NUCLEAR SCIENCE SERIES

NAS-NS-3118

Radiochemical Techniques

ULTRAFAST CHEMICAL SEPARATIONS

by

Krishnaswamy Rengan

Department of Chemistry

Eastern Michigan University

Ypsilanti, Michigan 48197

and

Richard A. Meyer

Office of High Energy and Nuclear Physics

ER-23, U.S. Department of Energy

Washington, D.C. 20585

and

Nuclear Chemistry Division

Lawrence Livermore National Laboratory

Prepared for the

Committee on Nuclear and Radiochemistry

Board on Chemical Sciences and Technology

Commission on Physical Sciences, Mathematics, and Applications

National Research Council

National Academy Press
Washington, D.C.
1993



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ULTRAFAST CHEMICAL SEPARATIONS NUCLEAR SCIENCE SERIES NAS-NS-3118 Radiochemical Techniques ULTRAFAST CHEMICAL SEPARATIONS by Krishnaswamy Rengan Department of Chemistry Eastern Michigan University Ypsilanti, Michigan 48197 and Richard A. Meyer Office of High Energy and Nuclear Physics ER-23, U.S. Department of Energy Washington, D.C. 20585 and Nuclear Chemistry Division Lawrence Livermore National Laboratory Prepared for the Committee on Nuclear and Radiochemistry Board on Chemical Sciences and Technology Commission on Physical Sciences, Mathematics, and Applications National Research Council National Academy Press Washington, D.C. 1993

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ULTRAFAST CHEMICAL SEPARATIONS 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 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 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. Robert M. White 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 Alberts and Dr. Robert M. White are chairman and vice chairman, respectively, of the National Research Council. Support for this project was provided by the U.S. Department of Energy under Grant No. DE-FG05-89ER14032 and by Lawrence Livermore National Laboratory under Contract W-7405-Eng-48. Available from Board on Chemical Sciences and Technology National Research Council 2101 Constitution Avenue, NW Washington, DC 20418 Printed in the United States of America

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ULTRAFAST CHEMICAL SEPARATIONS COMMITTEE ON NUCLEAR AND RADIOCHEMISTRY RICHARD L. HAHN, Brookhaven National Laboratory, Chair JOSEPH R. PETERSON, University of Tennessee, Vice Chair FRED BASOLO, Northwestern University WILLIAM C. ECKELMAN, The Bristol-Myers Squibb Pharmaceutical Research Institute JOHN M. MATUSZEK, New York State Health Department ALICE C. MIGNEREY, University of Maryland HEINO NITSCHE, Lawrence Berkeley Laboratory J. KENNETH POGGENENBURG, Hybritech, Inc. IVOR L. PREISS, Rensselaer Polytechnic Institute JERRY B. WILHELMY, Los Alamos National Laboratory STEVEN W. YATES, University of Kentucky PEGGY J. POSEY, Staff Officer Monograph Coordinators J. KENNETH POGGENENBURG, Hybritech, Inc. STEVEN W. YATES, University of Kentucky BOARD ON CHEMICAL SCIENCES AND TECHNOLOGY PETER B. DERVAN, California Institute of Technology, Co-Chair EDWIN P. PRZYBYLOWICZ, Eastman Kodak Company, Co-Chair PAUL S. ANDERSON, Merck Sharp & Dohme Research Laboratories ALEXIS T. BELL, University of California, Berkeley DAVID C. BONNER, Premix, Inc. PHILIP H. BRODSKY, Monsanto Company GREGORY R. CHOPPIN, Florida State University FRED P. CORSON, Dow Chemical Company MICHAEL P. DOYLE, Trinity University BERTRAM O. FRASER-REID, Duke University JOSEPH G. GORDON, IBM Corporation L. LOUIS HEGEDUS, W.R. Grace & Company KENDALL N. HOUK, University of California, Los Angeles DOUGLAS A. LAUFFENBERGER, University of Illinois at Urbana-Champaign MARSHA I. LESTER, University of Pennsylvania W. CARL LINEBERGER, University of Colorado, Boulder ROYCE W. MURRAY, University of North Carolina JEANNE E. PEMBERTON, University of Arizona W. HARMON RAY, University of Wisconsin JOANNE STUBBE, Massachusetts Institute of Technology LARRY F. THOMPSON, AT&T Bell Laboratories DOUGLAS J. RABER, Director PEGGY J. POSEY, Program Officer SCOTT WEIDMAN, Program Officer TAMAE M. WONG, Program Officer SYBIL A. PAIGE, Administrative Associate MARIA P. JONES, Administrative Secretary KASANDRA D. GOWEN, Senior Secretary TAÑA L. SPENCER, Secretary

