EP0112771B1 - Procédé de conditionnement de déchets constitués par des particules métalliques radioactives telles que les fines de dissolution des éléments combustibles irradiés - Google Patents

Procédé de conditionnement de déchets constitués par des particules métalliques radioactives telles que les fines de dissolution des éléments combustibles irradiés Download PDF

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Publication number
EP0112771B1
EP0112771B1 EP83402466A EP83402466A EP0112771B1 EP 0112771 B1 EP0112771 B1 EP 0112771B1 EP 83402466 A EP83402466 A EP 83402466A EP 83402466 A EP83402466 A EP 83402466A EP 0112771 B1 EP0112771 B1 EP 0112771B1
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EP
European Patent Office
Prior art keywords
process according
alloy
metal
tube
powder
Prior art date
Legal status (The legal status 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 status listed.)
Expired
Application number
EP83402466A
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German (de)
English (en)
French (fr)
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EP0112771A1 (fr
Inventor
Roger Bonniaud
Antoine Jouan
Yves Hery
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Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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Commissariat a lEnergie Atomique CEA
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    • 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
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • 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
    • G21F9/008—Apparatus specially adapted for mixing or disposing radioactively contamined material

Definitions

  • the subject of the present invention is a process for conditioning waste constituted by radioactive metallic particles such as the fines obtained during the dissolution of the irradiated fuel elements and the dust obtained during the cutting and / or mechanical stripping operations of the irradiated fuel elements. .
  • dissolving fines consist essentially of ruthenium, rhodium, palladium, molybdenum and, to a lesser extent, zirconium, niobium, technetium, uranium and plutonium.
  • dissolving fines consist essentially of ruthenium, rhodium, palladium, molybdenum and, to a lesser extent, zirconium, niobium, technetium, uranium and plutonium.
  • the cladding is made of Zircalloy and the quantities of shearing fines produced are generally of the order of 3 kg / t; in the case of fuel elements of fast neutron reactors for which the cladding is generally made of stainless steel, these shear fines represent approximately 1 kg / t of uranium.
  • radioactive waste consisting of oxide or glass particles obtained from solu tions, using metal matrices as described in patents FR-A 2 387 093 and GB-A 1 446016.
  • the products obtained by these processes have a heterogeneous structure, the particles of oxides or radioactive glasses being dispersed in the metallic matrix.
  • the process described in patent FR-A 2 387 093 involves the preparation of a finely divided powder from a solution of radioactive waste containing a salt of the metal forming the matrix, then carrying out a step of hot compression.
  • this method cannot be used for the treatment of dissolving fines because it leads to the formation of a ceramic-metal, having from the thermal point of view the same drawbacks as glass.
  • the mixture of very energetic fines in an oxide which is a poor conductor of heat, leads to significant increases in temperature in the mixture, to agglomeration of the mixture and to the impossibility of obtaining a fine powder for sintering.
  • the present invention specifically relates to a process for packaging radioactive waste consisting of dissolving fines and / or parting and / or mechanical stripping fines, which overcomes the drawbacks of the methods currently known.
  • the process according to the invention for conditioning waste constituted by radioactive metallic particles insoluble in nitric solutions is characterized in that said particles are suspended in a liquid, in that the suspension is subjected to a heat treatment of evaporation by injection of said suspension on a hot bed of a powder of a metal or an alloy chosen from the group comprising copper, nickel, zinc, copper alloys, alloys nickel, zinc alloys and stainless steel, and in that the dry mixture of powder and metal particles obtained after this heat treatment is subjected to a melting carried out at a temperature sufficient to melt the metal powder or of alloy and form compounds defined between the metal of the powder and at least part of the metallic constituents of the radioactive particles.
  • the metal or alloy powder is thus used to fix, by chemical bonding, in the form of defined compounds, the metallic constituents of the radioactive particles, which has many advantages.
  • the choice of a metal or an alloy as a material for fixing radioactive waste makes it possible to solve the problems posed by the elimination of heat from radioactive particles because the metals have good thermal conductivity, which does not This is not the case with cement, glass and cermets in which large temperature gradients develop which can cause the appearance of cracks and an increase in the leaching rate because it increases with temperature. Furthermore, thanks to the good thermal conductivity of metals, it is possible to increase the rate of fixed radioactive particles and thereby reduce the volume of the packaging.
