EP2919237B1 - Radioactive waste solidification method - Google Patents

Radioactive waste solidification method Download PDF

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Publication number
EP2919237B1
EP2919237B1 EP15158743.3A EP15158743A EP2919237B1 EP 2919237 B1 EP2919237 B1 EP 2919237B1 EP 15158743 A EP15158743 A EP 15158743A EP 2919237 B1 EP2919237 B1 EP 2919237B1
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Prior art keywords
vessel
radioactive waste
glass raw
raw materials
adiabatic
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German (de)
English (en)
French (fr)
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EP2919237A1 (en
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Kenji Noshita
Takashi Asano
Atsushi Yukita
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Hitachi GE Nuclear Energy Ltd
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Hitachi GE Nuclear Energy Ltd
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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
    • G21F9/305—Glass or glass like 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
    • G21F9/28—Treating solids
    • G21F9/30—Processing

Definitions

  • the present invention relates to a radioactive waste solidification method, and more particularly to a radioactive waste solidification method suitable to processing of high-dose radioactive waste having a high radioactive level.
  • Radioactive waste generated from a nuclear facility and the like are solidified with cement or glass and are then converted to a form suitable for storage, transportation, and burial processing.
  • Solidification with cement of various types of solidification processing is a method in which radioactive waste is solidified with cement and water, so this method is inexpensive and is also advantageous in that processing is easily performed.
  • moisture included in the radioactive solidified body generated by the cement solidification is subjected to radiolysis, generating a hydrogen gas.
  • This hydrogen gas may affect the solidified body itself or a facility after burial processing (refer to Japanese Patent Laid-open No. 2007-132787 ). Therefore, in a radioactive waste solidification method described in Japanese Patent Laid-open No.
  • radioactive waste, cement, and water are mixed in a drum which is a solidifying vessel to produce a solidified body, and the solidified body is dried to eliminate moisture from the solidified body through heating or pressure reduction at a stage in which uniaxial compression strength is 1.5 MPa or more and is 75% or less of predicted strength.
  • Japanese Patent Laid-Open No. 62(1987)-124499 describes a radioactive waste solidification method.
  • solid or liquid radioactive waste are mixed with glass with a low melting point (the melting point is 400°C to 800°C), and the resulting mixture of the waste and glass is subjected to molding and baking or is melted by being heated and a solidified body is produced.
  • Japanese Patent Laid-Open No. 62(1987)-165198 describes a hydrothermal solidification method for high-level radioactive waste.
  • this hydrothermal solidification method for high-level radioactive waste high-level radioactive waste, glass, and quartz powder are mixed, and the resulting mixture is further mixed with water. This mixture is supplied into a canister. The mixture in the canister is heated to 300°C due to decay heat of the high-level radioactive waste, producing a solidified body through a hydrothermal reaction.
  • the surfaces of glass and quartz powder are melted due to decay heat and high-level radioactive waste is bonded.
  • solidification of high-dose radioactive waste solidification with glass in which a hydrogen gas due to radiation is not generated is preferable.
  • conventional methods of solidification with glass are problematic in that a large melting facility is needed, the hydrothermal solidification method for high-level radioactive waste described in Japanese Patent Laid-Open No. 62(1987)-124499 can solve the above problem because decay heat of high-level radioactive waste is used to melt glass and crystal powder.
  • high-level radioactive waste is solidified in a hydrothermal solidification method in which added water is used.
  • the high-level radioactive waste is solidified by melting only the surfaces of glass and crystal powder.
  • the produced solidified body is a non-uniform substance including water and steam and radioactive nuclides are thereby likely to leak from the solidified body.
  • An object of the present invention is to provide a radioactive waste solidification method that can produce a uniform vitrified radioactive waste through uniform heating without having to use a melting facility.
  • a feature of the present invention for attaining the above object is a radioactive waste solidification method comprising steps of:
  • the first vessel in which the radioactive waste including radioactive nuclides and glass raw materials exist is disposed in the adiabatic area in the second vessel and the glass raw materials in the first vessel are melted in the adiabatic area by heat generated from radiation emitted from the radioactive nuclides, a melting facility is not needed and the radioactive waste and glass raw materials in the first vessel are evenly heated, so a uniform vitrified radioactive waste can be obtained.
