US20040134785A1 - Advanced high-throughput electrorefiner design - Google Patents
Advanced high-throughput electrorefiner design Download PDFInfo
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- US20040134785A1 US20040134785A1 US10/339,955 US33995503A US2004134785A1 US 20040134785 A1 US20040134785 A1 US 20040134785A1 US 33995503 A US33995503 A US 33995503A US 2004134785 A1 US2004134785 A1 US 2004134785A1
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- electrorefiner
- cathode
- uranium
- anode baskets
- vessel
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- 238000013461 design Methods 0.000 title description 12
- 229910052770 Uranium Inorganic materials 0.000 claims abstract description 82
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims abstract description 75
- 229910052751 metal Inorganic materials 0.000 claims abstract description 56
- 239000002184 metal Substances 0.000 claims abstract description 56
- 239000003758 nuclear fuel Substances 0.000 claims abstract description 19
- 230000007246 mechanism Effects 0.000 claims abstract description 6
- 238000004891 communication Methods 0.000 claims abstract description 5
- 239000011824 nuclear material Substances 0.000 claims abstract description 5
- 239000003792 electrolyte Substances 0.000 claims description 8
- -1 uranium cations Chemical class 0.000 claims description 7
- 238000007790 scraping Methods 0.000 claims description 4
- 229910000831 Steel Inorganic materials 0.000 claims description 3
- 239000010959 steel Substances 0.000 claims description 3
- 239000004020 conductor Substances 0.000 claims 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims 1
- 229910052721 tungsten Inorganic materials 0.000 claims 1
- 239000010937 tungsten Substances 0.000 claims 1
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- 238000000034 method Methods 0.000 description 8
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- 238000007747 plating Methods 0.000 description 2
- 238000003752 polymerase chain reaction Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 239000002915 spent fuel radioactive waste Substances 0.000 description 2
- 229910052778 Plutonium Inorganic materials 0.000 description 1
- 241000490025 Schefflera digitata Species 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 125000002091 cationic group Chemical group 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
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- 230000008602 contraction Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 230000005496 eutectics Effects 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 229910001026 inconel Inorganic materials 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 235000015250 liver sausages Nutrition 0.000 description 1
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Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
- C25C3/00—Electrolytic production, recovery or refining of metals by electrolysis of melts
- C25C3/34—Electrolytic production, recovery or refining of metals by electrolysis of melts of metals not provided for in groups C25C3/02 - C25C3/32
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
- C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
- C25C7/02—Electrodes; Connections thereof
- C25C7/025—Electrodes; Connections thereof used in cells for the electrolysis of melts
Definitions
- Electrorefining is a metallurgical separation technique that has been used to recover uranium from fission products and other components of spent fuel from the Experimental Breeder Reactor-II (EBR-II), as well as to purify impure plutonium metal.
- the technique is well suited to this application because the separation is based on changes in oxidation state and is accomplished by the addition or removal of electrons at electrodes rather than the use of chemical oxidizing or reducing agents, which can significantly increase the volume of waste generated.
- uranium was loaded into anode baskets that rotated in a channel between cathode tubes.
- the anode assembly and the cathode tubes were submersed in a molten LiCI-KCI eutectic.
- the salt also contained 5 to 7 wt. % uranium cations.
- Uranium and the elements in the fuel that are less noble than uranium were oxidized at the anode and formed cationic species that dissolved in the molten salt. Uranium cations were then reduced at the cathode, and the reduced uranium metal deposited on the cathode surface.
- Scrapers mounted on the rotating anode basket assembly dislodged the electrodeposited uranium, which fell to the bottom of the unit where it was collected.
- FIG. 1 presents a cross-sectional rendering of the prior art high-throughput concept.
- FIG. 1 shows 12 anode baskets with attached scrapers in the unit.
- Four cathode tubes form three channels within which the anode baskets rotate.
- the uranium product is collected in a basket attached to the bottom of the outer cathode tube.
- With a 10-in. (25-cm) diameter module uranium can be removed from spent EBR-II fuel at an average rate of nearly half a kilogram per hour.
- four of these units are operated in a single process vessel.
- One of the key steps required in the opening profile is a periodic reversal of the current to remove a dense layer of uranium that builds up on the surface of the cathode and is not dislodged by the scrapers.
- next-generation high-throughput electrorefiner that is capable of treating as much as 20 metric tons of uranium per year.
