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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Electrometallurgical Techniques for DOE Spent Fuel Treatment FINAL REPORT Committee on Electrometallurgical Techniques for DOE Spent Fuel Treatment Board on Chemical Sciences and Technology Commission on Physical Sciences, Mathematics, and Applications National Research Council NATIONAL ACADEMY PRESS Washington, D.C.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report 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. Support for this project was provided by the National Academy of Sciences, the Howard Hughes Medical Foundation, the American Chemical Society, the U.S. Department of Energy, the National Institute of Standards and Technology, and the Camille and Henry Dreyfus Foundation. Any opinions, findings, conclusions, or recommendations are those of the author(s) and do not necessarily reflect the views of the organizations or agencies that provided support for this project. International Standard Book Number 0-309-07095-3 Copyright 2000 by the National Academy of Sciences. All rights reserved. Additional copies of this report are available from: Board on Chemical Sciences and Technology National Research Council 2101 Constitution Avenue, NW Washington, D.C. 20418 Printed in the United States of America
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report THE NATIONAL ACADEMIES National Academy of Sciences National Academy of Engineering Institute of Medicine National Research Council 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 Academy has a mandate that requires it to advise the federal government on scientific and technical matters. Dr. Bruce M. Alberts 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 engineers. 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 engineering programs aimed at meeting national needs, encourages education and research, and recognizes the superior achievements of engineers. Dr. William A. Wulf is president 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 Institute 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. Kenneth I. Shine 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. Bruce M. Alberts and Dr. William A. Wulf are chairman and vice chairman, respectively, of the National Research Council.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report COMMITTEE ON ELECTROMETALLURGICAL TECHNIQUES FOR DOE SPENT FUEL TREATMENT GREGORY R. CHOPPIN, Florida State University, Chair MICHAEL J. APTED, MonitorSci, Inc. PATRICIA A. BAISDEN, Lawrence Livermore National Laboratory EDITH M. FLANIGEN, UOP (retired) CHARLES L. HUSSEY, University of Mississippi FLORIAN MANSFELD, University of Southern California L. EUGENE MCNEESE, Oak Ridge National Laboratory ROBERT A. OSTERYOUNG, North Carolina State University PAUL G. SHEWMON, Ohio State University RALPH E. WHITE, University of South Carolina Staff CHRISTOPHER K. MURPHY, Study Director DOUGLAS J. RABER, Director, Board on Chemical Sciences and Technology
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report BOARD ON CHEMICAL SCIENCES AND TECHNOLOGY JOHN L. ANDERSON, Carnegie Mellon University, Co-chair LARRY E. OVERMAN, University of California at Irvine, Co-chair BARBARA J. GARRISON, Pennsylvania State University ALICE P. GAST, Stanford University LOUIS C. GLASGOW, DuPont Fluoroproducts KEITH E. GUBBINS, North Carolina State University NANCY B. JACKSON, Sandia National Laboratories JIRI JONAS, University of Illinois at Urbana-Champaign GEORGE E. KELLER II, Union Carbide Company (retired) RICHARD A. LERNER, Scripps Research Institute GREGORY A. PETSKO, Brandeis University WAYNE H. PITCHER, JR., Genencor International, Inc. KENNETH N. RAYMOND, University of California at Berkeley PAUL J. REIDER, Merck Research Laboratories LYNN F. SCHNEEMEYER, Bell Laboratories MARTIN B. SHERWIN, ChemVen Group, Inc. JEFFREY J. SIIROLA, Eastman Chemical Company CHRISTINE S. SLOANE, General Motors PETER J. STANG, University of Utah JOHN T. YATES, JR., University of Pittsburgh STEVEN W. YATES, University of Kentucky DOUGLAS J. RABER, Director RUTH MCDIARMID, Senior Program Officer CHRISTOPHER K. MURPHY, Program Officer SYBIL A. PAIGE, Administrative Associate MARIA P. JONES, Senior Project Assistant
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report COMMISSION ON PHYSICAL SCIENCES, MATHEMATICS, AND APPLICATIONS PETER M. BANKS, Veridian Corporation/ERIM International, Inc., Co-chair W. CARL LINEBERGER, University of Colorado, Co-chair WILLIAM F. BALLHAUS, JR., Lockheed Martin Corporation SHIRLEY CHIANG, University of California at Davis MARSHALL H. COHEN, California Institute of Technology RONALD G. DOUGLAS, Texas A&M University SAMUEL H. FULLER, Analog Devices, Inc. JERRY P. GOLLUB, Haverford College MICHAEL F. GOODCHILD, University of California at Santa Barbara MARTHA P. HAYNES, Cornell University WESLEY T. HUNTRESS, JR., Carnegie Institution CAROL M. JANTZEN, Savannah River Technology Center PAUL G. KAMINSKI, Technovation, Inc. KENNETH H. KELLER, University of Minnesota JOHN R. KREICK, Sanders, a Lockheed Martin Company (retired) MARSHA I. LESTER, University of Pennsylvania DUSA M. MCDUFF, State University of New York at Stony Brook JANET L. NORWOOD, Former U.S. Commissioner of Labor Statistics M. ELISABETH PATÉ-CORNELL, Stanford University NICHOLAS P. SAMIOS, Brookhaven National Laboratory ROBERT J. SPINRAD, Xerox PARC (retired) MYRON F. UMAN, Acting Executive Director
