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Removal of Plutonium from Uranium by Molten Metal Extraction A

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Removal of Plutonium from Uranium by Molten Metal Extraction A Ames Laboratory Technical Reports Ames Laboratory 5-1962 Removal of plutonium from uranium by molten metal extraction A. F. Voigt Iowa State University R. G. Clark Iowa State University J. G. Gonser Iowa State University D. L. Haes Iowa State University G. J. Lutz Iowa State University See next page for additional authors Follow this and additional works at: http://lib.dr.iastate.edu/ameslab_isreports Part of the Metallurgy Commons Recommended Citation Voigt, A. F.; Clark, R. G.; Gonser, J. G.; Haes, D. L.; Lutz, G. J.; and Malaby, K. L., "Removal of plutonium from uranium by molten metal extraction" (1962). Ames Laboratory Technical Reports. 49. http://lib.dr.iastate.edu/ameslab_isreports/49 This Report is brought to you for free and open access by the Ames Laboratory at Iowa State University Digital Repository. It has been accepted for inclusion in Ames Laboratory Technical Reports by an authorized administrator of Iowa State University Digital Repository. For more information, please contact [email protected]. Removal of plutonium from uranium by molten metal extraction Abstract The extraction of plutonium from molten uranium with immiscible molten metals, silver, lanthanum and cerium, has been investigated. A facility is described in which these experiments on uranium containing 0. 2% plutonium were conducted safely. The distribution coefficients and efficiency of removal from uranium were determined for silver and lanthanum at several temperatures in the range 1175-1375° C and for cerium at 1225o C. Disciplines Metallurgy Authors A. F. Voigt, R. G. Clark, J. G. Gonser, D. L. Haes, G. J. Lutz, and K. L. Malaby This report is available at Iowa State University Digital Repository: http://lib.dr.iastate.edu/ameslab_isreports/49 IS- 4 70 Chemical Separations Processes for Plutonium and Uranium (UC-10) TID 4500, December 15, 1960 UNITED STATES ATOMIC ENERGY COMMISSION Research and Development Report REMOVAL OF PLUTONIUM FROM URANIUM BY MOLTEN METAL EXTRACTION by A. F. Voigt, R. G. Clark, J. G. Gonser D. L. Haes, G. J. Lutz and K. L. Malaby ] ] ~I May, 1962 ] ] Ames Laboratory at ] Iowa State University of Science and Technology F. H. Spedding, Director Contract W -7405 eng-82 1 .. r r 2 IS-4 70 r This report is distributed according to the category Chemical Separations Processes for Plutonium and Uranium (UC-1 0) as listed in TID-4500, December 15, 1960. r Legal Notice 1 This report was prepared as an account of Government sponsored work. Neither the United States, nor the Commission, nor any person acting on behalf of the Commission: I A. Make s any warranty of representation, express or implied, with respect to the accuracy, completeness, or usefulness I o f the information contained in this report, or that the use of any information, apparatus, method, or process disclosed in this report may not infringe privately owned rights; or I B. Assum e s any liabilities with r e spe ct to the use of, o r fo r damages resulting from the us e of any informa ti o n, I a pparatus, method, or process disclos e d in this r e po rt. As used in the above, "pe rson acting on behalf of the Commission " includes any employee or contractor of the Commission, or employee of such contractor, to the extent that such employee or contractor of the Commission, or employee of such contractor prepares, disseminates, I or provide s access to, any information pursuant to his employment or contract with the Commission, or his e m _ployment with such contractor. I. I Printed m USA. Price $ . 75 Available from the Office of Technical Service s U. S. D e pa rtment of C omme rc e Washingto n 25, D . C. ] ] IS-4 70 3 ] CONTENTS ] Page ABSTRACT ••• 5 1 INTRODUCTION 6 ] EXPERIMENTAL • • 9 Apparatus •••••• 9 ] Materials • • • • • • 1 3 Uranium- Plutonium Alloy • 13 Metal Extractants 15 ] Procedure •••••• 15 Plutonium Analyses. 16 Treatment of Data ••••••. 18 ] Results ••• 19 DISCUSSION. • • 22 ] CONCLUSIONS 30 ] ACKNOWLEDGMENT 31 ] REFERENCES .•.. 32 ] ] J J J J I ] ] 5 ] IS-470 ] REMOVAL OF PLUTONIUM FROM URANIUM ] BY MOLTEN METAL EXTRACTION A. F. Voigt, R. G. Clark, J. G. Gonser, ] D. L. Haes, G. J. Lutz and K. L. Malaby ] ABSTRACT ] The extraction of plutonium from molten uranium with immiscible molten metals, silver, lanthanum and cerium, has been investigated. ] A facility is described in which these experiments on uranium containing ] 0. 