- Another object of the invention is to provide an electrorefiner with a peripherally driven anode assembly, independent removal of the product collector, and electrically isolated stripper rods located between the anode baskets.
- Yet another object of the present invention is to provide a nuclear fuel electrorefiner for recovering uranium from nuclear material containing uranium, comprising a cylindrical vessel having a longitudinal axis containing at the bottom thereof, a product collector movable axially of the cylindrical vessel, at least one cathode generally circular in horizontal cross section extending axially of and radially spaced inwardly of the vessel, a plurality of generally polyhedron-shaped anode baskets extending axially of the vessel, each anode basket having at least one face aligned with a radius of the vessel and circumferentially spaced from adjacent anode baskets and concentric with respect to the cathode, mechanism outside of the vessel rotating the generally polyhedron-shaped anode baskets with respect to the cathode, and an electrical power supply in selective electrical communication with the cathode and the anode baskets for causing uranium values in the anode baskets in the presence of a molten electrolyte containing
- Still another object of the present invention is to provide a nuclear fuel electrorefiner of the type set forth in which a plurality of axially extending metal rods are spaced circumferentially about the longitudinal axis of the vessel and are electrically insulated from and positioned between at least some of the anode baskets.
- Still another object of the present invention is to provide a nuclear electrorefiner of the type set forth in which there are a plurality of concentric radially spaced apart cathodes and a plurality of anode baskets arranged in the annular space(s) or channel(s) between the cathodes.
- FIG. 1 is a cross-sectional view of a representative prior art high-throughput electrorefiner design known as the Mark V operated at ANL-West;
- FIG. 2 is a peripheral drive center removable (PCR) electrorefiner full assembly
- FIG. 3 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing an enlarged view of the top;
- FIG. 4 is a PCR electrorefiner full assembly illustrated in FIG. 2 with the well and heaters removed;
- FIG. 5 is a PCR electrorefiner full assembly illustrated in FIG. 2 with the crucible removed;
- FIG. 6 is a PCR electrorefiner full assembly illustrated in FIG. 2 with the outer cathode removed;
- FIG. 7 is a PCR electrorefiner full assembly illustrated in FIG. 2, showing the removal/insertion of the anode baskets;
- FIG. 8 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing the removal/insertion of the scraper assembly
- FIG. 9 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing a close-up of the bottom;
- FIG. 10 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing the diverter, sweeper and product collector;
- FIG. 11 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing the center removal of the product collector
- FIG. 12 is a cross-sectional view of a PCR assembly
- FIG. 13 is a cross-sectional view of the PCR assembly of FIG. 12 taken along a different radial line.
- the present invention remedies several design inadequacies of the Mark V electrorefiner.
- the PCR design of the present invention includes concentric cathode tubes as well as cathode scrapers and anode baskets in the gap or annular space or channel between the concentric cathode tubes
- the present invention is a peripheral drive device in which the center portion of the refiner is free permitting anodes, cathodes and most importantly product to be removed axially independently of each other.
- Previous designs used a central drive shaft to rotate a plate from which the anode baskets were suspended.
- the baskets although suspended from a rotating plate similar to the Mark V electrorefiner is driven by a drive motor positioned outside the vessel so as to free the interior thereof.
- This inventive design makes possible the center removal of the electrorefined uranium product, unlike the Mark V electrorefiner which requires both the anode and cathode components to be removed prior to removal of the product.
- cathode scrapers are provided, their use is reduced and in fact some cases may be obviated entirely.
- the anode baskets because of their configuration produce a higher current density close to the cathode wall and scrape uranium product deposited on the cathode into the product collector at the bottom of the unit.
- stripper mandrels rods which are electrically insulated from the anode basket(s) is also an important feature.
- uranium is principally plated onto the stripper mandrels as well as on the anode baskets, thereby reducing the amount of uranium which must be removed from the outside of the anode baskets before the uranium values inside the anode baskets are transported to the cathodes.
- Tables 1 and 2 includes calculations based on the hereinafter described invention for both one channel and two channel PCRs.
- Two channel PCRs relate to three cathodes and two annular channels of anode baskets with stripper mandrels positioned between each of the anode baskets.
- a peripheral drive center removal PCR electrorefiner 10 which has an outer vessel 11 cylindrical in design having a cylindrical wall 12 and a horizontal bottom 13 .