  • the level of radioactive particles fixed in the blocks obtained after solidification of the mixture is generally limited to 10% by weight.
  • the choice according to the invention, of a powder of copper, nickel, zinc, copper alloy, nickel alloy, zinc alloy or stainless steel to constitute the medium of fixing of radioactive waste makes it possible to obtain products which retain this waste better and which moreover have satisfactory characteristics over time. Indeed, these materials can form defined compounds with most of the radioactive metallic constituents of the waste particles.
  • the rhodium which is the most radioactive of the mixture of fines to be treated forms a compound defined with copper, which dissolves in the matrix giving an alloy consisting of a solid solution Cu- Rh.
  • cupronickel makes it possible to obtain a solid solution also with the fission molybdenum.
  • a powder of copper or a copper alloy for example bronze, cupronickel or a copper and zirconium alloy, is used.
  • the fines for dissolving irradiated fuels and the shearing fines are conveyed in suspension in a liquid such as water. Indeed, to recover these fines after dissolution of the irradiated fuels, the dissolution solution is subjected to a clarifica tion using either a centrifugal decanter or a pulsed filter.
  • the fines thus separated are then washed and they are suspended in a stream of water, then the suspension is stored in suitable containers before being treated by the process of the invention.
  • the suspension obtained is generally acidic and can have a nitric acidity of about 0.8 N.
  • the suspension of radioactive particles is subjected to a thermal evaporation treatment carried out by injecting this suspension on a hot bed of metal or alloy powder which will constitute the fixing medium.
  • the liquid in the suspension is evaporated simultaneously and a homogeneous mixture of radioactive particles with the metal or alloy powder of the bed which is preferably in motion during this heat treatment.
  • this treatment is carried out in a substantially horizontal tube heated and driven in rotation about its axis, which contains the bed of metal or alloy powder.
  • this tube further comprises means such as a scraper to prevent sticking of the powder particles on the wall of the tube.
  • This scraper can be constituted by a crazy bar of star section, which is supported on the tube in the bed of metal or alloy powder.
  • the suspension of radioactive particles and the metal or alloy powder are advantageously introduced at one end of the heated tube which is rotated around of its axis, and the dry mixture obtained is recovered at the other end of the tube, then it is transferred to a melting furnace.
  • a metal or alloy powder is advantageously used having a particle size of 100 to 500 ⁇ m and, preferably, a tormented surface to facilitate the mechanical attachment of the radioactive particles to the powder, because given their small dimensions (from 0.3 to 15 ⁇ m) the particles would risk being entrained by the gases circulating in the device used for thermal evaporation treatment.
  • the volumes of metal or alloy powder are chosen relative to the volume of radioactive particles to be treated, so as to obtain, after solidification, a block having satisfactory qualities. .
  • the volume ratio between the metal and alloy powder and the radioactive particles is 10, but thermal conditions (release of heat from the ingot produced, cooling conditions, etc.) can cause this ratio to be modified, by example to double it.
  • the apparatus used to carry out the thermal evaporation treatment can be constituted in particular by a calciner such as that described in patent FR-A 2 262 854.
  • the metal or alloy powder used can be oxidized by this acid solution, the dry mixture of powder and metal particles obtained following the evaporation treatment, a reduction treatment with hydrogen before carrying out the fusion.
  • This reduction treatment can be carried out in the rotary tube containing the bed of metal or alloy powder.
  • the rotary tube comprises at least two zones heated to different temperatures and a reducing gas mixture consisting, for example, of circulating in the rotary tube against the suspension and the bed of metal or alloy powder. argon or nitrogen with added hydrogen.
  • a reducing gas mixture consisting, for example, of circulating in the rotary tube against the suspension and the bed of metal or alloy powder. argon or nitrogen with added hydrogen.
  • the dry mixture obtained is then subjected to a fusion.
  • This can be carried out in a vacuum induction furnace or in a controlled atmosphere, for example under an argon atmosphere containing hydrogen.
  • the dry mixture obtained is transferred directly from the rotary tube into the melting furnace by making it flow by gravity into the crucible of the furnace and the melting is carried out at a temperature ranging from 1100 to 1500 ° C.
  • a liquid bath is generally obtained by heating the mixture to a temperature of 1300 to 1500 ° C. After fusion, the liquid bath is poured into an ingot mold. A metallic ingot is thus obtained in which the different radioactive constituents of the fines are alloyed or dispersed.
  • a flux can be added to the liquid bath, for example consisting of glass frit to digest the remaining oxides which come from the surface oxidation of the metal powder or of alloy by water vapor. After separation of the glass, upon cooling, an ingot having a clean surface is obtained.
  • the vapors and gases which escape from this tube can cause radioactive particles which it is necessary to separate.
