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Aug. 21, 1973 3,753,920 Aug. 21, 1973 L. J.ANASTASIA ETAL 3,753,920 FLUORIDE REPROCESSING OF BREEDER FUELS Original Filed Oct. 24, 1968 2 Sheets-Sheet 1 Aug. 21, 1973 L. J. ANASTASIA ET AL 3,753,920 FLUORIDE REPROCESSING OF BREEDER FUELS 2 Sheets-Sheet 3 Original Filed Oct. 24, 1968 1 1 I, £ 1 M fcl it O Lk N C* Uj vn el 3,753,920 United States Patent Office Patented Aug. 21, 1973 erate large quantities of plutonium while at the same time 3 753 920 producing power. It is necessary to reprocess spent breeder FLUORIDE REPROCESSING OF BREEDER FUELS fuel to separate the uranium and plutonium from fission Louis J. Anastasia, Midlothian, Erwin L. Carls, Glen products produced during irradiation. New processes are Ellyn, Albert A. Chilenskas, Chicago, Johan E. A. g necessary for handling the new breeder fuels. Graae, and Albert A. Jonke, Elmhurst, Norman M. A fluoride volatility process has been developed at Levitz, Bellwood, Martin J. Steindler, Park Forest, and La Verne E. Trevorrow, Glen Ellyn, HI., assignors Argonne National Laboratory for continuously reprocess- to the United States of America as represented by the ing spent breeder fuels. The object of this invention is to United States Atomic Energy Commission reprocess spent oxide fuel to produce either plutonium Continuation of abandoned application Ser. No. 770,145, 10 dioxide and uranium dioxide separately or a mixed prod- Oct. 24, 1968. This application Aug. 12, 1971, Ser. uct of 23% plutonium dioxide-uranium dioxide with a No. 171,315 fission product decontamination factor of 106 to 107. The Int. CI. COlg 43/06 decontamination factor is the ratio of the concentration of U.S. CI. 252—301.1 R 2 Claims fission products in the spent fuel to the concentration of 15 fission products in the product. The subject process is ABSTRACT OF THE DISCLOSURE based on a plant capacity of about one metric ton actinides per day, which is taken as the daily average discharge rate Spent fuel oxides are fluorinated to produce a pluto- from a 15,000 megawatt electric network. Exact equip- nium-rich stream and a uranium-rich stream. Each stream ment size and shape are influenced by heat balance and is cold trapped to remove high boiling fission products and 2o criticality considerations which vary according to the fed to a thermal decomposer, via a common feed pot which type of fuel and the extent of burnup. The process may be acts as a batch distiller. From the thermal decomposer, a better understood by reference to the following figures. plutonium-rich stream is cold trapped and sent to a con- verter and a uranium-rich stream is purified by means of BRIEF DESCRIPTION OF THE DRAWINGS various traps and distillation columns and sent to the con- verter. In the converter, the uranium-rich stream and plu- 25 FIGS. 1 and 2 represent a flowsheet of the process of tonium-rich stream are combined and converted to mixed the invention. oxides. DESCRIPTION OF THE PREFERRED EMBODIMENT This is a continuation of application S.N. 770,145, now 30 abandoned, filed Oct. 24, 1968. With reference to the figures which represent a typical flowsheet except for the broken lines at the gas coolers CONTRACTUAL ORIGIN OF THE INVENTION and cold traps which represent batch operations, each The invention described herein was made in the course piece of equipment is labelled and numbered where there of, or under, a contract with' the United States Atomic are more than one of that particular type. Table I lists the Energy Commission. 