WO1998042035A2 - Cellule electrolytique et procede servant a desactiver une matiere radioactive - Google Patents

Cellule electrolytique et procede servant a desactiver une matiere radioactive Download PDF

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Publication number
WO1998042035A2
WO1998042035A2 PCT/US1998/005319 US9805319W WO9842035A2 WO 1998042035 A2 WO1998042035 A2 WO 1998042035A2 US 9805319 W US9805319 W US 9805319W WO 9842035 A2 WO9842035 A2 WO 9842035A2
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WO
WIPO (PCT)
Prior art keywords
conductive
beads
electrolytic cell
housing
radioactive
Prior art date
Application number
PCT/US1998/005319
Other languages
English (en)
Other versions
WO1998042035A3 (fr
Inventor
James A. Patterson
Original Assignee
Patterson James A
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Patterson James A filed Critical Patterson James A
Priority to AU69394/98A priority Critical patent/AU6939498A/en
Publication of WO1998042035A2 publication Critical patent/WO1998042035A2/fr
Publication of WO1998042035A3 publication Critical patent/WO1998042035A3/fr

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Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21B—FUSION REACTORS
    • G21B3/00—Low temperature nuclear fusion reactors, e.g. alleged cold fusion reactors
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/28—Treating solids
    • G21F9/30—Processing
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00—Energy generation of nuclear origin
    • Y02E30/10—Nuclear fusion reactors