  • the dust entrained by the vapors released during the recovery is recovered. heat treatment of evaporation, for example by washing gases and vapors, and this dust is recycled in the suspension of radioactive particles to be treated.
  • the heat treatment of evaporation is advantageously carried out by heating the rotary tube to temperatures of 250 to 450 ° C and operating under pressure lower than atmospheric pressure.
  • the device for conditioning radioactive waste in the form of particles comprises an evaporation assembly 1 and a melting furnace 2.
  • the assembly 1 comprises a tube 3 produced for example from an alloy sold under the URANUS brand, which can be rotated about its axis by means of an electric gear motor 5 via an assembly 6 with chain and gears.
  • the rotary tube 3 can be arranged either horizontally or in such a way that its axis is slightly inclined, for example up to around 3%, relative to the horizontal. It is provided at its ends with flanges 7 and 9.
  • a ferrule 11 is fixed on the flange 7 and a sealing device 13 is fitted around the ferrule 11 to seal the tube at one of its ends during of its rotation.
  • a conduit 15 connected to a suspension reservoir crosses the end piece 13 to open at the end of the tube 3 and it makes it possible to introduce into the tube 3 the suspension of radioactive particles at the desired flow rate.
  • a conduit 17 connected to a hopper 19 filled with metal or alloy powder also passes through the nozzle 13 to open into the tube 3. This conduit 17 is provided with a supply screw 21 and it makes it possible to introduce into the tube 3 the metal powder at the desired flow rate.
  • the end piece 13 is still crossed by a conduit 23 for discharging the gases.
  • This conduit then passes through a dedusting installation (not shown in the drawing), in which the entrained radioactive particles are recovered by washing the gas. The particles thus recovered are then recycled to the suspension tank associated with line 15.
  • the tube 3 is closed by a fixed sealing end piece 25 comprising a sealing connection assembly to the melting furnace 2.
  • the tube 3 is supported by rollers 26 to support the latter when the latter is in a fixed position or in rotation.
  • a conduit 27 passes through the nozzle 25 in order to circulate in the tube 3 a gas such as argon containing 5% of hydrogen against the current of the powder bed 29 which circulates in the tube 3.
  • a scraper 31 made up a crazy star-shaped bar prevents sticking of the powder particles on the walls of the tube 3 during the heat treatment.
  • the tube is placed inside an oven 33 which comprises three heating zones I, II and III in order to be able to bring the corresponding zones of the tube 3 to different temperatures.
  • the melting installation 2 comprises an induction furnace 41 inside which is placed a crucible 43 receiving the dry mixture of powder and metallic particles, coming from the tube 3, which is transferred by gravity by the light provided for this purpose in the flange 9.
  • a conduit 45 for introducing into the crucible a neutral or reducing gas such as hydrogenated argon in order to protect the bed in the crucible and push the vapors towards the nozzle 13. After fusion, the molten bath flows into an ingot mold 47.
  • a suspension containing 50 g / l of dissolving fines having a particle size of the order of a few microns is kept under stirring in the storage tank associated with line 15, and the suspension is introduced into the rotary tube 3 through line 15 at a flow rate of 5 l / h, which corresponds to the introduction of 250 g / h of fines.
  • a neutral gas containing hydrogen is introduced through the tube 27.
  • the rotation of the tube 3 is adjusted at a speed of approximately 5 revolutions / min. and zones I and II are heated to a temperature of 425 ° C and zone III to a temperature of approximately 350 ° C.
  • a bed of powders 29 having a thickness of approximately 3 cm and weighing approximately 13 kg are formed inside the tube 3, which remains in the tube for a period of approximately 5 hours.
  • the temperature of the bed rises to 80, 195 and 250 ° C. in the zones which correspond respectively to the heating zones I, II and III, and the water vapor is evacuated with the purging gas by the conduit 23 while the dry product flows by gravity into the crucible 43 of the melting installation 2.
  • the supply of tube 3 is interrupted to go to the melting phase. This can be done in about 1 hour 30 minutes when operating under 23 KW. After fusion, the liquid bath is poured into the ingot mold 47.
  • cupronickel powder was used containing for certain tests: 80% copper and 20% nickel, for other tests: 60% copper and 40% nickel. After fusion, ingots were obtained, the analysis of which confirms the formation of a solid solution with Mo.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Manufacture Of Metal Powder And Suspensions Thereof (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Processing Of Solid Wastes (AREA)
EP83402466A 1982-12-23 1983-12-19 Procédé de conditionnement de déchets constitués par des particules métalliques radioactives telles que les fines de dissolution des éléments combustibles irradiés Expired EP0112771B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR8221665A FR2538603B1 (fr) 1982-12-23 1982-12-23 Procede de conditionnement de dechets constitues par des particules metalliques radioactives telles que les fines de dissolution des elements combustibles irradies
FR8221665 1982-12-23

