOONHONG AHN, University of California, Berkeley MICHAEL J. APTED, Monitor Scientific, LLC, Denver, Colorado PETER C. BURNS, University of Notre Dame, Notre Dame, Indiana MANUK COLAKYAN, Dow Chemical Company, South Charleston, West Virginia JUNE FABRYKA-MARTIN, Los Alamos National Laboratory, Los Alamos, New Mexico CAROL M. JANTZEN, Savannah River National Laboratory, Aiken, South Carolina DAVID W. JOHNSON, Bell Labs (retired), Bedminster, New Jersey KENNETH L. NASH, Washington State University, Pullman TINA NENOFF, Sandia National Laboratories, Albuquerque, New Mexico Staff KEVIN D. CROWLEY, Study Director DANIELA STRICKLIN, Study Director (Through February 12, 2010) SARAH CASE, Senior Staff Officer TONI GREENLEAF, Administrative and Financial Associate SHAUNTEÉ WHETSTONE, Senior Program Assistant JAMES YATES, JR., Office Assistant v

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NUCLEAR AND RADIATION STUDIES BOARD JAY DAVIS (Chair), Hertz Foundation, Livermore, California BARBARA J. MCNEIL (Vice Chair), Harvard Medical School, Boston, Massachusetts JOONHONG AHN, University of California, Berkeley JOHN S. APPLEGATE, Indiana University, Bloomington MICHAEL L. CORRADINI, University of Wisconsin, Madison PATRICIA J. CULLIGAN, Columbia University, New York ROBERT C. DYNES, University of California, San Diego JOE GRAY, Lawrence Berkeley National Laboratory, Berkeley, California DAVID G. HOEL, Medical University of South Carolina, Charleston HEDVIG HRICAK, Memorial Sloan-Kettering Cancer Center, New York THOMAS H. ISAACS, Stanford University, Palo Alto, California ANNIE B. KERSTING, Glenn T. Seaborg Institute, Lawrence Livermore National Laboratory, Livermore, California MARTHA S. LINET, National Cancer Institute, Bethesda, Maryland FRED A. METTLER, JR., New Mexico VA Health Care System, Albuquerque BORIS F. MYASOEDOV, Russian Academy of Sciences, Moscow RICHARD J. VETTER, Mayo Clinic (retired), Rochester, Minnesota RAYMOND G. WYMER, Oak Ridge National Laboratory (retired), Oak Ridge, Tennessee Staff KEVIN D. CROWLEY, Senior Board Director SARAH CASE, Senior Program Officer OURANIA KOSTI, Program Officer TONI GREENLEAF, Administrative and Financial Associate LAURA D. LLANOS, Administrative and Financial Associate SHAUNTEÉ WHETSTONE, Senior Program Assistant ERIN WINGO, Senior Program Assistant JAMES YATES, JR., Office Assistant vi

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Preface N uclear waste forms are at the center of a successful strategy for the cleanup and isolation of radioactive waste from the environment. Initially, the radioactivity is entirely contained in the waste form, which is the first barrier to the release of radionuclides, making an impor- tant contribution to the performance of the disposal system. Realizing that much of its work lies ahead, the Department of Energy’s Office of Envi- ronmental Management (DOE-EM) recognized the potential importance of new waste forms that could offer enhanced performance and more efficient production and requested this study by the National Research Council. The history of nuclear waste form development and evaluation stretches back more than 30 years. During that time there have been new ideas about the types of materials that could be used; innovations in the technologies for the production of these materials; new strategies for evaluating their performance in a geologic repository; and substantial advances in the rel- evant fields of materials science, geochemistry, processing technologies, and computational simulations. In this report, we attempt to summarize the advances in waste form science with the parallel advances in related fields. Several important messages emerged from this study, including the following: • The evaluation of waste form performance requires careful consid- eration of the near-field disposal environment. Only by matching the disposal environment to a waste form material’s properties can repository performance be optimized. vii

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viii PREFACE • Different materials respond to their disposal environments in dif- ferent ways. “One shoe does not fit all.” One waste form may not be appropriate for all disposal environments. As an example, the optimal disposal environments for spent nuclear fuel and vitrified waste may be different. • There have been important advances in processing technologies, some for other industrial applications. These new or modified tech- nologies may find important applications in waste form production for nuclear applications. • It is important to recognize the limits of current modeling. Unless the mechanisms of waste form degradation are understood, model- ing results are best used for comparing options as opposed to determining quantitative values of risk. We hope that this report stimulates renewed effort in this field and that the recommendations of the committee enable DOE-EM to progress efficiently in its remediation efforts. Milt Levenson (Chair) Rod Ewing (Vice Chair)