Definitions

  • This invention relates generally to electrolytic cells, and more particularly to an electrolytic cell and method for deactivating radioactive material by electrolysis. 5
  • the utilization of palladium coated microspheres or beads as a catalytic agent for the absorption of hydrogen is taught in prior U.S. patents 4,943,355 ('355) and 5,036,031 (O31).
  • the utilization of cross linked polymer microspheres forming an inner core and having a coating of palladium and other halide forming metals thereatop exhibit significant improvements in the level of hydrogen absorption and the absorption of l o isotopes of hydrogen.
  • U.S. patent 5,494,559 discloses an improvement in the layer 15 structure of the catalytic microspheres or beads within an electrolytic cell.
  • the combination of nickel/palladium layers enhance the production of excess heat within the liquid electrolyte.
  • This invention is directed to an electrolytic cell, method and carbon matrix for deactivating radioactive metals by electrolysis in an aqueous media.
  • the electrolytic cell is directed to an electrolytic cell, method and carbon matrix for deactivating radioactive metals by electrolysis in an aqueous media.
  • a non-conductive housing having an inlet and an outlet and spaced apart first and second conductive grids positioned within the housing.
  • An ion exchange resin in the form of a plurality of preferably cross linked polystyrene-divinyl benzene beads are initially loaded with the radioactive salt and then fused at a temperature sufficiently high to decompose the salt and to form a carbon matrix. These carbonized loaded beads form a bed of conductive beads positioned within the housing between the first and second grids in electrical contact with the first grid adjacent the inlet.
  • An electric power source in a system incorporating the cell is operably connected across the first and second grids whereby electrical current flows between the grids within the aqueous media flowing through the cell.
  • Figure 1 is a schematic view of a system and electrolytic cell embodying the present invention.
  • Figure 2 is a section view of the electrolytic cell shown in Figure 1.
  • Figure 3 is a Geiger count calibration curve for determining the percentage of Uranium and Thorium salt present in lithium sulphate electrolyte.
  • This system 10 includes an electrolytic cell shown generally at numeral 12 interconnected at each end with a closed loop electrolyte circulation system.
  • the circulation system includes a constant volume pump 18 which draws a liquid electrolyte 59 from a reservoir 32 and forces the electrolyte 59 in the direction of the arrow into inlet 54 of electrolytic cell 12. After the electrolytic cell 12 is completely filled with the electrolyte 59, the electrolyte then exits an outlet 56, thereafter flows into a gas separator 26 which is provided to separate and recombine hydrogen and oxygen gas from the electrolyte 59.
  • An in-line filter 22 capable of filtering down to 1.2 microns of particle size is provided for filtration of debris within the system.
  • the heater 21 may be positioned anywhere in the closed system electrolyte flow path as the heating applied is of a steady state nature rather than only a pre-heating condition of the electrolyte, although positioning of the heater 21 is preferred to be adjacent the inlet 54 of the cell 12 for better liquid electrolyte temperature control.
  • the heating of the electrolyte external to the cell 12 is one means for triggering and enhancing the catalytic reaction within the cell 12 to produce a positive temperature differential ( ⁇ T) of the electrolyte as it flows through the cell 12.
  • ⁇ T positive temperature differential
  • Another means preferred for triggering this heat production reaction between the electrolyte 59 and a bed 35 of conductive particles 36 within the cell 12 is by the application of sufficient electric d.c. current across electrodes 15 and 16 as described herebelow.
  • Each of the end members 46 and 48 includes an inlet stopper 54 and an outlet stopper 56, respectively. Each of these stoppers 54 and 56 define an inlet and an outlet passage, respectively into and out of the interior volume, respectively, of the electrolytic cell 12.
  • These end members 46 and 48 also include a fluid chamber 58 and 60, respectively within which are mounted electrodes 15 and 16, respectively, which extend from these chambers 58 and 60 to the exterior of the electrolytic cell 12 for interconnection to a constant current-type d.c. power supply (not shown) having its negative and positive terminals connected as shown. Also positioned within the chambers 58 and 60 are thermocouples 70 and 72 for monitoring the electrolyte temperature at these points of inlet and outlet of the electrolytic cell 12.
  • a plurality of separate, packed conductive beads or particles 36 are positioned to define a bead bed 35 within housing 14 immediately adjacent and against a conductive foraminous or porous grid 38 formed of platinum and positioned transversely across the housing 14 as shown. These conductive beads 36 are described in detail herebelow.
  • a non-conducive foraminous or porous nylon mesh 40 is positioned against the other end of these conductive particles 36 so as to retain them in the position shown.
  • Adjacent the opposite surface of this non-conductive mesh 40 is a plurality of non-conductive spherical beads, or more generally particles, 42 formed of cross-linked polystyrene and having a nominal diameter of about 3.0 mm.
  • a conductive foraminous or porous grid 44 formed of platinum and positioned transversely across the housing 14 as shown.
  • non-conductive beads 42 replaces the non-conductive beads 42 with non-metallic spherical cation ion exchange polymer conductive beads preferably made of cross-linked styrene divinyl benzene having fully pre-sulfonated surfaces which have been ion exchanged with a lithium salt.
  • This preferred non-metallic conductive microbead structure will thus form a "salt bridge" between the anode 44 and the conductive particles 36, the non-conductive mesh 40 having apertures sufficiently large to permit contact between the conductive particles 36 and the conductive non-metallic microbeads.
  • the mesh size of mesh 40 is in the range of 200-500 micrometers. This preferred embodiment thus prevents melting of the sulfonated non-conductive beads 42 while reducing cell resistance during high loading and normal operation.
  • the end of the electrode 15 is in electrical contact at 66 with conductive grid 38, while electrode 16 is in electrical contact at 68 with conductive grid 44 as shown.
  • the preferred formulation for this electrolyte 59 is generally that of a conductive salt in solution with water.
  • the preferred embodiment of water is that of either light water (H 2 1 0) or heavy water and, preferably deuterium (H 2 2 0).
  • the purity of all of the electrolyte components is of utmost importance.
  • the water (H 2 1 0) and the deuterium (H 2 2 0) must have a minimum resistance of one megohm with a turbidity of less than 0.2 N.T.U. This turbidity is controlled by ultra membrane filtration.
  • the preferred salt solution is lithium sulfate (Li 2 S0 ) in a 1 -molar mixture with water and is of chemically pure quality. In general, although a lithium sulfate is preferred, other conductive salts chosen from the group containing boron, aluminum, gallium, and thallium, as well as lithium, may be utilized.
  • the preferred pH or acidity of the electrolyte is 9.0.
  • Uranium and thorium salts obtained from a depleted source used in these tests are in the form of UO 2 (NO 3 ) 2 *6H 2 O and Th(NO 3 ) *4H 2 O.
  • Ion exchange resins (cation) are loaded with a mixture of these uranium and thorium salts.
  • the uranium and thorium are converted from ionic soluble salts to insoluble oxides during the process.
  • the reactions proceeded as follows:
  • the carbon source is derived from the polymer bead. Also, reductive heating converts the uranium salt to uranium metal and uranium oxide.
  • the combined reaction containing both U and Th salts is as follows: t t t
  • This reaction converts the uranium and thorium into the metal and oxide forms in a carbon matrix.
  • carbon is the reducing agent through the reaction C + 0 2 ⁇ C0 2 , which robs the oxygen from the metal oxides.
  • Some of the metal oxides (M0 2 ) are 5 converted to M° + C0 2 .
  • This carbon matrix is used to evaluate radioactive ratios before and after a reaction.
  • This mixture was heated with an infrared lamp along with mixing to drive off all of the water present.
  • the dry sample was heated to 500°C for 30 minutes.
  • the final weight of this product was 10.211 g.
  • a sub-sample of the product was taken to measure the radioactivity.
  • the sample was counted using a Geiger-Mueller counter which employed a 24 mm 5 diameter probe.
  • the sample was placed in a well which measured 28 mm in diameter and
  • the sub-sample product measured 3500 cpm.
  • Th0 2 The potential for Th0 2 is as follows (Latimer, Id):
  • the voltage potential is sufficient to convert the reduction of all metal at the cathode.
  • U 4+ ⁇ U° + 4e " .
  • U + + 3H forms a hydride as an insoluble molecule.
  • the radioactive U and Th at the cathode is insoluble and, therefore, is the source of all radioactivity.
  • Shaw (1967) reported that a metallic hydride, such as UH 3 2+ , is an insoluble hydride which migrates to the cathode in aqueous media. The migration rate is equivalent to the charge on the cell (45 VDC).
  • the testing procedures incorporated two stages.
  • the first stage may be viewed as a loading stage during which a relatively low level current (approx. .05 amps) is introduced across the conductive members, that current facilitated by the presence of the electrolyte 59 as previously described.
  • the current level between conductive members is then incrementally increased, during which time the electrolyte temperature differential is monitored.
  • the temperature of the electrolyte 59 circulating through the electrolytic cell 12 and system 10 was fully monitored, along with temperature differential between thermocouples 70 and 72 and flow rate of the liquid electrolyte 59.
  • the electrolyte inlet temperature was monitored immediately upstream of stopper 54 to more accurately reflect temperature differential ( ⁇ T).
  • Table I represents a sample of radioactive amelioration (reduction) runs performed on the uranium and thorium loaded carbon matrix with the cell 12. Radioactive counts were taken on the samples using a Geiger-Mueller counter manufactured by Technical Associates, Model PUG-7 or Model PRS-5. The initial and final counts represent those of the bead contents present in the cell as determined under dry conditions with the Geiger-Mueller counter. This data does not include correction factors based upon difference in particle size distribution.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Plasma & Fusion (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Electrolytic Production Of Metals (AREA)