  • radioactive waste and glass raw materials are uniformly heated without having to use a melting facility and a uniform vitrified radioactive waste can be obtained.
  • the inventors made various studies and found that when a solidifying vessel filled with a mixture of a radioactive waste and glass raw materials, which are solidifying materials, is disposed in an adiabatic region formed by, for example, surrounding the solidifying vessel with an adiabatic member or vacuating the interior of the solidifying vessel and the glass raw materials in the solidifying vessel are melted by using decay heat of radioactive nuclides included in the radioactive waste, the glass raw materials in the solidifying vessel are uniformly heated and a uniform solidified body of radioactive waste can thereby be produced due to the melted glass raw materials.
  • the temperature in the glass raw materials in the solidifying vessel can be substantially uniformly raised to a temperature needed to melt the glass raw materials, regardless of the positions of the glass raw materials in the solidifying vessel.
  • the solidifying vessel filled with the radioactive waste and glass raw materials is uniformly heated, and a more uniform solidified body of radioactive wastes can thereby be produced.
  • a radioactive waste solidification method according to embodiment 1, which is a preferred embodiment of the present invention, will be described with reference to FIGs. 1 and 2 .
  • 100 kg of high-dose radioactive waste that includes 10 16 Bq of Cs-137 (for example, zeolite to which Cs-137 has been adsorbed) as high-dose radioactive waste and 100 kg of soda lime glass, which is a glass raw material, with a glass softening point of about 700°C were supplied into a solidifying vessel and a vitrified radioactive waste is produced.
  • the radioactive waste solidification method of the present embodiment will be described below with reference to the procedure illustrated in FIG. 1 .
  • Radioactive waste and glass raw materials are supplied into a solidifying vessel (step S1). Specifically, a metallic (or ceramic) vacant solidifying vessel (a first vessel) 3 is disposed below a waste tank 1 in which radioactive waste 4 has been stored. High-dose radioactive waste 4 that include 10 16 Bq of Cs-137 in the waste tank 1 are supplied by 100 kg into the solidifying vessel 3 through a waste supply pipe 2.
  • the radioactive waste 4 supplied into the solidifying vessel 3 is, for example, zeolite to which the above Cs-137 was adsorbed. After that, the solidifying vessel 3 filled with the radioactive waste 4 is moved to a position immediately below a glass raw material tank 1A.
  • 100 kg of soda lime glass which is a glass raw material 6 in the glass raw material tank 1A, is supplied into the solidifying vessel 3 through a glass raw material supply pipe 5.
  • Glass raw materials 6 may be supplied into the solidifying vessel 3 first, and after the supply of the glass raw materials 6, radioactive waste 4 may be supplied into the solidifying vessel 3.
  • the glass raw materials 6 and radioactive waste 4 may be supplied into the solidifying vessel 3 at the same time.
  • the radioactive waste 4 supplied into the solidifying vessel 3 may be a liquid radioactive waste, a solid radioactive waste, or a mixture of a liquid radioactive waste and a solid radioactive waste.
  • Adiabatic processing is performed for the solidifying vessel 3 filled with the radioactive waste 4 and the glass raw materials 6 is melted (step S2). Specifically, the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6 is disposed in an adiabatic vessel (a second vessel) 7 with its upper end open.
  • the adiabatic vessel 7 has a lid 7A, which is removable, at the upper end.
  • the lid 7A is removed, making the solidifying vessel 3 upwardly open. In this state, the solidifying vessel 3 is disposed in the adiabatic vessel 7 from above.
  • the lid 7A is attached to the upper end of the adiabatic vessel 7 to seal the adiabatic vessel 7 in which the solidifying vessel 3 is disposed.
  • the adiabatic vessel 7 and lid 7A are made of an adiabatic material. For example, they are made of glass wool.