Publications (2)

Publication Number Publication Date
EP0112771A1 EP0112771A1 (fr) 1984-07-04
EP0112771B1 true EP0112771B1 (fr) 1987-04-01

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ID=9280456

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EP83402466A Expired EP0112771B1 (fr) 1982-12-23 1983-12-19 Procédé de conditionnement de déchets constitués par des particules métalliques radioactives telles que les fines de dissolution des éléments combustibles irradiés

Country Status (5)

Country Link
US (1) US4571307A (enrdf_load_stackoverflow)
EP (1) EP0112771B1 (enrdf_load_stackoverflow)
JP (1) JPS59133499A (enrdf_load_stackoverflow)
DE (1) DE3370715D1 (enrdf_load_stackoverflow)
FR (1) FR2538603B1 (enrdf_load_stackoverflow)

Families Citing this family (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
IT1176516B (it) * 1984-07-31 1987-08-18 Agip Spa Procedimento per la immobilizzazione di elementi di prodotti di fissione e/o elementi transuranici contenuti in scorie liquide radioattive ed apparecchiatura atta allo scopo
DE3702320A1 (de) * 1987-01-27 1988-08-04 Siempelkamp Gmbh & Co Verfahren zum entsorgen von hauptsaechlich aus eisenoxalat bestehenden radioaktiven abfaellen
JPH0648314B2 (ja) * 1987-02-13 1994-06-22 動力炉・核燃料開発事業団 放射性廃液の処理方法
US6069290A (en) * 1990-05-16 2000-05-30 Clean Technologies International Corporation Waste treatment process and reactant metal alloy
US5640702A (en) * 1992-03-17 1997-06-17 Shultz; Clifford G. Method of and system for treating mixed radioactive and hazardous wastes
US6355857B1 (en) * 1999-06-17 2002-03-12 Clean Technologies International Corporation Metal alloy treatment process for radioactive waste
US7034197B2 (en) 1998-06-12 2006-04-25 Clean Technologies International Corporation Metal alloy and metal alloy storage product for storing radioactive materials
US6037517A (en) * 1998-11-04 2000-03-14 Clean Technologies International Corporation Apparatus and method for treating waste materials which include charged particle emitters
US7365237B2 (en) * 2002-09-26 2008-04-29 Clean Technologies International Corporation Liquid metal reactor and method for treating materials in a liquid metal reactor
RU2377676C1 (ru) * 2008-03-24 2009-12-27 Государственное унитарное предприятие города Москвы - объединенный эколого-технологический и научно-исследовательский центр по обезвреживанию РАО и охране окружающей среды (ГУП МосНПО"Радон") Устройство для включения высокоактивных источников ионизирующего излучения в металлические матрицы
RU2403460C1 (ru) * 2009-05-25 2010-11-10 Геннадий Анатольевич Шаталов Трубная вставка для закручивания потока

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BE632265A (enrdf_load_stackoverflow) * 1962-05-14
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US3778295A (en) * 1972-03-08 1973-12-11 Atomic Energy Commission Chemical plating method of preparing radiation source material
GB1446016A (en) * 1973-07-24 1976-08-11 Europ Pour Le Traitement Chimi Method for the conditioning of high level radioactive wastes for their safe storage and disposal
US4040973A (en) * 1974-01-03 1977-08-09 Magyar Tudomanyos Akademia Izotop Intezete Process and apparatus for the concentration and storage of liquid radioactive wastes
JPS521399A (en) * 1975-06-24 1977-01-07 Toshiba Corp The fixation treatment method of a radioactive gas and its device
DE2704147C2 (de) * 1977-02-02 1986-04-10 Deutsche Gesellschaft für Wiederaufarbeitung von Kernbrennstoffen mbH, 3000 Hannover Verfahren zur Herstellung eines endlagerfähigen, radioaktive Stoffe enthaltenden, stabilen Verfestigungsproduktes
US4072501A (en) * 1977-04-13 1978-02-07 The United States Of America As Represented By The United States Department Of Energy Method of producing homogeneous mixed metal oxides and metal-metal oxide mixtures
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JPS54130798A (en) * 1978-03-31 1979-10-11 Toshiba Corp Radioactive waste solidifying method
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FR2456371A1 (fr) * 1979-05-07 1980-12-05 Commissariat Energie Atomique Procede de decontamination en ruthenium d'effluents radio-actifs liquides et dispositif pour la mise en oeuvre de ce procede
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US4770817A (en) * 1982-04-30 1988-09-13 Westinghouse Electric Corp. Encapsulation of solids in alpha-alumina

Also Published As

Publication number Publication date
EP0112771A1 (fr) 1984-07-04
FR2538603B1 (fr) 1988-07-01
JPS59133499A (ja) 1984-07-31
US4571307A (en) 1986-02-18
JPH0356439B2 (enrdf_load_stackoverflow) 1991-08-28
FR2538603A1 (fr) 1984-06-29
DE3370715D1 (en) 1987-05-07

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