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2071 to Form the Uranium Dioxide (UO2). This Uranium Diox 58) Field of Search US00542.1855A UnitedO States Patent 19 11 Patent Number: 5,421,855 Hayden, Jr. et al. 45 Date of Patent: Jun. 6, 1995 54 PROCESS FOR CONTINUOUS 4,552,588 11/1985 Elliott .................................. 75/84.4 PRODUCTION OF METALLIC URANUM 4,564,507 1/1986 Elliott ..................................... 423/5 AND URANUMALLOYS 4,591,382 5/1986 Elliott ... ... 75/84.1 R 4,636,250 1/1987 Elliott ....... ... 75/84.1 A (75. I nventors: HowardOw W.... Hayden,tilayden, Jr.,Jr., Oakrid 3C 5,104,095 4/1992 Elliott et al. .......................... 266/87 Tenn.; James A. Horton, Livermore, 5,164,050 11/1992 Bertaud et al. ...................... 204/1.5 S; Guy R. B. Elliott, Los Alamos, Primary Examiner-Ngoclan Mai . Mex Attorney, Agent, or Firm-Miguel A. Valdes; William C. 73) Assignee: The United States of America as Daubenspeck; William R. Moser represented by the United States STRA Department of Energy, Washington, 57 AB CT D.C. A method is described for forming metallic uranium, or a uranium alloy, from uranium oxide in a manner which (21) Appl. No.: 67,909 substantially eliminates the formation of uranium-con 22 Filed: May 27, 1993 taining wastes. A source of uranium dioxide is first 51l Int. Cl.............................................. 2 O provided, for example, by reducing uranium trioxide : s Cl. ........................................ 75% (UO3), or any other substantially stable uranium oxide, 2071 to form the uranium dioxide (UO2). This uranium diox 58) Field of Search ...................... 75/393, 399,423/s; ide is then chlorinated to form uranium tetrachloride 204/1.5 (UCl4), and the uranium tetrachloride is then reduced to d metallic uranium by reacting the uranium chloride with (56) References Cited a metal which will form the chloride of the metal. This U.S. PATENT DOCUMENTS last step may be carried out in the presence of another H857 12/1990 Haas..................................... oys metal capable offorming one or more alloys with metal 2,834,672 5/1958 Foster et al. ..... ... is/399 lic uranium to thereby lower the melting point of the 2,886,429 5/1959 Cooke et al. .......................... 75/399 reduced uranium product. The metal chloride formed 2,887,356 5/1959 Arnoff.......... ... 423/257 during the uranium tetrachloride reduction step may 3,109,731 11/1963 Knighton .............................. 75/399 then be reduced in an electrolysis cell to recover and E; 2,I Ed “2: recycle the metal back to the uranium tetrachloride 3606081 5/1975 Wy w w w was a a w w w a sa as a 423/261 reduction operation and the chlorine gas back to the 4,026,146 4/1977 Knudsen. .232 uranium dioxide chlorination operation. 4,412,861 11/1983 Kreuzmann ........................... 75/399 4,534,792 8/1985 Elliott .............................. 75/84.1 R 30 Claims, 4 Drawing Sheets VRANAM coaomi) OYulse resubgton OPERAOn Port? via ANM dowe Fees M URANUM Tatrack ease reduction Cao Molen MAenessW AYR seco- More Melesium, SSO NSS CLORASe so c cleu- ua ER. Mouen URANM /IRON ACY ANR URANun AROn AUCY U.S. Patent June 6, 1995 Sheet 1 of 4 5,421,855 PRON ONG ASOURCE OF VRANVM2OuWe RELSUCNG Ae VRANUM RAOKASE VVVA A REVSVCANGo Agen SVUCA AS ANVROgben OR CARAON TO FORM URANVM SVOKVe CAORN AWG WE URAWVUM WSVOXWE Wn A 2A W. OF MOSN. URANVUM S2ACVORANG. W. We ORESSYNCS OF CARson CAND GPONALLY CARSON MONOYOSE GAS) O FORM URAN UW EVA ACAVORVW). COLLECVNG TE U2ANAVSM VERAC AOR Abe As A SOUV) OR VGRVJW) REDUCANG TAE URANUM WERAC ORWe N E OPOY A MRSSSNCE OF A SECONV) META CASAE OF FORMVWG. A EUTECWC WJAYA METALLC. URANUM) SY REACV Ne VRAN\UM EWACAORASe WYY-A A ARA) Me WAV CAPAVE OF REUCLANGo URANUMVEWACUORADS TO mEALLC. URANVUM WVUE FORMVNG AS CALORAVye OF AE V2) MSA REOUCWG E WESULTAN We A CAVORSE N AN E ECROVNSS C6 to RORW WAGe. WRO META ANS ASO FORM CAORNS GAS RECYCUANG WIS RESVCS) METAV 3ACVCTO TAe URAN V)M SPACOR AWe RS WSVCON See AND RECYCLNG GE CAVORWE gas RACC. O AE CO2 NAYON SEP FIG. 1 U.S. Patent June 6, 1995 Sheet 2 of 4 5,421,855 URANVUM COMSOVSN) ReSUCAWAG ASSN Oyu-VyS RESUCOYN O OPE2 AON 1999 O FORM URANUM OO OC ) OY WE FESV) UC24 NAPORS CX CNUORNA. On ReSUCNG OeeRA. ON eNSAOA AGEN URAnyM.O FORM C PSRA ON SOU) OR UGRVW) UCLA URANVUM Yn TC2ACAUORV) Sis RESUCTACYN ASYN OPSAVON MOVVEN NAGYNASS VUWA LAYSR SUEC2 Mouen MAenesiuM 59.O UYSA9 CRVORWSE SO C. CEU- 2 ANER NAOUTEYN VRANUM /IRON ALOY ANER URANUM /RON AllOY FIG. 2 U.S. Patent June 6, 1995 Sheet 3 of 4 5,421,855 Tyy!—<>\/e)opQ-\op ---- 5,421,855 1. 