  • an adiabatic area which is thermally insulated by the adiabatic vessel 7, is formed.
  • the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6 are disposed in this adiabatic area.
  • the adiabatic vessel 7 has a double structure of a metallic outer vessel (not shown) and an inner vessel (not shown) which is disposed in the outer vessel.
  • Glass wool is disposed in an annular area between the outer vessel and the inner vessel and in a space between a bottom of the outer vessel and a bottom of the inner vessel.
  • An upper end of the annular area between the outer vessel and the inner vessel is sealed with a ring-shaped plate attached to both upper ends of the outer vessel and inner vessel.
  • the lid 7A is formed by a metal hollow case (not shown) filled with glass wool.
  • the adiabatic processing means a processing to suppress heat of the solidifying vessel 3 from being emitted to the outside.
  • heat decay heat
  • the adiabatic vessel 7 sealed with the lid 7A Emission of this decay heat to the outside is suppressed by the adiabatic vessel 7 sealed with the lid 7A, and the decay heat is stored in the interior of the adiabatic vessel 7 sealed with the lid 7A, that is, in the adiabatic vessel 7 sealed with the lid 7A.
  • the glass raw materials 6 in the solidifying vessel 3 are heated due to this decay heat and melted.
  • the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6 is surrounded by the adiabatic vessel 7 and lid 7A, the solidifying vessel 3 is heated by decay heat of the radioactive waste 4.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 stored in the solidifying vessel 3 in the adiabatic vessel 7 become substantially uniform; these temperature do not become non-uniform depending on the positions of the radioactive wastes 4 and glass raw materials 6 in the solidifying vessel 3.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 are each raised by about 66°C per hour. Soda lime glass, which is the glass raw material 6, is melted due to this temperature rise and flows into clearances among the radioactive waste 4.
  • the radioactive waste 4 and glass raw materials 6 are mixed with an agitator. If a liquid is included in the radioactive waste 4, this liquid is heated by the heat described above and is turned into a vapor.
  • a vitrified radioactive waste is produced (step S3). Specifically, since some heat is emitted to the outside through the adiabatic vessel 7 and lid 7A, an actual temperature rise rate in the solidifying vessel 3 is lower than 66°C/h. However, a temperature rise is continued with time, so all glass raw materials 6 in the solidifying vessel 3 are melted. As a result, clearances between radioactive waste 4 are filled with the melted substances of the glass raw materials 6, and a vitrified radioactive waste 9 in which a glass-solidified substance 8 exists in the solidifying vessel 3 is produced. In the vitrified radioactive waste 9, the radioactive waste 4 have been integrated by the melted substances of the glass raw materials 6. After the vitrified radioactive waste 9 has been produced, the lid 7A is removed.
  • the vitrified radioactive waste 9 is taken out of the adiabatic vessel 7 and a lid (not shown) is attached to the solidifying vessel 3 of the vitrified radioactive waste 9 to seal it. Thereafter, the vitrified radioactive waste 9 is stored as a waste body at a prescribed storage place (not shown).
  • the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6 is surrounded by the adiabatic vessel 7 sealed with the lid 7A, radiation emitted as a result of the decay of radioactive nuclides included in the radioactive waste 4 is absorbed in the radioactive waste 4 and glass raw materials 6 disposed in the adiabatic area in the adiabatic vessel 7 and the resulting thermal energy (decay heat) heats the radioactive waste 4 and glass raw materials 6. Therefore, the radioactive waste 4 and glass raw materials 6 existing in the adiabatic area are uniformly heated, so the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 become more uniform. This suppresses corrosion of the solidifying vessel 3 at high temperatures and volatilization of the radioactive wastes 4. In addition, a uniform vitrified radioactive waste of the radioactive waste 4 is obtained. This vitrified radioactive waste is stable.
  • the radioactive waste 4 and glass raw materials 6 are heated by thermal energy generated by the absorption of radiation emitted due to the decay of the radioactive waste 4 in the solidifying vessel 3.