- the cylindrical wall 12 ends in an outwardly extending flange 14 at the top of the outer vessel 11 .
- An insulator ring 15 is positioned on top of the flange 14 and receives or carries a plate 17 which is normally Z-shaped cross section as is seen in the left hand portion of FIG. 12. Heater shields 18 are suspended from the plate 17 , and there is also provided an insulator ring 19 as seen in FIG. 12.
- a cylindrical crucible 20 is positioned inside the outer vessel 11 and has a vertically extending cylindrical wall 21 and a bottom 22 .
- the double wall nature of the crucible 20 and the outer vessel 11 are safety features.
- An annular fixture 25 sits on top of the insulating ring 19 and includes a top flange 26 and a bottom flange 27 interconnected by a vertically extending bight 28 .
- An outer ring 29 provides support for a top plate 30 and includes a gear ring 33 on the outer periphery thereof which is engaged by a peripheral drive motor 35 having an output gear 36 .
- a mounting structure 37 mounts the peripheral drive motor 35 to the fixture 25 .
- the top plate 30 has a horizontal flange 40 connected to an upstanding vertical flange 41 , the horizontal flange 40 being provided with spaced apart circular apertures 42 , spaced apart rectangular apertures 43 and spaced apart rectangular apertures 44 , the apertures 43 being wider than the apertures 44 , both having the longer dimension positioned radially of the vessel 11 .
- a slip ring 45 is mounted interior of the flange 41 and is electrically insulated therefrom and carries a plurality of horizontally extending supports from which extend a plurality of mandrel rods 50 , each of the mandrel rods 50 being electrically insulated from the horizontal flange 40 of the top plate 30 .
- each anode basket 55 is polyhedron-shaped and may be of any convenient design, such as pentahedron or hexahedron.
- the anode basket 55 is a hexahedron with the two faces extending radially of the vessel 11 being longer than the two opposed faces extending perpendicularly to the radial faces.
- each anode basket 55 includes opposed faces 55 ( a ) which are smaller in dimension than opposed faces 55 ( b ), the faces 55 ( b ) being positioned along the radius of the cylindrical vessel 11 .
- the anode baskets 55 are perforated and may be provided with screens to retain fines within the anode basket during the electrorefining process.
- Scraper assemblies 57 are positioned preferably intermediate each anode basket 55 and each mandrel rod 50 .
- the scraper assemblies 57 extend axially of the vessel 11 the length of the cathodes 60 , 65 and are standard in the art. In the inventive PCR 10 , the scraper assemblies 57 may or may not be required depending on the efficiency of the mandrel rods 50 and the anode baskets 55 scraping deposited uranium from the cathodes, as will be described.
- Cathodes 60 , 65 are supported at the bottom of the vessel 11 by means of a cathode support 70 , generally U-shaped in vertical cross section to support the outer and inner cathode 60 and 65 respectively, as best seen in FIG. 13.
- a product diverter 72 which is mounted to or depends from the cathode support 70 , the product diverter 72 having a frustoconical portion 73 and a vertical flange portion 74 which may be mounted, as illustrated in FIGS. 12 and 13 to the outer cathode 60 and/or the cathode support 70 .
- the product diverter 72 would be electrically insulated from the cathodes 60 and 65 in order to prevent a product from being deposited thereon during the electro refining process.
- the frustoconical portion 73 of the product diverter 72 is reenforced by a plurality of circumferentially spaced apart struts 76 which may be welded or otherwise fixed to either or both of the inner vessel bottom 22 and the cylindrical wall 21 .
- the product diverter 72 may also include a cylindrical pan 77 in addition to or in lieu of the bottom 22 of the crucible or inner vessel 20 .
- Ring structure 78 is internal of the vertical flange 74 and may provide support for a plurality of blade shaped sweepers 79 which may be rotatable independent of the product collector 80 which is a cylindrical container having wall 81 and a bottom 82 .
- a handle 83 extends vertically upwardly through the product collector 80 and preferably is aligned with the longitudinal axis of the PCR 10 .
- the materials from which the PCR 10 is made are well known in the art and may include any suitable metal for the inner container or crucible 20 and the outer vessel 11 , representative metals being steel, stainless steel, Inconel or other well known metals in the nuclear electrorefining art. Similarly, insulation between the various metal components of the PCR 10 are also well known and are art recognized. Although there is shown in the above figures two cathodes 60 and 65 and a plurality of circumferentially spaced anode baskets 55 between the two cathodes, it should be understood that a larger plurality of concentric cathodes and concentric anode baskets may be employed as illustrated in the prior art shown in FIG.