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ULTRAFAST CHEMICAL SEPARATIONS COMMISSION ON PHYSICAL SCIENCES, MATHEMATICS, AND APPLICATIONS RICHARD N. ZARE, Stanford University, Chair RICHARD S. NICHOLSON, American Association for the Advancement of Science, Vice Chair STEPHEN L. ADLER, The Institute for Advanced Study JOHN A. ARMSTRONG, IBM Corporation (Ret.) SYLVIA T. CEYER, Massachusetts Institute of Technology AVNER FRIEDMAN, University of Minnesota SUSAN L. GRAHAM, University of California, Berkeley ROBERT J. HERMANN, United Technologies Corporation HANS MARK, The University of Texas at Austin CLAIRE E. MAX, Lawrence Livermore Laboratory CHRISTOPHER F. MCKEE, University of California, Berkeley JAMES W. MITCHELL, AT&T Bell Laboratories JEROME SACKS, National Institute of Statistical Sciences A. RICHARD SEEBASS III, University of Colorado CHARLES P. SLICHTER, University of Illinois at Urbana-Champaign ALVIN W. TRIVELPIECE, Oak Ridge National Laboratory NORMAN METZGER, Executive Director

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ULTRAFAST CHEMICAL SEPARATIONS FOREWORD The Committee on Nuclear and Radiochemistry is one of a number of committees working under the Board on Chemical Sciences and Technology of the Commission on Physical Sciences, Mathematics, and Applications of the National Research Council. Its members are drawn from academic, industrial, and government laboratories and represent the areas of nuclear chemistry, radiochemistry, and nuclear medicine. The committee has concerned itself with those areas of nuclear science that involve the chemist, such as the collection and distribution of radiochemical procedures, specialized techniques and instrumentation, the place of nuclear and radiochemistry in college and university programs, the training of nuclear and radiochemists, radiochemistry in environmental science, and radionuclides in nuclear medicine. A major interest of the committee is the publication of the Nuclear Science Series monographs on Radiochemistry, Radiochemical Techniques, and Nuclear Medicine. The committee has endeavored to present monographs that will be of maximum use to the working scientist. Each monograph presents pertinent information required for radiochemical work with an individual element or with a specialized technique or with the use of radionuclides in nuclear medicine. Experts on the various subjects have been recruited to write the monographs. The U.S. Department of Energy sponsors the printing of the series. Support for the present monograph also was provided by Lawrence Livermore National Laboratory. This monograph is an up-to-date review and compilation of radiochemical separations that must be accomplished in a very short time. The present monograph, one of the series on Radiochemical Techniques, is published as part of our continuing effort to update, revise, and expand the previously published monographs to keep them current and relevant. Richard L. Hahn, Chair Committee on Nuclear and Radiochemistry

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ULTRAFAST CHEMICAL SEPARATIONS PREFACE A monograph entitled Rapid Radiochemical Procedures by Kusaka and Meinke was published in 1961. In the three decades since its publication, the requirement to study nuclides with half-lives in the sub-seconds range has led to entirely new approaches to separation procedures—new techniques, concepts, and automation have evolved. In the present monograph, Ultrafast Chemical Separations, we review these developments and provide a review of present-day separation techniques. The monograph is presented in two parts. In Part I, we review the general techniques used in radiochemical separations, and we discuss, with examples, autobatch and continuous separation techniques used for nuclides with very short half-lives. In Part II, we present a collection of procedures, arranged according to elements. The elements for which procedures are included are shown in a periodic table format at the beginning of Part II. Each entry also shows the time of separation for the fastest procedure for that element. We have received generous assistance from a number of individuals during the preparation of this monograph. We are grateful to Professors Herrmann, Denschlag, and Trautmann, as well as the rest of the nuclear chemists at the University of Mainz, for reviewing the monograph and for providing a number of valuable suggestions. We are also thankful to Dr. Gehrke of the Idaho National Engineering Laboratory and Professor Skarnemark of Chalmers University for providing prints of figures and giving permission to reproduce them. We are indebted to the staff of the Technical Information Division of the Lawrence Livermore National Laboratory (LLNL) for their assistance in searching the literature and to Yves Dardenne, a graduate of Eastern Michigan University. Help was provided by a large number of individuals in typing, preparation of figures, and technical editing. We would like to recognize the contribution of Debbie Wilson, Becky Gonzalez, Sara Smith, and Pat Parks in this endeavor. We are grateful for the excellent technical editing done by Coralyn K. McGregor and Jane Olivera of LLNL. One of us (KR) would like to thank the Graduate School at Eastern Michigan University for the support provided through the Faculty Research Fellowship Program and the Chemistry Department of Eastern Michigan University. Last, but hardly least, we wish to thank the LLNL Nuclear Chemistry Division leaders and Dr. Christopher Gatrousis, associate director for chemistry and materials science at LLNL, whose efforts initiated the development of this book. One of us (RAM) is indebted to Professor Oliver Robert Brown, provost, Montgomery College (Takoma Park), for providing the environs for the final completion of this book. This monograph is dedicated to three American pioneers in nuclear and radiochemistry: Dr. Peter Cooper Stevenson (deceased) of LLNL, Professor (emeritus) Arthur C. Wahl of Washington University, and Professor W. Wayne Meinke (formerly of the University of Michigan and a past chairman of the Subcommittee on Radiochemistry, National Academy of Sciences). Krishnaswamy Rengan Ypsilanti, Michigan Richard A. Meyer Germantown, Maryland December 1992

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