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Acknowledgments T he successful completion of this report would not have been possible without the cooperation and assistance of a large number of organi- zations and individuals. The committee is especially grateful to the following individuals and organizations for providing logistical support, advice, and information for this study: Department of Energy, Office of Environmental Management: Mark Gilberston, Yvette Collazo, Kurt Gerdes, Steve Schneider, Monica Regulbuto, Steve Krahn, and Daryl Haefner International Atomic Energy Agency: Zoran Drace U.S. Nuclear Regulatory Commission: David Esh and Tim McCartin Staff, contractors, and regulators at the Hanford Site: Paul Bredt, Tom Brouns, Kirk Cantrell, Nicholas Ceto III, Tom Crawford, Suzanne Dahl, Roy Gephart, Rob Gilbert, Douglas Hildebrand, Lori Huffman, Chris Kemp, Albert Kruger, Ken Krupka, Dean Kurath, Brad Mason, Matthew McCormick, Eric Pierce, Jake Reynolds, Terry Sams, John Vienna, Mike Weis, and James Wicks Staff and contractors at the Idaho National Laboratory: Scott Anderson, Rod Arbon, Ken Bateman, Bruce Begg, Barbara Beller, Steve Butterworth, Jim Cooper, Ric Craun, Keith Farmer, Ray ix

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x ACKNOWLEDGMENTS Geimer, Jan Hagers, Thomas Johnson, Bill Lloyd, Keith Lockie, Ian Milgate, Joe Nenni, Marcus Pinzel, Jay Roach, Nick Soelberg, Mark Stubblefield, Mike Swenson, Terry Todd, and Jerry Wells Staff and contractors at the Savannah River Site: Jeff Allison, Tom Cantey, Neil Davis, Ginger Dickert, Jim Folk, Eric Freed, Phil Giles, Sam Glenn, Jeff Griffen, Allen Gunter, James Marra, Sharon Marra, David Peeler, Laurie Posey, Jeff Ray, Jean Ridley, Mike Smith, Karthik Subramanian, George Wicks, Steve Wilkerson, and Cliff Winkler Speakers at the November 2009 Workshop of Waste Forms Technology and Performance (see Appendix B): Bruce Begg (ANSTO), Claude Degueldre (Paul Sheerer Institute), Fred Glasser (Univ. Aberdeen), Berndt Grambow (SUBATECH), David Kosson (Vanderbilt Univ.), Werner Lutze (Catholic Univ.), Rod McCullum (NEI), Ian Pegg (Catholic Univ.), Mark Peters (ANL), Kath Smith (ANSTO), Carl Steefel (LBNL), Sergey Stefanovsky (SIA Radon), Peter Swift (SNL), Etienne Vernaz (CEA), and Bill Weber (PNNL) The committee extends special thanks to the National Research Coun- cil staff who supported the work of this committee. Study director Daniela Strickland initiated the committee’s activities, made the arrangements for most of the site visits, and organized the international workshop on waste forms. Her early work for the committee shaped the content of the report. Shaunteé Whetstone handled the logistics for the committee’s meetings and site visits with great skill and attention to the needs of the committee. Kevin Crowley stepped in as the study director for the second half of the study period, even as he continued as the director of the Nuclear and Radiation Studies Board. Kevin provided essential guidance to the committee and worked tirelessly to assemble the final report. Kevin’s advice and questions to the committee greatly improved the content of the report, and without Kevin’s extraordinary effort, the report could not have been finished in a timely manner. This report has been reviewed in draft form by individuals chosen for their diverse perspectives and technical expertise in accordance with procedures approved by the National Research Council’s Report Review Committee. The purpose of this independent review is to provide candid and critical comments that will assist the institution in making its published report as sound as possible and to ensure that the report meets institutional standards of objectivity, evidence, and responsiveness to the study charge. The content of the review comments and draft manuscript remain confi-

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xi ACKNOWLEDGMENTS dential to protect the integrity of the deliberative process. We wish to thank the following individuals for their participation in the review of this report: David Clarke, Harvard University Allen Croff, Oak Ridge National Laboratory (retired) Patricia Culligan, Columbia University Delbert Day, Missouri University of Science and Technology William Ebert, Argonne National Laboratory Berndt Grambow, SUBATECH Lisa Klein, Rutgers University William Murphy, California State University, Chico Alexandra Navrotsky, University of California, Davis Michael Ojovan, The University of Sheffield Barry Scheetz, Pennsylvania State University Although the reviewers listed above have provided many constructive comments and suggestions, they were not asked to endorse the report’s conclusions or recommendations, nor did they see the final draft of the report before its release. The review of this report was overseen by Edwin Przybylowicz, Eastman Kodak Company (retired). Appointed by the Divi- sion on Earth and Life Studies, he was responsible for making certain that an independent examination of this report was carried out in accordance with institutional procedures and that all review comments were carefully considered. Responsibility for the final content of this report rests entirely with the authoring committee and the National Research Council.

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Contents Executive Summary 1 1 Findings and Recommendations 3 2 Background and Study Task 15 3 Waste Forms 29 4 Waste Processing and Waste Form Production 87 5 Waste Form Testing 119 6 Waste Forms and Disposal Environments 153 7 Waste Form Performance in Disposal Systems 175 8 Legal and Regulatory Factors for Waste Form Performance 197 9 Possible Opportunities in Waste Form Science and Technology 219 Appendixes A Biographical Sketches of Committee Members 243 B Workshop on Waste Form Technology and Performance 251 C Interim Report 255 D Glossary 285 E Acronyms 291 xiii

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