  • a melting facility to melt the glass raw materials 6 is not needed, unlike solidification of radioactive waste with glass, which is described in Japanese Patent Laid-open No. 2011-46996 . That is, a simple system can be used to solidify the radioactive waste 4 with the glass raw materials 6.
  • zeolite to which Cs-137 was adsorbed was supplied into the solidifying vessel 3 as the radioactive waste 4 and was solidified with the glass raw materials 6.
  • clinoptilolite, mordenitem, chabazite, insoluble ferrocyanide, or a titanate compound may be supplied into the solidifying vessel 3 and may be solidified by melting the glass raw materials 6 by the decay heat, as the radioactive waste 4.
  • any one of silicate glass and borosilicate glass may be used as the glass raw material 6.
  • any one of lead glass, phosphate glass, and vanadium-based glass, which have a softening point lower than soda lime glass, silicate glass, and borosilicate glass may be used.
  • lead glass, phosphate glass, and vanadium-based glass solidification with glass is possible in an area at a lower temperature.
  • the radioactive waste 4 can be solidified with glass in the solidifying vessel 3 and volatilization of the radioactive waste 4 can be suppressed to a lower level.
  • Glass wool used in the adiabatic vessel 7 and lid 7A which are used adiabatic processing in the present embodiment, may be replaced with any one of cellulose fiber, which is a fiber-based adiabatic material, carbonized cork, urethane foam, phenol foam, polystyrene foam, and a potassium silicate board, which is a porous adiabatic material.
  • cellulose fiber which is a fiber-based adiabatic material
  • carbonized cork carbonized cork
  • urethane foam urethane foam
  • phenol foam phenol foam
  • polystyrene foam polystyrene foam
  • a potassium silicate board which is a porous adiabatic material.
  • a radioactive waste solidification method according to embodiment 2, which is another preferred embodiment of the present invention, will be described with reference to FIGs. 1 and 2 .
  • 100 kg of high-dose radioactive waste that includes 10 16 Bq of Sr-90 for example, spent adsorbents, for radioactive nuclides, the main component of which is a titanate compound to which Sr-90 was adsorbed (the adsorbent will be referred to as the titanate compound adsorbent)
  • 100 kg of borosilicate glass which is a glass raw material, with a glass softening point of about 800°C were supplied into a solidifying vessel and a vitrified radioactive waste was produced.
  • the radioactive waste solidification method of the present embodiment will be described below.
  • a vitrified radioactive waste 9 is produced in steps S1, S2, and S3, as in embodiment 1.
  • step S1 100 kg of high-dose radioactive waste 4, including 10 16 Bq of Sr-90, stored in the waste tank 1 and 100 kg of borosilicate glass, which is glass raw materials 6, stored in the glass raw material tank 1A are supplied into the solidifying vessel 3.
  • the radioactive waste 4 supplied into the solidifying vessel 3 is a titanate compound adsorbent to which Sr-90 was adsorbed.
  • step S2 is executed. That is, as in the embodiment 1, the solidifying vessel 3 which was filled with the radioactive waste 4 and glass raw materials 6 is disposed in the adiabatic vessel 7, and the lid 7A is attached to the adiabatic vessel 7 to seal it. Radiation emitted by the decay of Sr-90 included in the radioactive waste 4 existing in the solidifying vessel 3 enclosed with the lid 7A and adiabatic vessel 7 is absorbed by the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 and is then converted to thermal energy. The radioactive waste 4 and glass raw materials 6 enclosed with the lid 7A and adiabatic vessel 7 are heated due to this thermal energy and their temperatures are raised.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 enclosed with the lid 7A and adiabatic vessel 7 become substantially uniform; these temperatures do not become non-uniform depending on the positions of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3.
  • An adiabatic area is formed in the sealed adiabatic vessel 7 as described above. In the present embodiment as well, the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6 is disposed in this adiabatic area.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 are each raised by about 160°C per hour. Borosilicate glass, which is the glass raw material 6, is melted due to this temperature rise and flows into clearances among the radioactive waste 4.