2o/o plutonium were conducted safely. The distribution coefficients and efficiency of removal from uranium were determined for silver and ] lanthanum at several temperatures in the range 1175-1375° C and for ] c e r i urn at 1 2 2 5o C. In order to permit a statistical analysis of the results, 20-30 g of ] metal were used for each phase and, after cooling, the phases were J sectioned and the sections analyzed individually. It was found that the extraction into silver was accompanied by slagging reactions which J removed variable quantities of the plutonium and led to poor agreement J among runs. Hence the distribution coefficient and its temperature dependence could not be determined with much accuracy. An average J value of 14 .±. 1 was obtained for the coefficient defined on a molar basis. J J r 6 r The lanthanum and cerium extractions were much more reproducible r since slagging of plutonium is not as likely in the presence of these I more active metals. They extract much less of the plutonium, with I a distribution coefficient of 0. 4 for lanthanum and 0. 5 for cerium. Comparison is made with the results of McKenzie et al. on the [ same system but under greatly different experimental conditions. [ INTRODUCTION Very early experiments with tracer plutonium in uranium revealed I that plutonium could be removed from uranium by liquid metal I extraction. tee h n1ques.. 1 Among the systems studied was a group of metals which exhibit immiscibility with uranium in the liquid phase such I as silver, copper, rare-earth metals, etc. The early work was a survey I of a variety of systems and did not go into details on any of them. Later, a new program was initiated to make a more comprehensive I study of pyrometallurgical proce ssing with emphasis on liquid m etal I systems. In this work the distribution coefficients of plutonium and many of the fission products betwee n the uranium and various I e xtractants w e re d eterm1ne. d . 2 • 3 T h e e fficiency o f r e moval was a l so I d etermined and expressed both as a decontamination factor and as the p e rce ntage r e move d. I Silve r, cerium and lantha num were the pri n c ipa l extract a nts s tudied [ a t two l e v e ls of plutonium concentration (Table I). I I I 7 I The silver results showed a definite difference in the degree of I plutonium extraction at the two concentrations while little change was I noted in the results with rare- earth metals. Work at Chalk River on these systems was reported by McKenzie, I et a 1 • , 4, 5 at a b out t h'1s tlme.. For the uranium- silver system they 1 reported extraction coefficients which increased with increasing temperature and decreased with increasing plutonium concentration. ] Our work indicated an increasing extraction coefficient with increasing ] plutonium concentration. In the rare- earth metal e xtrac tions, thei r data and ours were in agree m e nt. ] T ah l e I ] Distribution Coefficienta D econtam1nat1on. F actor b Pu Cone. o/o 0.0018 0. 023 0.0018 0.023 ] Extractant ] Ag 2. 1 3. 2 3. 7 5. 1 ] La 0. 38 0. 33 1. 28 1. 22 C e 0.56 0. 60 1. 50 l. 58 ] aK = g Pu/ mole E xt bD. F . = g Pu/ g ori g i n a l U ] d g Pu/mole U g Pu/ g U Phase ] J J r r 8 r Our results at these lower concentrations were of sufficient interest and potential value in fuel reproc ss ing to indicate the desirability of I doing experiments at higher concentrations, closer to those of actual I fuel elements or breeding blanket materials. A comparison with the Chalk River data would be possible, which would be valuable because of [ the very different techniques employed in the experiments. [ In January 1958, first experirnents were started with a uranium- 0. 2% plutonium alloy. This plutonium concentration was twice as large [ as that in used in the Chalk River silver extractions and ten times the I highest previously used in this Laboratory. In order to allow comparisons, the same three metals were used as extractants. The first phase of this I work was concerned with the determinaticn of the time necessary to I establish equilibrium conditions for the extraction at 1225° C. Secondly, an investigation was made into the effect of temperature in the range I 122 5-1 3 7 5° C on the distribution of plutonium between uranium and the I three metals. Previous experience with the liquid metal extraction of fission I products indicated that the extracted rnaterial might n ot be homogeneously I distributed within a phase even after equilibrium had apparently been established. Therefor e , as another objective, experin1ents were designed to check this for the plutonium extractions. PlutoniUin analyses were mad e of four samples of equal size from I 1 9 1 each phase of each extraction, and the analytical results were I compared statistically to measure the degree of uniformity in a phase.
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