Abstract

L'invention concerne une cellule électrolytique (12) et un procédé servant à réduire le niveau de radioactivité d'une matière radioactive par électrolyse dans un milieu aqueux (59). La cellule électrolytique (12) comporte un logement (14) non conducteur équipé d'une entrée (54), d'une sortie (56) et de deux grilles conductrices (38, 44) espacées entre elles, qui sont placées à l'intérieur du logement. Plusieurs billes (36) de résine échangeuse d'ions, dont chacune a été chargée de matière radioactive, puis fondue dans un environnement réducteur à haute température, forment un lit tassé (35) de billes (36) conductrices placé à l'intérieur du logement (14) entre les grilles conductrices (38, 44), de façon à être en contact électrique avec la première grille (38) adjacente à l'entrée (54). Les noyaux sont de préférence chargés d'une forme saline de la matière radioactive, séchés et cuits à la température de décomposition du sel ou à une température supérieure, afin de transformer la matière radioactive en une forme d'oxyde métallique ou de métal pur. On connecte de façon exploitable une source d'alimentation électrique (15, 16), dans un système (10) incorporant la cellule (12), à la première et à la deuxième grille (38, 44), de sorte que le courant électrique passe entre les grilles (38, 44) et à l'intérieur du milieu aqueux de lithium (59) à travers la cellule (12).
PCT/US1998/005319 1997-03-19 1998-03-18 Cellule electrolytique et procede servant a desactiver une matiere radioactive WO1998042035A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU69394/98A AU6939498A (en) 1997-03-19 1998-03-18 Electrolytic cell and method for deactivating a radioactive material

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US3935497P 1997-03-19 1997-03-19
US60/039,354 1997-03-19

Publications (2)

Publication Number Publication Date
WO1998042035A2 true WO1998042035A2 (fr) 1998-09-24
WO1998042035A3 WO1998042035A3 (fr) 2000-01-20

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AU (1) AU6939498A (fr)
WO (1) WO1998042035A2 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2003098640A2 (fr) * 2002-05-17 2003-11-27 The State Of Oregon Acting By And Through The State Board Of Higher Education On Behalf Of Portland State University Traitement de materiaux radioactifs avec des noyaux d'isotope d'hydrogene