  • a vitrified radioactive waste 9 is produced. Specifically, since some heat is emitted to the outside through the adiabatic vessel 7 and lid 7A, an actual temperature rise rate in the solidifying vessel 3 is lower than 160°C/h. However, a temperature rise is continued with time, so all glass raw materials 6 in the solidifying vessel 3 are melted. As a result, clearances between radioactive waste 4 are filled with the molted substances of the glass raw materials 6, and a vitrified radioactive waste 9 in which a glass-solidified substance 8 exists in the solidifying vessel 3 is produced; in the vitrified radioactive waste 9, the radioactive waste 4 have been integrated by the melted substances of the glass raw materials 6.
  • the vitrified radioactive waste 9 is taken out of the adiabatic vessel 7 and a lid (not shown) is attached to the solidifying vessel 3 of the vitrified radioactive waste 9 to seal it. Thereafter, the vitrified radioactive waste 9 is stored as a waste body at a prescribed storage place (not shown).
  • the present embodiment can be obtained the effects generated in the embodiment 1.
  • any one of glass raw materials described in embodiment 1 may be used as the glass raw material 6.
  • the radioactive waste 4 solidified with the glass raw material 6 may be zeolite, clinoptilolite, mordenitem, chabazite, or insoluble ferrocyanide, besides a titanate compound adsorbent.
  • a radioactive waste solidification method according to embodiment 3, which is another preferred embodiment of the present invention, will be described with reference to FIGs. 1 and 3 .
  • 100 kg of high-dose radioactive waste that include 10 15 Bq of Cs-137 for example, a spent adsorbent, for radioactive nuclides, the main component of which is insoluble ferrocyanide and to which Cs-137 was adsorbed (the adsorbent will be referred to as the insoluble ferrocyanide compound adsorbent)
  • 100 kg of vanadium-based glass, which is a glass raw material, with a glass softening point of about 300°C were supplied into a solidifying vessel and a vitrified radioactive waste was produced.
  • the radioactive waste solidification method of the present embodiment will be described below.
  • a vitrified radioactive waste 9 is produced in steps S1, S2 and S3, as in embodiment 1.
  • a pressure reducing vessel (second vessel) 10 is used instead of the adiabatic vessel 7 used in step S2 in embodiments 1 and 2.
  • 100 kg of insoluble ferrocyanide compound adsorbent, which is the radioactive waste 4 in the waste tank 1, and 100 kg of vanadium-based glass, which is the glass raw material 6 in the glass raw material tank 1A, are supplied into the solidifying vessel (first vessel) 3 in step S1.
  • the solidifying vessel 3 into which the radioactive waste 4 and vanadium-based glass were supplied is then disposed in the pressure reducing vessel 10 in step S2.
  • a lid 10A is attached to the pressure reducing vessel 10 to seal it.
  • An exhaust pipe 12 connected to the pressure reducing vessel 10 is connected to a pressure reducing pump 11.
  • an exhaust pipe 13 is connected to the pressure reducing pump 11.
  • step S2 the pressure in the sealed pressure reducing vessel 10 is reduced as described below.
  • the pressure reducing pump 11 is driven and an opening/closing valve (not shown) attached to the exhaust pipe 12 is opened.
  • an opening/closing valve (not shown) attached to the exhaust pipe 12 is opened.
  • the gas in the sealed pressure reducing vessel 10 in which the solidifying vessel 3 is disposed is released to the outside through the exhaust pipe 12.
  • This exhaust of the gas by the exhaust pipe 12 is performed until the pressure in the pressure reducing vessel 10 drops to one-tenth the atmospheric pressure.
  • the pressure reducing pump 11 is stopped and the opening/closing valve attached to the exhaust pipe 12 is closed.
  • adiabatic performance is improved by a factor of about 10 as compared with the use of the adiabatic vessel 7.
  • the solidifying vessel 3 When the solidifying vessel 3 is thermally insulated by pressure reduction as described above, radiation generated due to the decay of Cs-137 included in the radioactive waste 4 in the solidifying vessel 3 is absorbed by the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 and is then converted to thermal energy.
