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United States Patent (19) [11] 3,714,324 Weech (45) Jan

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United States Patent (19) [11] 3,714,324 Weech (45) Jan United States Patent (19) [11] 3,714,324 Weech (45) Jan. 30, 1973 54 IRRADIATED FUEL RECOVERY Chemical Processing of Nuclear Fuels, F. S. Martin & SYSTEM G. L. Miles, Academic Press Inc., N.Y., 1958 pp. 105 75 Inventor: Marx E. Weech, Pico Rivera, Calif. & 08 (73) Assignee: General Electric Company Primary Examiner-Carl D. Quarforth Assistant Examiner-F. M. Gittes 22 Filed: June 18, 1968 Attorney-Ivor J. James, Jr., Samuel E. Turner, John (21) Appl. No.: 738,009 R. Duncan, Frank L. Neuhauser, Oscar B. Waddell and Melvin M. Goldenberg 52 U.S. Cl........................................ 23/341, 23/344 57 ABSTRACT (51 int. Cl. ............................................. B01d 11100 58 Field of Search......................... 23/341, 343, 344 An improved process for recovering irradiated nuclear reactor fuel material is disclosed. This process in cludes the steps of extracting uranium, plutonium and 56 References Cited neptunium from a solution of irradiated fuel, passing UNITED STATES PATENTS this stream to a reflux column, where a high saturation of uranium is maintained. Separation of uranium from 2,848,300 8/1958 Warf...................................... 23/341 plutonium and neptunium, and further decontamina 2,979,379 4/1961 Schmieding et al.................... 23/34 tion of uranium results from this high saturation. This 3,092,446 6/1963 Morgan et al.......................... 23.1341 process is simple, has a high recovery efficiency and 3,276,850 101966 Huet et al............................... 23.1341 high decontamination, uses relatively small amounts of 3,387,945 6, 1968 Boudry et al........................... 23/341 process reagents and produces a relatively small OTHER PUBLICATIONS volume of radioactive waste material. Progress in Nucl. Chem. Series III Process Chem. ed 8 Claims, 1 Drawing Figure F. R. Bruce et al. Pergamon Press, 1956, pp. 140, 141, 96-199 NRC REFLUX STREAM A CD AQUEOUS SOLUTION STRIP EVAPORATED WATER ORGANIC WASTE 2 o s 43 FR 2 REFLUX AQUEOUS 2 picSt is to PRODUCT RRADAD d o FUEL SOLUTION - C d O Ud g Ud X c 2 d 9 RECYCLE f/ 5 - - - - - CONCENTRATED Z URANUM CONDENSAE oRGANIC / SOWENT ReCYCLE URANUM SOLUTION URANIUM PRODUCT ORGANC SOWENT AQUEOUS PLUTONIUM. 33 35 WASTE NEPTUNUM PRODUCT 3,714,324 1 2 IRRADIATED FUEL RECOVERY SYSTEM fore, it is highly desirable that the irradiated fuel material be reprocessed to recover and separate these BACKGROUND OF THE INVENTION materials for reuse. The fuel and fertile materials Nuclear chain fission reactions and the reactors in separated for reuse must be sufficiently free of highly which they take place are now well known. A typical radioactive fission products to permit direct handling. nuclear reactor includes a chain reacting assembly or Fission product separation or "decontamination" suffi core made up of nuclear fuel material contained in fuel cient to reduce the original radioactivity to on the elements. The fuel material is generally encased in a order of 10 to 10 of its original value is required. A corrosion resistant heat conductive shell or cladding. "decontamination factor" of 10, for example, in The reactor core, made up of a plurality of these ele 10 dicates that the original radioactivity has been reduced ments in spaced relationship, is enclosed in a container by a factor of 10 in the decontamination process, through which the reactor coolant flows. As the coo One currently utilized irradiated fuel reprocessing lant passes between the spaced fuel elements, it is system has been termed the "Purex' process. This heated by thermal energy released during the fission process is currently in use in the chemical processing of reaction. The heated coolant then leaves the reactor, 15 fuel from plutonium production reactors. The Purex the heat energy is used to perform useful work such as process utilizes an organic solvent consisting of tributyl by driving a turbine, and the now-cooled coolant is phosphate diluted with kerosene to extract the uranium recycled back to the reactor. and plutonium selectively from a nitric acid solution of The nuclear fuel material contains fissionable atoms, 20 irradiated fuel. The process uses nitric acid as a "- such as U-233, U-235, Pu-239 and Pu-241. The fuel salting' agent in that moderate concentrations cause may be in elemental or compound form. When the the uranium and plutonium to extract into the organic nucleus of such an atom absorbs a neutron, a nuclear solvent while lower concentrations permit the elements fission frequently occurs. This produces on the average to return to the aqueous phase. The Purex process uses two fission product atoms of lower atomic weight, 25 two or three separate cycles of such extraction and several high energy neutrons and a large amount of stripping on the uranium and plutonium, each cycle kinetic energy. The kinetic energy of the fission consisting of a transfer of the uranium and/or plutoni products and fission neutrons is quickly dissipated, um, from the aqueous phase into the organic phase and producing