Citations (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US1530392A (en) * 1922-03-31 1925-03-17 Jacque C Morrell Process of making compound adsorbent catalysts
US3228849A (en) * 1959-10-29 1966-01-11 Socony Mobil Oil Co Inc Utilization of nuclear fission for chemical reactions
US3920534A (en) * 1973-11-30 1975-11-18 Mead Corp Ion exchange membrane - cathode cartridge for an electrolytic cell
US4242226A (en) * 1978-02-21 1980-12-30 Siren Matti J Filter material and a method of manufacturing and using the same
US4482641A (en) * 1983-02-28 1984-11-13 Standard Oil Company (Indiana) Metal-containing active carbon and method for making same
US4637990A (en) * 1978-08-28 1987-01-20 Torobin Leonard B Hollow porous microspheres as substrates and containers for catalysts and method of making same
WO1990013129A2 (fr) * 1989-04-10 1990-11-01 Massachusetts Institute Of Technology Appareil de fusion
US4970189A (en) * 1988-06-24 1990-11-13 Somar Corporation Porous, metal-containing carbonaceous material
WO1991006103A1 (fr) * 1989-10-16 1991-05-02 Zachariah Chacko P Dispositif de production d'elements et d'energie
US5051392A (en) * 1989-05-24 1991-09-24 Institut Francais Du Petrole Multifunctional catalyst for treating exhaust fumes from internal combustion engines, containing uranium, at least one uranium promotor and at least one precious metal, and its preparation
DE4027784A1 (de) * 1990-03-20 1992-04-30 Hora Heinrich Vervielfachung der kalten fusion mit zwischenschichten
WO1993014503A1 (fr) * 1992-01-10 1993-07-22 Chlorine Engineers Corp., Ltd. Procede de production d'energie fonde sur l'affaissement gravitationnel
US5372688A (en) * 1993-07-20 1994-12-13 Patterson; James A. System for electrolysis of liquid electrolyte
US5488023A (en) * 1994-08-12 1996-01-30 Corning Incorporated Method of making activated carbon having dispersed catalyst

Patent Citations (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US1530392A (en) * 1922-03-31 1925-03-17 Jacque C Morrell Process of making compound adsorbent catalysts
US3228849A (en) * 1959-10-29 1966-01-11 Socony Mobil Oil Co Inc Utilization of nuclear fission for chemical reactions
US3920534A (en) * 1973-11-30 1975-11-18 Mead Corp Ion exchange membrane - cathode cartridge for an electrolytic cell
US4242226A (en) * 1978-02-21 1980-12-30 Siren Matti J Filter material and a method of manufacturing and using the same
US4637990A (en) * 1978-08-28 1987-01-20 Torobin Leonard B Hollow porous microspheres as substrates and containers for catalysts and method of making same
US4482641A (en) * 1983-02-28 1984-11-13 Standard Oil Company (Indiana) Metal-containing active carbon and method for making same
US4970189A (en) * 1988-06-24 1990-11-13 Somar Corporation Porous, metal-containing carbonaceous material
WO1990013129A2 (fr) * 1989-04-10 1990-11-01 Massachusetts Institute Of Technology Appareil de fusion
US5051392A (en) * 1989-05-24 1991-09-24 Institut Francais Du Petrole Multifunctional catalyst for treating exhaust fumes from internal combustion engines, containing uranium, at least one uranium promotor and at least one precious metal, and its preparation
WO1991006103A1 (fr) * 1989-10-16 1991-05-02 Zachariah Chacko P Dispositif de production d'elements et d'energie
DE4027784A1 (de) * 1990-03-20 1992-04-30 Hora Heinrich Vervielfachung der kalten fusion mit zwischenschichten
WO1993014503A1 (fr) * 1992-01-10 1993-07-22 Chlorine Engineers Corp., Ltd. Procede de production d'energie fonde sur l'affaissement gravitationnel
US5372688A (en) * 1993-07-20 1994-12-13 Patterson; James A. System for electrolysis of liquid electrolyte
US5488023A (en) * 1994-08-12 1996-01-30 Corning Incorporated Method of making activated carbon having dispersed catalyst

Non-Patent Citations (6)

* Cited by examiner, † Cited by third party
Title
ALBAGLI et al., J. OF FUSION ENERGY, Vol. 9, No. 2, 1990, pages 133-148, XP002934944. *
CHASE et al., Principles of Radioisotope Methodology, Third Edition, 1968, BURGESS PUB. CO., MINNEAPOLIS, MINN., pages 149-152, 154, 155, 157, 162, XP002934940. *
Memo from BENNETT MILLER to DR. ROBERT W. BASS dated 09 October 1997, pages 1-10, XP002934941. *
MERRIMEN et al., "An Attempted Replication of the CETI Cold Fusion Experiment", pages 1-17, Obtained Online 5/1/97, available http://www.math.ucla.edu/-barry/CF/CETIX.ht ml, XP002934943. *
SHELTON et al., THERMOCHIMICA ACTA, Vol. 297, (1997), pages 7-15, XP002934942. *
WILLIAMS et al., NATURE, Vol. 342, 23 November 1989, pages 375-384, XP002934945. *

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2003098640A2 (fr) * 2002-05-17 2003-11-27 The State Of Oregon Acting By And Through The State Board Of Higher Education On Behalf Of Portland State University Traitement de materiaux radioactifs avec des noyaux d'isotope d'hydrogene
WO2003098640A3 (fr) * 2002-05-17 2004-08-19 Oregon State Traitement de materiaux radioactifs avec des noyaux d'isotope d'hydrogene

Also Published As

Publication number Publication date
WO1998042035A3 (fr) 2000-01-20
AU6939498A (en) 1998-10-12

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