  • the radioactive waste 4 and glass raw materials 6 enclosed with the lid 10A and pressure reducing vessel 10 and existing in the area at a reduced pressure (adiabatic area) are heated due to this thermal energy. Accordingly, the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 are raised. These temperatures become substantially uniform; these temperatures do not become non-uniform depending on the positions of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3.
  • Cs-137 emits radiation with about 1.15 MeV of energy per disintegration, as described in embodiment 1.
  • the radiation is converted to thermal energy.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 are each raised by about 6.6°C per hour.
  • a vitrified radioactive waste 9 is produced. Specifically, since some heat is emitted to the outside through the adiabatic vessel 7 and lid 7A, an actual temperature rise rate in the solidifying vessel 3 is lower than 6.6°C/h. However, a temperature rise is continued with time, so all glass raw materials 6 in the solidifying vessel 3 are melted. As a result, clearances between radioactive waste 4 are filled with the molted substances of the glass raw materials 6, and a vitrified radioactive waste 9 in which a glass-solidified substance 8 exists in the solidifying vessel 3 is produced; in the vitrified radioactive waste 9, the radioactive waste 4 have been integrated by the melted substances of the glass raw materials 6.
  • the vitrified radioactive waste 9 is taken out of the pressure reducing vessel 10 and a lid (not shown) is attached to the solidifying vessel 3 of the vitrified radioactive waste 9 to seal it. Thereafter, the vitrified radioactive waste 9 is stored as a waste body at a prescribed storage place (not shown).
  • the present embodiment can be obtained the effects generated in the embodiment 1.
  • the radioactive waste 4 and glass raw materials 6 existing in the adiabatic area in the sealed pressure reducing vessel 10 are uniformly heated, so the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 become more uniform.
  • the solidifying vessel 3 including the radioactive waste 4 and glass raw materials 6 is disposed in the sealed pressure reducing vessel 10 and the pressure in the pressure reducing vessel 10 is reduced, so a desired adiabatic effect can be obtained by adjusting the degree of pressure reduction.
  • any one of the glasses described in embodiment 1 may be used as the glass raw material 6.
  • the radioactive waste 4 solidified with the glass raw material 6 may be zeolite, clinoptilolite, mordenitem, chabazite, or a titanate compound, besides an insoluble ferrocyanide compound adsorbent.
  • a radioactive waste solidification method according to embodiment 4, which is another preferred embodiment of the present invention, will be described with reference to FIGs. 1 and 4 .
  • 100 kg of high-dose radioactive waste that includes 10 15 Bq of Co-60 for example, a solid-state radioactive waste the main component of which is an iron oxide including Co-60 (the radioactive waste will be referred to as the iron oxide)
  • 100 kg of soda lime glass, which is a glass raw material, with a glass softening point of about 700°C were supplied into a solidifying vessel to produce a vitrified radioactive waste.
  • the radioactive waste solidification method of the present embodiment will be described below.
  • a vitrified radioactive waste 9 is produced in steps S1, S2 and S3, as in embodiment 1.
  • the radioactive waste (for example, iron oxides) 4 and glass raw materials (soda-lime glass) 6 supplied into the solidifying vessel 3 are mixed with an agitator in step S1 and in adiabatic processing in step S2, the adiabatic vessel 7 to which an air supply pipe that has an air supply pump is connected and further, an exhaust pipe is also connected is used instead of the adiabatic vessel 7 used in step S2 in embodiments 1 and 2.
  • 100 kg of iron oxide, which is the radioactive waste 4 supplied from the waste tank 1, and 100 kg of soda lime glass, which is the glass raw material 6 supplied from the glass raw material tank 1A, are supplied into the solidifying vessel 3 in step S1.
  • an agitator 14 is inserted into the solidifying vessel 3 in step S1.
  • the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 are mixed with this agitator 14.
  • the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6 is disposed in the adiabatic vessel 7 in step S2.
  • the lid 7A is attached to the adiabatic vessel 7 to seal it.
  • An air supply pipe 17 to which an air supply pump 16 and an opening/closing valve (not shown) are attached and an exhaust pipe 18 to which an opening/closing valve (not shown) is attached are connected to the adiabatic vessel 7.