- cathode tubes form three channels within which the anode baskets rotate.
- rotational driving mechanism being located exterior to the outermost cathode thereby freeing the center of the PCR 10 for removal of the product collector 80 axially of the vessels.
- the present invention significantly reduces this problem by providing a plurality of axially extending metal mandrel rods 50 which may be of any suitable metal from the anodes but electrically connected to said cathodes 60 , 65 by an independent power supply so that during current reversal onto uranium metal pates onto the rods 50 . Accordingly, uranium metal when dissolved from the cathodes 60 , 65 will plate onto the mandrels 50 in lieu of the anode baskets 55 . This is important because the uranium values which plate on the rods 50 reduce or eliminate the amount of uranium metal plating on the anode baskets 55 during current reversal.
- PCR electrorefiner 10 operation of the current PCR electrorefiner 10 and the Mark V are similar. Both use the same materials of contraction, the same anode and cathode materials, the same electrolytes and operating cycles.
- the PCR 10 of the present invention provides faster throughput, easier handling and less down time and maintenance, although requiring an extra power supply to the mandrels or rod 50 connected to the cathodes 60 , 65 .
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Abstract
Description
- [0001] The United States Government has rights in this invention pursuant to Contract No. W-31-109-ENG-38 between the U.S. Department of Energy (DOE) and The University of Chicago representing Argonne National Laboratory.
- Electrorefining is a metallurgical separation technique that has been used to recover uranium from fission products and other components of spent fuel from the Experimental Breeder Reactor-II (EBR-II), as well as to purify impure plutonium metal. The technique is well suited to this application because the separation is based on changes in oxidation state and is accomplished by the addition or removal of electrons at electrodes rather than the use of chemical oxidizing or reducing agents, which can significantly increase the volume of waste generated.
- For the last six years, personnel at Argonne National Laboratory (ANL) have mounted a significant effort to increase the throughput of this process as it is applied to the treatment of spent EBR-II fuel. In that time ANL personnel have moved from a small prototype device to a working unit that was demonstrated successfully at a throughput of 150 kg uranium/month with actual spent fuel in the Fuel Cycle Facility at ANL-West. The throughput still needs to be substantially increased, however, to handle the large inventory of EBR-II blanket fuel and other spent metal fuels at DOE sites. The basic electrochemistry of the process is now well understood and optimized. Consequently, increasing the throughput has focused primarily on improving the engineering of the process.
- In the high-throughput electrorefiner design, uranium was loaded into anode baskets that rotated in a channel between cathode tubes. The anode assembly and the cathode tubes were submersed in a molten LiCI-KCI eutectic. The salt also contained 5 to 7 wt. % uranium cations. Uranium and the elements in the fuel that are less noble than uranium were oxidized at the anode and formed cationic species that dissolved in the molten salt. Uranium cations were then reduced at the cathode, and the reduced uranium metal deposited on the cathode surface. Scrapers mounted on the rotating anode basket assembly dislodged the electrodeposited uranium, which fell to the bottom of the unit where it was collected.
- The schematic of FIG. 1 presents a cross-sectional rendering of the prior art high-throughput concept. FIG. 1 shows 12 anode baskets with attached scrapers in the unit. Four cathode tubes form three channels within which the anode baskets rotate. After being scraped off the cathode tubes, the uranium product is collected in a basket attached to the bottom of the outer cathode tube. With a 10-in. (25-cm) diameter module, uranium can be removed from spent EBR-II fuel at an average rate of nearly half a kilogram per hour. In the Fuel Cycle Facility at ANL-West, four of these units are operated in a single process vessel. One of the key steps required in the opening profile is a periodic reversal of the current to remove a dense layer of uranium that builds up on the surface of the cathode and is not dislodged by the scrapers.
- Accordingly, it is an object of the present invention to provide next-generation high-throughput electrorefiner that is capable of treating as much as 20 metric tons of uranium per year.
- Another object of the invention is to provide an electrorefiner with a peripherally driven anode assembly, independent removal of the product collector, and electrically isolated stripper rods located between the anode baskets.