2 It is still another object of the invention to produce PROCESS FOR CONTINUOUS PRODUCTION OF metallic uranium and/or one or more uranium-contain METALLC URANUMANDURANUMALLOYS ing alloys from uranium oxide by converting the ura nium oxide into a uranium salt which is then reacted The invention described herein arose in the course of, 5 with a metal to form the corresponding salt of that or under, Contract No. W-7405-ENG-48 between the metal while reducing the uranium salt to metallic ura United States Department of Energy and the University of California for the operation of Lawrence Livermore It is yet another object of the invention to produce National Laboratory; and in the course of, or under metallic uranium and/or one or more uranium-contain Contract No. DE-AC05-84OR21400 between the 10 ing alloys from uranium oxide by converting the ura United States Department of Energy and Martin nium oxide into a uranium chloride which is then re Marieta Energy Systems, Inc. for the operation of Oak acted with a metal to form the chloride of that metal Ridge National Laboratory. while reducing the uranium chloride to metallic ura BACKGROUND OF THE INVENTION 15 This invention relates to the production of uranium It is another object of the invention to produce metal metal and uranium-containing eutectic alloys useful in lic uranium and/or one or more uranium-containing the production of fuel for nuclear reactors. alloys from uranium oxide by converting the uranium Conventionally uranium fuel for nuclear reactors is oxide into a uranium chloride in a bath of molten ura produced from a naturally occurring isotopic mixture of 20 nium chloride and then reacting the uranium chloride 238U and 235U which is converted to the hexafluoride intermediate reactant with a metal to form the chloride usually referred to as UF6, and which has been pro of that metal while reducing the uranium chloride to cessed to form the desired isotopic ratio of the two metallic uranium. uranium hexafluorides by the well known gaseous diffu It is a further object of the invention to produce me sion (GDP) or gas centrifuge (GCP) processes and then 25 tallic uranium and/or one or more uranium-containing typically converted to uranium oxide which is then alloys from uranium oxide by converting the uranium fabricated into the desired shape, e.g., pellets, for use in oxide into a uranium chloride in a molten bath of ura fuel rods for nuclear reactors. nium chloride and then reacting the uranium chloride However, the gaseous diffusion process requires with a metal to form the chloride of that metal while large amounts of energy to carry out the isotopic sepa 30 reducing the uranium chloride to metallic uranium ration and also results in the productions of large wherein the resulting metal chloride is reducible to amounts of fluoride wastes (frequently referred to as form chlorine and recyclable metal useful, respectively, "tails'), creating an enormous disposal problem. This, in the step of chlorinating the uranium oxide and in the in turn, has led to the development of better processes step of reducing the uranium chloride, whereby the for separating uranium isotopes which are more cost 35 production of waste products contaminated by uranium effective and which generate less undesirable waste side is substantially eliminated. products. One such isotopic separation process uses It is yet a further object of the invention to produce metallic uranium, or uranium-containing alloys, as a metallic uranium and/or one or more uranium-contain starting material. ing alloys from uranium oxide by converting the ura UF6 could be used as auranium source to produce the nium oxide into a uranium chloride in a molten uranium metallic uranium (or uranium-containing metal alloy) chloride bath and then reacting the uranium chloride starting material needed for such a separation process, with lithium or an alkaline earth metal to form the cor by reducing the UF6 using a reduction process such as, responding lithium chloride or alkaline earth metal for example, the well known metallothermic reduction chloride, such as magnesium chloride, while reducing process (Ames process) by first reducing the UF6 to 45 the uranium chloride to metallic uranium. UF4, and then reducing the UF4 with metallic magne It is a still a further object of the invention to produce sium to form metallic uranium and a magnesium fluo metallic uranium and/or one or more uranium-contain ride by-product. Reduction processes such as this, how ing alloys from uranium oxide by converting the ura ever, still result in the undesirable formation of large nium oxide into a uranium chloride in a molten uranium amounts of uranium-contaminated fluoride wastes and 50 chloride bath and then reacting the uranium chloride is highly labor intensive. with lithium or an alkaline earth metal, in the presence It would, therefore, be desirable to provide a process of controlled quantities of other metals, such as iron, for the production of metallic uranium and/or uranium which form eutectic alloys with metallic uranium, to containing alloys which would be economical and re permit molten metal formation at temperatures lower sult in the production of little, if any, uranium-con 55 than the melting point of pure metallic uranium.
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