  • a thermometer 19 is attached to the adiabatic vessel 7.
  • adiabatic processing in step S2 is performed for the solidifying vessel 3 filled with the radioactive waste 4 and glass raw materials 6.
  • Radiation emitted by the decay of Co-60 included in the radioactive waste 4 existing in the solidifying vessel 3 enclosed with the sealed adiabatic vessel 7 is absorbed by the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 and is then converted to thermal energy.
  • the radioactive waste 4 and glass raw materials 6 enclosed with the lid 7A and adiabatic vessel 7 are heated due to this thermal energy and their temperatures are raised.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 enclosed with the lid 7A and adiabatic vessel 7 become substantially uniform; these temperatures do not become non-uniform depending on the positions of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3.
  • Co-60 emits radiation with about 2.5 MeV of energy per disintegration.
  • this radiation is absorbed in the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3, the radiation is converted to thermal energy.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 are each raised by about 144°C per hour.
  • step S3 a vitrified radioactive waste 9 is produced. Specifically, since some heat is emitted to the outside through the adiabatic vessel 7 and lid 7A, an actual temperature rise rate in the solidifying vessel 3 is lower than 144°C/h. However, a temperature rise is continued with time, so all glass raw materials 6 in the solidifying vessel 3 are melted. At that time, the temperature of the solidifying vessel 3 in the adiabatic vessel 7 is measured with the thermometer 19.
  • the opening/closing valve attached to the air supply pipe 17 and the opening/closing valve attached to the exhaust pipe 18 are opened and the air supply pump 16 is driven.
  • an external gas (air) is supplied into the interior of the adiabatic vessel 7 through the air supply pipe 17 and the temperature of the solidifying vessel 3 is maintained at an appropriate temperature.
  • the air supplied into the adiabatic vessel 7 is exhausted to the outside of the adiabatic vessel 7 through the exhaust pipe 18.
  • the amount of air to be supplied into the adiabatic vessel 7 according to the temperature of the solidifying vessel 3 can be adjusted by controlling the rotational speed of the air supply pump 16.
  • the radioactive waste 4 As a result, clearances between the radioactive waste 4 are filled with the molted substances of the glass raw materials 6, and a vitrified radioactive waste 9 in which a glass-solidified substance 8 exists in the solidifying vessel 3 is produced; in the vitrified radioactive waste 9, the radioactive waste 4 have been integrated by the melted substances of the glass raw materials 6.
  • the vitrified radioactive waste 9 is taken out of the adiabatic vessel 7 and a lid (not shown) is attached to the solidifying vessel 3 of the vitrified radioactive waste 9 to seal it. Thereafter, the vitrified radioactive waste 9 is stored as a waste body at a prescribed storage place (not shown).
  • the present embodiment can be obtained the effects generated in the embodiment 1.
  • the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 are mixed with the agitator 14, a uniform vitrified radioactive waste 9 can be produced in a shorter time.
  • the amount of gas (for example, air) to be supplied into the adiabatic vessel 7 is adjusted based on the measured temperature of the solidifying vessel 3 in the adiabatic vessel 7, so that it is possible to prevent the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3, which are raised by heat generated due to the decay of radioactive nuclides (for example, Co-60), from exceeding a temperature necessary for glass solidification. Therefore, the evaporation of radioactive nuclides included in the radioactive waste 4 can be suppressed.
  • the amount of gas to be supplied into the adiabatic vessel 7 can also be adjusted based on the measured temperature of the solidifying vessel 3. Since the temperature during solidification with glass is measured and the amount of gas to be supplied is controlled, the rate at which the glass raw materials 6 are cooled can be adjusted. This can suppress the vitrified radioactive waste 9 from being cracked due to thermal distortion.
  • any one of the glasses described in embodiment 1 may be used as the glass raw materials 6.
  • the radioactive waste 4 solidified with the glass raw material 6 may be zeolite, clinoptilolite, mordenitem, chabazite, an insoluble ferrocyanide compound, or a titanate compound, besides iron oxides.