- Yet another object of the present invention is to provide a nuclear fuel electrorefiner for recovering uranium from nuclear material containing uranium, comprising a cylindrical vessel having a longitudinal axis containing at the bottom thereof, a product collector movable axially of the cylindrical vessel, at least one cathode generally circular in horizontal cross section extending axially of and radially spaced inwardly of the vessel, a plurality of generally polyhedron-shaped anode baskets extending axially of the vessel, each anode basket having at least one face aligned with a radius of the vessel and circumferentially spaced from adjacent anode baskets and concentric with respect to the cathode, mechanism outside of the vessel rotating the generally polyhedron-shaped anode baskets with respect to the cathode, and an electrical power supply in selective electrical communication with the cathode and the anode baskets for causing uranium values in the anode baskets in the presence of a molten electrolyte containing uranium cations to move between the anode baskets and the cathode where uranium values are reduced to uranium metal and thereafter uranium metal is transported from the cathode to the product collector axially removable from the vessel without removing either the anode baskets or the cathode.
- Still another object of the present invention is to provide a nuclear fuel electrorefiner of the type set forth in which a plurality of axially extending metal rods are spaced circumferentially about the longitudinal axis of the vessel and are electrically insulated from and positioned between at least some of the anode baskets.
- Still another object of the present invention is to provide a nuclear electrorefiner of the type set forth in which there are a plurality of concentric radially spaced apart cathodes and a plurality of anode baskets arranged in the annular space(s) or channel(s) between the cathodes.
- The invention consists of certain novel features and a combination of parts hereinafter fully described, illustrated in the accompanying drawings, and particularly pointed out in the appended claims, it being understood that various changes in the details may be made without departing from the spirit, or sacrificing any of the advantages of the present invention.
- FIG. 1 is a cross-sectional view of a representative prior art high-throughput electrorefiner design known as the Mark V operated at ANL-West;
- FIG. 2 is a peripheral drive center removable (PCR) electrorefiner full assembly;
- FIG. 3 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing an enlarged view of the top;
- FIG. 4 is a PCR electrorefiner full assembly illustrated in FIG. 2 with the well and heaters removed;
- FIG. 5 is a PCR electrorefiner full assembly illustrated in FIG. 2 with the crucible removed;
- FIG. 6 is a PCR electrorefiner full assembly illustrated in FIG. 2 with the outer cathode removed;
- FIG. 7 is a PCR electrorefiner full assembly illustrated in FIG. 2, showing the removal/insertion of the anode baskets;
- FIG. 8 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing the removal/insertion of the scraper assembly;
- FIG. 9 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing a close-up of the bottom;
- FIG. 10 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing the diverter, sweeper and product collector;
- FIG. 11 is a PCR electrorefiner full assembly illustrated in FIG. 2 showing the center removal of the product collector;
- FIG. 12 is a cross-sectional view of a PCR assembly; and
- FIG. 13 is a cross-sectional view of the PCR assembly of FIG. 12 taken along a different radial line.
- The present invention remedies several design inadequacies of the Mark V electrorefiner. Although the PCR design of the present invention includes concentric cathode tubes as well as cathode scrapers and anode baskets in the gap or annular space or channel between the concentric cathode tubes, the present invention is a peripheral drive device in which the center portion of the refiner is free permitting anodes, cathodes and most importantly product to be removed axially independently of each other. Previous designs used a central drive shaft to rotate a plate from which the anode baskets were suspended. In the present design the baskets although suspended from a rotating plate similar to the Mark V electrorefiner is driven by a drive motor positioned outside the vessel so as to free the interior thereof. This inventive design makes possible the center removal of the electrorefined uranium product, unlike the Mark V electrorefiner which requires both the anode and cathode components to be removed prior to removal of the product.
- Another important feature of the present invention is that although cathode scrapers are provided, their use is reduced and in fact some cases may be obviated entirely. In the present design, the anode baskets because of their configuration produce a higher current density close to the cathode wall and scrape uranium product deposited on the cathode into the product collector at the bottom of the unit. In addition, the inclusion of stripper mandrels rods which are electrically insulated from the anode basket(s) is also an important feature. During operation of the Mark V electrorefiner it was found that a hard uranium dentritic coating formed on the cathodes and the only way to remove it was to reverse the current to the vessel thereby electrolytically removing the uranium from the cathode while simultaneously plating the uranium values on the outside of the anode baskets. While effective in removing the hard or dense uranium dentritic coating on the cathodes, this required the outside coating of uranium on the anode baskets to be removed from the anode baskets prior to removal of uranium from the chopped fuel elements inside the anode baskets after current had been reversed once again. This entire reversal requirement slowed down the electrorefining process to a significant extent. With the use of stripper mandrels as hereinafter described, when the current is reversed, uranium is principally plated onto the stripper mandrels as well as on the anode baskets, thereby reducing the amount of uranium which must be removed from the outside of the anode baskets before the uranium values inside the anode baskets are transported to the cathodes.