35 number, size or capacity, construction material and op- erating temperature for each piece of equipment. The BACKGROUND OF THE INVENTION reference numbers corresponding to each stream leaving This invention relates to a process for reprocessing or entering each piece of equipment are keyed to Table nuclear fuels and in particular to a nonaqueous process II, which shows the actinide and fission product distribu- for reprocessing fast breeder fuels. The next generation 40 tion for the process as well as the gas flow rate of each of nuclear reactors will be breeder reactors that will gen- stream. TABLE I Number Construction Operating Equipment item required Size or capacity material temp., ° C. Fluorinator A 1 Slab, 4" x 48" x 10' Nickel 350 Gas cooler, 1 2 Slab, 4" x 24" x 9'. do IS Cold trap, 1 — 2 Slab, 4" x 24" x 17' —do -80 Becycle pump 2 40s.c.f.m Nickel or Monel >70 3W, solid waste container — 2' diameter x 9' Stainless steel.............. Fluorinator B — 1 Slab, 4" x 30" x 10' Nickel 500-550 Gas cooler, 2 2 Slab, 4" x 24" x 5' do -10 Cold trap, 2. 2 Slab, 4'x 24" x 3lA' —do -80 Eeeycle pump 2 30s.c.f.m Nickel or Monel.-- >70 LiF traps, A & B 2 10" diameter X 3%' Nickel 300,450 20W, Solid waste container — 1 2'diameter x 9 Stainless steel.. 12W, solid waste container 1 2'diameter x 9 -do........ ........ Feed pot 2 Slab, 4" x 4'x 11.2' Nickel... 80 Thermal decomposer and fluorinator 2 Slab , 4" x 31" x W do 350-500 NaF, 1,2,3 traps 1 3" diameter x 4' do 350 31W, solid waste container — 1 2' diameter x 9' Stainless steel Cold trap, 3 - 3 4" x 24" x 3'. - Nickel —80 Recycle pump. 2 20 s.c.f.m Nickel or Monel— >70 Distillation column, 1 — 1 Column, 4" diameter x 11' Nickel i.- ~80 Distillation column, 2. ~ 1 Column, 5" diameter x 29'.. do ~80 MgFatrap '.. — 2 18" diameter x 4' do 125 Activated alumina traps, 1 Fluid Bed (F2 reaction). 2 10" diameter x T}4'— do Activated alumina trap, packed, 1 (TeFe sorption)... 2 18" diameter X iW Copper Soda-lime trap 2 10' diameter x ~6' ...do Drier, molecular sieve — 2 10" diameter x 6' do Oxygsn-hydrogen burner 1 12" diameter s 6' Stainless steel Xe-Kr compressor 2 —1 s.c.f.m .do Xe-Kr storage tank 1 3' diameter x 12.5' do Converter 1 2' x 2' x 10' Inconel 650 Sorber 1 5'diameter x 15'. — Monel 8,758,920 3 4 TABLE II— GRAMS OF ELEMENT OB COMPOUND Stream 1 3 3W 4 5 6 36 7 10>> Flow rates (s.c.f.m.) . 32.7 2.2 PuFi "123 (+3) 4,920 0 4,920 4,919.5 0.5 .03 .47 .47 UF« 1,290 (+3) 1,277 (+3) 0 1,277 (+3) 1,277 (+3) 18 1 17 17 NpFs 242 121 0 121 121 .04 .003 .037 . 037 NbFj 152 137 103 34 34 •>8.0 (-13) 7.8 (-13) 1.0 (-11) 1.0 ( -11) MoFt 8,120 7,308 0 7,308 7,280 13 1 17 17 TcF« 1,990 1,791 0 1,791 1,791 0.46 .03 0.43 0.43 RuFj 7,470 6,723 6,721 2 2 1.3 (-16) 9.4 (-18) 1.2 (-16) 1.2 (•-lfi ) SbF< 248 223 0 223 223 .094 .007 .087 .087 TeFi 1,620 0 .. 1,365 93 . IFj 882 794 0 794 794 .025 .002 .023 .023 Kr 133 0 .. 0 133 . Xe 4,680 0 .. 0 4,680 . Stream 11 12 12W 13 14 15 16 20 20W Flow rates (s.c.f.m.). 23.0 PuF« 118.0 (+3) 117.8 (+3) 0 117.8 (+3) 117.8 (+3) 76 76 1.3S (+3) 250 UF« 12.9 (+3) 12.8 (+3) 0 12.8 (+3) 12.8 (+3) 1 1 130 130 NpF« 121 119 0 119 118.7 0.3 0.3 0.32 2 NbFj 15 14 13.4 0.6 0.6 2.9 (-11) 2.9 (-11) 3.5 1 MoF« 829 827 0 827 813 14 14 14.8 ]fl TcF« 199 198 0 198 197.7 0.32 0.32 0.52 t RUFB 747 745 744.97 0.03 0.03 3.9 (-11) 3.9 (-11) 0.2 2 SbFs 25 24 0 24 24 7.2 (-4) 7.2 (-4) 25 1 TeF« 162 _ • 0 .. 159 .15 3 IFt 88 86 0 88 86 1.8 (-3) 1.8 (-3) 0.8 2 0 - - 0 0 Xe 0 . 0 0 Stream 21 22 23 24 25 26 27 28 29 Flow rates (s.c.f.m.). 23.0 2.0 FuFi 122.6: (+3) 0.8 (+3) 121. S! (+3) 12.1 (+3) 133.9 (+3) 133.4 (+3) 0.5 (+3) 121.2 (+3) 1.30 (+3) TTFe 1,289. £1 (+3) 1.29 (+3) 1,288. t) (+3) 52 1,288.6 (+3) 1.29 (+3) 1,287.3 (+3) 1.24 (+3) 1,288.6 (+3) NpF« 239.7 0.5 239.2 0.1 239.3 0.2 239.1 0.2 239.6 NbFj 34.6 34.6 .028 2.8 (-5) .028 2.8 (-5) .028 3.9 (-8) 34.6 MoFi 8,103 0 8,103 0 8,103 8 8,095 8 8,095 TcFj 1,989 0 1,989 0 1,989 2 1,987 2 1,987 RuF5 2 2 .025 2.5 (-5) .025 2.5 (-5) .025 2.6 (-8) 2.02 SbFs 247 187 60 .053 60 .0603 60 .0073 247 TeFe 1,524 0 1,524 0 1,524 2 1,522 2 1,522 IF5 880 235 645 0.35 645 .64 645 0.29 880 Kr - Stream 31 31W 32 32W 33 33W 34 34W 35 Flow rates (s.c.f.m.) .
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