heat. So long as at least one neutron from back into an aqueous phase. each fission event induces a subsequent fission event, 30 The Purex process has a number of inherent disad the fission reaction is self-sustaining. The fissionable vantages. There is a substantial amount of duplicate atoms are thus gradually consumed. Some of the fission equipment in view of the two or three complete solvent products produced are strong neutron absorbers extraction cycles required to produce sufficiently (neutron poisons) which absorb neutrons which would decontaminated uranium and plutonium products. otherwise contribute to the chain reaction. The fission 35 There is produced a large volume of radioactive waste reaction, therefore, tends to decrease and cannot be materials, due to the necessity of treating the organic maintained indefinitely on a given level. solvent with various chemical reagents to remove In some nuclear reactors, fertile materials such as U degradation products before the solvent is recycled. 238 may be included in the fuel elements in addition to This organic solvent degradation becomes quite rapid the fissionable material. During the fission reaction, the 40 fertile material, e.g., U-238, is irradiated with neutrons in the radiation field created by the fission products which convert a part of the U-238 to the fissionable and it adversely affects processing capabilities. Large isotope, Pu-239. The concentration of Pu-239 in the quantities of heat are consumed in liquid evaporation fuel gradually rises with irradiation and reaches an which is required in the concentration of streams equilibrium value. The Pu-239 atoms fission similarly 45 between the several solvent extraction cycles. to the original U-235 fuel, thus contributing to the The separation of uranium from plutonium in the maintenance of the chain reaction. Purex process is accomplished by reducing the valence Except in the breeder-converter type of reactor, the state of plutonium from four to three, using chemical quantity of fissionable material created by fertile atom reductants such as ferrous iron with a stabilizing agent conversion is always less than the rate at which the 50 such as sulfamic iron. The use of these reductants and original fissionable atom quantity is consumed. Ulti stabilizing reagents are disadvantageous due to the cost mately, the operating power level of the reactor of the chemicals and the fact that these reagents in decreases to the point at which the reactor must be shut crease the waste volume. Costs for storage and long down for refueling. At least a suitable fraction of the ir term surveillance of radioactive wastes are very high. radiated fuel assemblies are removed and replaced with 55 Another solvent extraction process for irradiated new fuel having the desired concentration of fissiona fuel reprocessing is termed the Redox process. The ble atoms and no fission product neutron poisons. The Redox process uses a non-volatile salting agent and a reactivity of the refueled core is thus increased to the volatile solvent, in contrast to the non-volatile solvent extent necessary so that the desired power level can be and volatile salting agent used in the Purex process. In maintained. 60 the Redox process, a nitric acid solution is irradiated The irradiated reactor fuel removed from the reactor fuel is extracted with methylisobutyl ketone as the or contains a valuable quantity of the original fissionable ganic solvent. This solvent extracts the plutonium and material. In addition, the irradiated fuel contains a sig uranium, leaving an aqueous solution of the fission nificant quantity of fertile material, and of fissionable products. An aqueous solution of aluminum nitrate is material converted from fertile material. In addition, 65 used as the salting agent. Plutonium is separated from certain fission product and/or transuranic isotopes of the organic phase into an aqueous phase and uranium is considerable value may be contained in the fuel. There extracted from the organic phase with dilute nitric acid. 3,714,324 3 4. Both the uranium and plutonium containing streams acid stream enters the middle of the reflux column to are subjected to second cycles of solvent extraction to maintain the acid concentration at a value permitting improve separation and decontamination. effective extraction of uranium in the lower portion of Although solvent recovery in the Redox process is the reflux column while plutonium and neptunium are simplified by its volatile nature, substantial volumes of 5 not extracted. The uranium product stream exiting the waste are created in the form of solutions of the salting reflux column enters a third multi-stage extraction con agent which is not recovered for reuse. The equipment tactor where the uranium is stripped by an aqueous is extensive and complex since the desired plutonium stream. Part of the aqueous stream from this contactor, and uranium product decontamination factors are containing a high concentration of uranium, is returned achieved only through three solvent extraction 10 as the reflux stream to the upper portion of the reflux stripping cycles, with final product cleanup through ion column.
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