- It is believed that use of the hereinafter described invention will be able to achieve a 450 kpm throughput. Tables 1 and 2 includes calculations based on the hereinafter described invention for both one channel and two channel PCRs. Two channel PCRs relate to three cathodes and two annular channels of anode baskets with stripper mandrels positioned between each of the anode baskets.
TABLE 1 Throughput calculations - Basis 1-Channel PCR stripper (25″ diameter) cathode anode mandrel Electrode Area, cm2 13406 7392 4750 sticking coefficient 0.8 N/A 0.5 deposition current density, A/cm2 0.135 0.15 0.15 stripping current density, A/cm2 0.102 0 0.287 2-Channel PCR (36″ diameter) cathode anode stripper mandrel Electrode Area, cm2 26126 19712 11260 sticking coefficient 0.8 N/A 0.5 deposition current density, A/cm2 0.178 0.15 0.15 stripping current density, A/cm2 0.107 0 0.249 -
TABLE 2 Operational Cycle and Throughput A-h I/A time/h 1-Channel PCR Deposition 500 1821.3 0.27 Rods 200 712.5 0.28 Baskets 300 11.08.8 0.27 Strip 400 1362 0.29 Wash 0.10 peak throughput = 1112 g/hr avg monthly throughput = 450 kg/mo 2-Channel PCR Deposition 500 4646 0.11 Rods 200 1689 0.12 Baskets 300 2957 0.10 Strip 400 2804 0.14 Wash 0.10 peak throughput = 2077 g/hr avg monthly throughput = 841 kg/mo - Referring now to the drawings, there is disclosed a peripheral drive center
removal PCR electrorefiner 10 which has anouter vessel 11 cylindrical in design having acylindrical wall 12 and ahorizontal bottom 13. Thecylindrical wall 12 ends in an outwardly extendingflange 14 at the top of theouter vessel 11. Aninsulator ring 15 is positioned on top of theflange 14 and receives or carries aplate 17 which is normally Z-shaped cross section as is seen in the left hand portion of FIG. 12. Heater shields 18 are suspended from theplate 17, and there is also provided aninsulator ring 19 as seen in FIG. 12. - A
cylindrical crucible 20 is positioned inside theouter vessel 11 and has a vertically extending cylindrical wall 21 and a bottom 22. The double wall nature of thecrucible 20 and theouter vessel 11 are safety features. Anannular fixture 25 sits on top of the insulatingring 19 and includes atop flange 26 and a bottom flange 27 interconnected by a vertically extendingbight 28. Anouter ring 29 provides support for atop plate 30 and includes agear ring 33 on the outer periphery thereof which is engaged by aperipheral drive motor 35 having anoutput gear 36. A mountingstructure 37 mounts theperipheral drive motor 35 to thefixture 25. - The
top plate 30 has ahorizontal flange 40 connected to an upstandingvertical flange 41, thehorizontal flange 40 being provided with spaced apartcircular apertures 42, spaced apartrectangular apertures 43 and spaced apartrectangular apertures 44, theapertures 43 being wider than theapertures 44, both having the longer dimension positioned radially of thevessel 11. - A
slip ring 45 is mounted interior of theflange 41 and is electrically insulated therefrom and carries a plurality of horizontally extending supports from which extend a plurality ofmandrel rods 50, each of themandrel rods 50 being electrically insulated from thehorizontal flange 40 of thetop plate 30. - A plurality of axially extending circumferentially spaced apart
anode baskets 55 are positioned within theapertures 43. Eachanode basket 55 as seen in FIG. 7 is polyhedron-shaped and may be of any convenient design, such as pentahedron or hexahedron. In the preferred embodiment, theanode basket 55 is a hexahedron with the two faces extending radially of thevessel 11 being longer than the two opposed faces extending perpendicularly to the radial faces. More particularly, as seen in FIG. 7, eachanode basket 55 includes opposed faces 55(a) which are smaller in dimension than opposed faces 55(b), the faces 55(b) being positioned along the radius of thecylindrical vessel 11. As is well known in the art, theanode baskets 55 are perforated and may be provided with screens to retain fines within the anode basket during the electrorefining process. -
Scraper assemblies 57 are positioned preferably intermediate eachanode basket 55 and eachmandrel rod 50. Thescraper assemblies 57 extend axially of thevessel 11 the length of thecathodes inventive PCR 10, thescraper assemblies 57 may or may not be required depending on the efficiency of themandrel rods 50 and theanode baskets 55 scraping deposited uranium from the cathodes, as will be described. There are provided two cathodes, anouter cathode 60 having a cylindrical wall 61 and aninner cathode 65 having a cylindrical wall 66.Cathodes vessel 11 by means of a cathode support 70, generally U-shaped in vertical cross section to support the outer andinner cathode - As illustrated in FIGS.8-13, there is provided a
