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Stable Isotope Separation in Calutrons

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Stable Isotope Separation in Calutrons Printed ill tho llnitzd Statss ot 4mcm 4vailsble frurii Nations' Technical Information Service U S :3ep?rtmelli uf Commerce 5285 Port 4oyal Cosd Spririizflald Viryinis 22161 NTlS ptwiodes P~III~~Copy ,498, Microfiche P,C1 I his rcpoti \*!is prspxed as an account of >,dSi-k sponsored by a3 agsncy of the United Sraies Governr;,ent. Neither thc !J nited Skiics i<n.~cti $IK~: nor any agency th2reof. no? any of thzir employoes, (ciakc?.Aijy ivarranty, express or irripiled, or assunias any legal liability or responsibility for ihe accuracy. compleienass, or usefulness of any inforriraiton. ;p ius, product, or process disclosed, or represents that its usewould not infr privately o-v?d ilghts Rcferencc herein to ai-y specific commercial product, process, or service by trade nziile, Zi'adei*lark, manufacturer, or otherwise, does not necsssarily constitute or imply its enduisemcat, recorn,n faVOiii-,g by ille United States(;ovc;riiiie!ii 01- any Zgency thereof Th opinions of auiihols cxp:essed here:!: d~ ~iui neccssarily statc or refisc?!host of the United Sta?ezGovernmer:?or any ngcncy therccf. ____ ___________... ..... .____ ORNL/TM-10356 OPERATIONS DIVISION STABLE ISOTOPE SEPARATION IN CALUTRONS: FORTY YEARS OF PRODUCTION AND DISTRIBUTION W. A. Bell J. G. Tracy Date Published: November 1987 Prepared by the OAK RIDGE NATIONAL LABORATORY Oak Ridge, Tennessee 37831 operated by MARTIN MARIETTA ENERGY SYSTEMS, INC. for the U.S. DEPARTMENT OF ENERGY under Contract No. DE-AC05-840R21400 iti CONTENTS Page ACKNOWLEDGMENTS ................................................. iv I. INTRODUCTION .............................................. 1 11. PROGRAM EVOLUTION ......................................... 1 111. RESEARCH AND DEVELOPMENT .................................. 5 IV. CHEMISTRY ................................................. 8 V. PRODUCTION ................................................ 11 VI- DISTRIBUTION BY SALES ..................................... 13 VII. EFFECT OF' PRICING PRACTICES ON INVENTORY MAINTENANCE ...... 15 REFEKENCES ..................................................... 19 TABLES AND FIGURES .............................................. 20 APPENDIX A: Table A-2. Prices of separated isotopes (1954 vs 1984) ................................... 84 UPENDIX B: Publications .................................... 92 APPENDIX C: Patents .......................................... 104 APPENDIX D: Average sales per year ........................... 106 iv ACKNOWLEDGmNTS The compilers of this report wish to recognize the dedication and the accomplishments of all those who have participated in the program. It has been and continues to be a unified team effort, providing to the world a very unique and valuable commodity. Special thanks are extended to Ramona Mayfield for the time, effort, and dedication expended in the preparation of this manuscript. V ABSTRACT The stable isotope separation program, established in 1945, has operated continually to provide enriched stable isotopes and selected radioactive isotopes, including the actinides, for use in research, medicine, and industrial applications. This report summarizes the first forty years of effort in the production and distribution of stable isotopes. Evolution of the program along with the research and development, chemical processing, and production efforts are high- lighted. A total of 3.86 million separator hours has been utilized to separate 235 isotopes of 56 elements. Relative effort expended toward processing each of these elements is shown. Collection rates (mg/separator h), which vary by a factor of 20,000 from the highest to the lowest (205Tl to 46Ca), and the attainable isotopic purity for each isotope are presented. Policies related to isotope pricing, isotope distribution, and support for the enrichment program are discussed. Changes in government funding, coupled with large variations in sales revenue, have resulted in 7-fold pertubations in production levels. I. INTRODUCTION The program to separate stable isotopes using electromagnetic equip- ment was formulated late in 1945 by the Manhattan Engineering District and its contractor, Tennessee Eastman Corporation. This outgrowth of the wartime separation of 235U was intended to provide many unique materials to government laboratories. Initial studies planned for those new materials primarily involved nuclear cross-section measurements, but program initiators also foresaw the eventual extension of government- sponsored research into broader fields. As the potential value of separated isotopes to the private sectors of industry and medicine soon becaime apparent, the program objective was expanded to inelude the world- wide distribution of enriched materials by both sales and loan programs. Forty years of efforts in the production and distribution of stable isotopes are summarized briefly in this report. Neither the actinide nor the special high-purity separations are included; their importance warrants coverage in a separate report of this type. 11- PROGRAM EVOLUTION The first samples separated (63Cu and 65Cu) were allocated by the Manhattan District for irradiation in the pile of Clinton Laboratories, now Oak Ridge National Laboratory (ORNL). From this irradiation, the first positive assignment of the 2.6-h halE-life nickel isotope to mass number 65 was made. The early years of the isotope separations program have been sum- marized by other authors. 