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Preface The Committee on Electrometallurgical Techniques for DOE Spent Fuel Treatment was appointed by the National Research Council in 1994 as a result of an initial request by the U.S. Department of Energy (DOE) for an independent evaluation of the technical viability of electrometallurgical processing technology proposed by Argonne National Laboratory (ANL) as a potential approach for the treatment of DOE spent nuclear fuel. The committee completes its technical evaluation with this, its tenth and final report. Evaluation of the scientific progress of ANL’s electrometallurgical program has remained at the core of the committee’s charge throughout its existence. Within this core mission, the committee has also responded to other, more focused requests by DOE to examine specific issues related to the potential use of electrometallurgical technology. This evaluation has led to ten reports covering all aspects of ANL’s electrometallurgical demonstration project. As the specific tasks undertaken by the committee have evolved over the last five years, the committee membership has evolved accordingly as the National Research Council (NRC) has enlisted the assistance of volunteers with appropriate expertise (dates of service are in parentheses), whose contributions to the work of the committee are acknowledged here: FRED BASOLO, Northwestern University, Chair (1994-1995), GREGORY R. CHOPPIN, Florida State University, Chair (1996-2000), JOHN F. AHEARNE, Duke University and Sigma Xi, The Scientific Research Society (1996-1997), MICHAEL J. APTED, MonitorSci, Inc. (1994-2000), PATRICIA A. BAISDEN, Lawrence Livermore National Laboratory (1994-2000), SOL BURSTEIN, Wisconsin Electric Power Co. (retired) (1994-1996), EDITH M. FLANIGEN, UOP (retired) (1996-2000), CHARLES L. HUSSEY, University of Mississippi (1998-2000), BERNARD KEAR, Rutgers University (1998-1999), ALFRED F. LACAMERA, ALCOA Technical Center (1994-1995), FLORIAN MANSFELD, University of Southern California (1998-2000), L. EUGENE MCNEESE, Oak Ridge National Laboratory (1994-2000), LAWRENCE J. MULLINS, Los Alamos National Laboratory (retired) (1994-1995), ROBERT A. OSTERYOUNG, North Carolina State University (1994-2000), JOHN D. SHERMAN, UOP (1996-1997),
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report PAUL G. SHEWMON, The Ohio State University (1999-2000), RALPH E. WHITE, University of South Carolina (1998-2000), JOEL D. WILLIAMS, Los Alamos National Laboratory (1996-1999), and RAYMOND G. WYMER, Oak Ridge National Laboratory (retired) (1994-1997). This study was conducted under the auspices of the NRC’s Board on Chemical Sciences and Technology with assistance provided by its staff. The committee also acknowledges this support. Gregory R. Choppin, Chair Committee on Electrometallurgical Techniques for DOE Spent Fuel Treatment
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Acknowledgment of Reviewers 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 (NRC’s) Report Review Committee. The purpose of this independent review is to provide candid and critical comments that will assist the authors and the NRC in making its published report as sound as possible and to ensure that the report meets institutional standards for objectivity, evidence, and responsiveness to the study charge. The review comments and draft manuscript remain confidential to protect the integrity of the deliberative process. We wish to thank the following individuals for their participation in the review of this report: John F. Ahearne, Duke University and Sigma Xi, The Scientific Research Society, Robert Budnitz, Future Resources Associates, Inc., Robert L. Fleischer, Union College, Harold Forsen, Bechtel Corporation, Lloyd Heldt, Michigan Technological University, J. Brent Hiskey, University of Arizona, Royce W. Murray, University of North Carolina at Chapel Hill, and Thomas Pigford, University of California at Berkeley. Although the reviewers listed above have provided many constructive comments and suggestions, they were not asked to endorse the conclusions or recommendations, nor did they see the final draft of the report before its release. The review of this report was overseen by Norman Hackerman (The Robert A. Welch Foundation), appointed by the Commission on Physical Sciences, Mathematics, and Applications, and Robert Connick (University of California at Berkeley), appointed by the Report Review Committee, who were 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 NRC.
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Electrometallurgical Techniques for DOE Spent Fuel Treatment: Final Report Contents EXECUTIVE SUMMARY 1 1 INTRODUCTION 11 2 BACKGROUND AND DEVELOPMENT OF ELECTROMETALLURGICAL TECHNOLOGY FOR THE TREATMENT OF SPENT NUCLEAR FUEL 17 3 THE ELECTROMETALLURGICAL PROCESS AT ARGONNE NATIONAL LABORATORY 25 4 WASTE STREAMS PRODUCED BY THE ELECTROMETALLURGICAL TECHNOLOGY PROCESS 45 5 POST-DEMONSTRATION ACTIVITIES 61 6 ELECTROMETALLURGICAL TECHNOLOGY DEMONSTRATION PROJECT SUCCESS CRITERIA 71 APPENDIXES A Committee Charge and Statements of Task 79 B Meeting Summary, July 21-22, 1999 85 C Meeting Summary, September 19-21, 1999 103 D Recommendations and Selected Findings and Conclusions from Previous Reports of the Committee on Electrometallurgical Techniques for DOE Spent Fuel Treatment 107 E Abbreviations and Acronyms 115
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