product diverter 72 which is mounted to or depends from the cathode support 70, theproduct diverter 72 having afrustoconical portion 73 and avertical flange portion 74 which may be mounted, as illustrated in FIGS. 12 and 13 to theouter cathode 60 and/or the cathode support 70. As is known, theproduct diverter 72 would be electrically insulated from thecathodes frustoconical portion 73 of theproduct diverter 72 is reenforced by a plurality of circumferentially spaced apart struts 76 which may be welded or otherwise fixed to either or both of the inner vessel bottom 22 and the cylindrical wall 21. As best seen in FIG. 10, theproduct diverter 72 may also include acylindrical pan 77 in addition to or in lieu of the bottom 22 of the crucible orinner vessel 20. -
Ring structure 78 is internal of thevertical flange 74 and may provide support for a plurality of blade shapedsweepers 79 which may be rotatable independent of theproduct collector 80 which is a cylindricalcontainer having wall 81 and a bottom 82. Ahandle 83 extends vertically upwardly through theproduct collector 80 and preferably is aligned with the longitudinal axis of thePCR 10. - The materials from which the
PCR 10 is made are well known in the art and may include any suitable metal for the inner container orcrucible 20 and theouter vessel 11, representative metals being steel, stainless steel, Inconel or other well known metals in the nuclear electrorefining art. Similarly, insulation between the various metal components of thePCR 10 are also well known and are art recognized. Although there is shown in the above figures twocathodes anode baskets 55 between the two cathodes, it should be understood that a larger plurality of concentric cathodes and concentric anode baskets may be employed as illustrated in the prior art shown in FIG. 1, wherein four cathode tubes form three channels within which the anode baskets rotate. A similar configuration may be used in the present invention with rotational driving mechanism being located exterior to the outermost cathode thereby freeing the center of thePCR 10 for removal of theproduct collector 80 axially of the vessels. - As is well known in the art, electrical power supplies are available and when a current flows between the
anode baskets 55 and thecathodes metal mandrel rods 50 which may be of any suitable metal from the anodes but electrically connected to saidcathodes rods 50. Accordingly, uranium metal when dissolved from thecathodes mandrels 50 in lieu of theanode baskets 55. This is important because the uranium values which plate on therods 50 reduce or eliminate the amount of uranium metal plating on theanode baskets 55 during current reversal. Because in the Mark V electrorefiner, uranium metal plates onto the outside of the anode baskets during current reversal, when the current is again reversed, the uranium metal on the outside of the baskets must be removed first prior to any uranium values inside the baskets being transported via the electrolyte to the cathodes. - As seen in Tables 1 and 2, calculations show a significantly improved transfer rate throughput for the PCR electrorefiner of the present invention. While the Marl V electrorefiner has demonstrated a 150 kg/mo throughput, the PCR of the present invention is calculated to be able to move 450 kg/mo. for a second channel refiner and 840 1/mo or a two channel electrorefiner and this is a significant advantage over the current state of the art.
- In other respects, operation of the
current PCR electrorefiner 10 and the Mark V are similar. Both use the same materials of contraction, the same anode and cathode materials, the same electrolytes and operating cycles. ThePCR 10 of the present invention provides faster throughput, easier handling and less down time and maintenance, although requiring an extra power supply to the mandrels orrod 50 connected to thecathodes - While particular embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that changes, modifications and improvements may be made, for example in the processing of the materials or in the electrode and/or cell design without departing from the true spirit and scope of the invention.