2-5 Some delved into specific problems ; all stressed productivity and the expanding distribution of the separated products. Eventually, the monopoly on the usage of these isotopes by government laboratories began to be challenged by universities and industrial organizations liaving government contracts. What had been an in-house production-and-use system was to become more complicated. By that time, Union Carbide Corporation (UCC) had replaced Tennessee Eastman Corporation and the Atomic Energy Commission (AEC) had been formed e 1 2 On December 26, 1947, 15 requests for loans O€ isotopes to tion-NEC institutions and organizations were first approved and allocations were made by representatives from two organizations: Atomic Energy Commission (AEC) and Union Carbide Corporation (UCC). Formal O~~C?KS from the MAC-approved users were to be submitted to UCC for pro- cessing. Specified applications of the approved isotopes were (1) cyclotron bombardment and (2) hyperfine structure studies In January 1948, the 15 approved distributions to non-AEC users made. Recipients were California Institute of Technology, 6Lti and 7Li; University of Chicago, 6Li and 7J.,i; Yale University, 29Si; General Electric, 54Fe; University of Wisconsin, 64Ni, 67Zn, and 204Pb; Ohio State [Jniversity, 7oGe, 74Se, 76Se, 92M0, 94M1,, and 98M~. Unapproved requests from non-AEG organizations 00. January 31, 1948, totaled 14. The MAC transfer charges, plus the nominal charge of $50 per ship- ment to non-AEC users of stable isotopes, totaled $70,000 on December 31, 1951, averaging -$l0,000 per year. Approximately two- thirds of this sum was derived from charges made against transfers of material within the AEC. The fees were charged to defray clerical and shipping costs only. All fees received in 1952 totaled $13,650. By March 31, 1954, total. shipments had reached 2034, 57.1% intra-AEC and 42.9% to non-AEC users. Of the shipments to non-AEC users, 760 went to universittes, wtth only 112 (5.5% of total) going to industrial- type users. In the latter half of 1954, isotopes were first shipped (sold on full-cost recovery basis) to foreign users. In that 6-month interval, Io8Cd, 11*Cd9 69Ga, and 58Ni went to Centre Nationale de la Recherche Scientifiqne; Ih2Nd, 14'+Nd, 149Sm, 150Srn, and 15L+Smwent to Atomic Energy of Canada; and 128Te went to Milan Polytechnic College. In the next 6 months, isotopes went to the Federal Republic of Germany, the University of South Africa, and the Joint Establishment for Nuclear Energy Research. No domestic user could buy isotopes at any price; however, if a loan was lost, the domestic customer was charged the established sales price. In the first half of 1956, the AEC approved the domestic sa?es of electromagnetically separated stable isotopes, Allocation by the AEC 3 was no longer necessary, al1d arrangements for purchase or loans were now made directly with the Stable Isotope Research and Production Division of UCC. The purchase of isotopes by the domestic user was to be encouraged, but "rare and expensive" isotopes would still be loaned (to domestic users only) provided they would not be diluted or con- taminated in any manner. Listed "for sale only" were the more abun- dant isotopes of B, Ba, Cd, Cr, Fe, €If, Li, Nd, Ni, Pb, Sn, and Ti bearing specified enrichment. No loans were made during a 3-month transition period implementing the new sales policy. Total shipments reached 3232 on May 20, 1956. In the next 6-month period, 312 ship- ments were made; the ratio of sales to loans was 252/60. Government bodies responsible for direction and management of the isotopes program at Oak Kidge were, at first, the Manhattan Engineering District, followed by the Atomic Energy Commission, the Energy Research and Development Administration (ERDA), and currently the Department of Energy (DOE). Contractors responsible for operating the program as outlined by governmental regulations were Tennessee Eastman Corporation, Union Carbide Corporation, and Martin Marietta Energy Systems, Inc. Under Tennessee Eastman and early Union Carbide manage- ment, immediate stable isotope supervision
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