Claims (35)
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US10/339,955 US20040134785A1 (en) | 2003-01-09 | 2003-01-09 | Advanced high-throughput electrorefiner design |
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US20080296151A1 (en) * | 2007-06-04 | 2008-12-04 | Jong-Hyeon Lee | Continuous electrolytic refining device for metal uranium |
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US20100084265A1 (en) * | 2008-10-08 | 2010-04-08 | Korea Atomic Energy Research Institute | Continuous electrorefining device for recovering metal uranium |
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US8746440B2 (en) | 2011-12-22 | 2014-06-10 | Ge-Hitachi Nuclear Energy Americas Llc | Continuous recovery system for electrorefiner system |
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US7097747B1 (en) * | 2003-08-05 | 2006-08-29 | Herceg Joseph E | Continuous process electrorefiner |
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US8771482B2 (en) | 2010-12-23 | 2014-07-08 | Ge-Hitachi Nuclear Energy Americas Llc | Anode shroud for off-gas capture and removal from electrolytic oxide reduction system |
US8900439B2 (en) | 2010-12-23 | 2014-12-02 | Ge-Hitachi Nuclear Energy Americas Llc | Modular cathode assemblies and methods of using the same for electrochemical reduction |
US9920443B2 (en) | 2010-12-23 | 2018-03-20 | Ge-Hitachi Nuclear Energy Americas Llc | Modular cathode assemblies and methods of using the same for electrochemical reduction |
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US8956524B2 (en) | 2010-12-23 | 2015-02-17 | Ge-Hitachi Nuclear Energy Americas Llc | Modular anode assemblies and methods of using the same for electrochemical reduction |
US8636892B2 (en) | 2010-12-23 | 2014-01-28 | Ge-Hitachi Nuclear Energy Americas Llc | Anode-cathode power distribution systems and methods of using the same for electrochemical reduction |
US8882973B2 (en) | 2011-12-22 | 2014-11-11 | Ge-Hitachi Nuclear Energy Americas Llc | Cathode power distribution system and method of using the same for power distribution |
JP2015503035A (en) * | 2011-12-22 | 2015-01-29 | ジーイー−ヒタチ・ニュークリア・エナジー・アメリカズ・エルエルシーGe−Hitachi Nuclear Energy Americas, Llc | Electrorefining system to recover refined metal from impure nuclear feedstock |
US8945354B2 (en) | 2011-12-22 | 2015-02-03 | Ge-Hitachi Nuclear Energy Americas Llc | Cathode scraper system and method of using the same for removing uranium |
KR20140093723A (en) * | 2011-12-22 | 2014-07-28 | 지이-히타치 뉴클리어 에너지 어메리카스 엘엘씨 | Electrorefiner system for recovering purified metal from impure nuclear feed material |
US8598473B2 (en) | 2011-12-22 | 2013-12-03 | Ge-Hitachi Nuclear Energy Americas Llc | Bus bar electrical feedthrough for electrorefiner system |
US9150975B2 (en) | 2011-12-22 | 2015-10-06 | Ge-Hitachi Nuclear Energy Americas Llc | Electrorefiner system for recovering purified metal from impure nuclear feed material |
KR101628588B1 (en) * | 2011-12-22 | 2016-06-08 | 지이-히타치 뉴클리어 에너지 어메리카스 엘엘씨 | Electrorefiner system for recovering purified metal from impure nuclear feed material |
US8746440B2 (en) | 2011-12-22 | 2014-06-10 | Ge-Hitachi Nuclear Energy Americas Llc | Continuous recovery system for electrorefiner system |
KR101925048B1 (en) | 2011-12-22 | 2018-12-04 | 지이-히타치 뉴클리어 에너지 어메리카스 엘엘씨 | Bus bar electrical feedthrough for electrorefiner system |
US8968547B2 (en) | 2012-04-23 | 2015-03-03 | Ge-Hitachi Nuclear Energy Americas Llc | Method for corium and used nuclear fuel stabilization processing |
US11613823B2 (en) * | 2016-07-11 | 2023-03-28 | Uchicago Argonne, Llc | Actinide and rare earth drawdown system for molten salt recycle |
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