  • a radioactive waste solidification method according to embodiment 5, which is another preferred embodiment of the present invention, will be described with reference to FIG. 5 .
  • 100 kg of high-dose radioactive waste that includes 10 16 Bq of Cs-137 (for example, zeolite to which Cs-137 was adsorbed) as high-dose radioactive waste and 300 kg of soda lime glass, which is a glass raw material, with a glass softening point of about 700°C were supplied into a solidifying vessel to produce a vitrified radioactive waste.
  • Cs-137 for example, zeolite to which Cs-137 was adsorbed
  • soda lime glass which is a glass raw material
  • a vitrified radioactive waste 9 is produced in steps S1, S2 and S3, as in embodiment 1.
  • the radioactive waste 4 and glass raw materials 6 are supplied into the solidifying vessel 3 at the same time in step S1 and, in adiabatic processing in step S2, the pressure reducing vessel 10 is used as in embodiment 1.
  • 100 kg of high-dose radioactive waste 4, including 10 16 Bq of Cs-137, supplied from the waste tank 1 and 300 kg of glass raw material 6 supplied from the glass raw material tank 1A are supplied into the solidifying vessel 3 at the same time in step S1.
  • the radioactive waste 4 is spent adsorbent the main component of which is insoluble ferrocyanide and to which Cs-137 was adsorbed.
  • the glass raw material 6 is soda lime glass.
  • the radioactive waste 4 and glass raw materials 6 are mixed in the solidifying vessel 3.
  • the mixed radioactive waste 4 and glass raw materials 6 will be referred to as the mixed filler 15.
  • the solidifying vessel 3 filled with the mixed filler 15 is disposed in the pressure reducing vessel 10 in step S2, as in embodiment 3.
  • the thermometer 19 is attached to the pressure reducing vessel 10.
  • the lid 10A is attached to the pressure reducing vessel 10 to seal it. After that, the pressure reducing pump 11 is driven and the pressure in the sealed pressure reducing vessel 10 is reduced to one-tenth the atmospheric pressure, as in embodiment 3.
  • the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3 are heated by thermal energy generated due to the decay of Cs-137 included in the radioactive waste 4.
  • the temperatures of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3, which is thermally insulated from the outside, are thereby raised. These temperatures become substantially uniform; these temperatures do not become non-uniform depending on the positions of the radioactive waste 4 and glass raw materials 6 in the solidifying vessel 3.
  • the glass raw materials 6 in the solidifying vessel 3 are melted and this molted glass raw materials 6 osmoses clearances among the radioactive waste 4.
  • the pressure in the pressure reducing vessel 10 is controlled by supplying air to and exhausting air from the pressure reducing vessel 10 with the pressure reducing pump 11. As a result, the temperatures of the glass raw materials 6 are maintained at an appropriate temperature.
  • Cs-137 emits radiation with about 1.15 MeV of energy per disintegration, as described above. Therefore, when the radioactive waste 4 includes 10 16 Bq of Cs-137, thermal energy at a heat generation rate of 1840 J/s is obtained. If the specific heat of the mixture of the radioactive waste (zeolite to which Cs-137 was adsorbed) 4 and glass raw material (soda lime glass) 6 is 0.5 J/(g.K), the temperatures of the radioactive waste 4 and glass raw materials 6 are each raised by about 33°C per hour.
  • a vitrified radioactive waste 9 is produced. Specifically, a temperature rise is continued with time, so all glass raw materials 6 are melted. As a result, clearances between radioactive waste 4 are filled with the molted substances of the glass raw materials 6, and a vitrified radioactive waste 9 in which a glass-solidified substance 8 exists in the solidifying vessel 3 is produced; in the vitrified radioactive waste 9, the radioactive waste 4 have been integrated by the melted substances of the glass raw materials 6.
  • the vitrified radioactive waste 9 is taken out of the pressure reducing vessel 10 and a lid (not shown) is attached to the solidifying vessel 3 of the vitrified radioactive waste 9 to seal it. Thereafter, the vitrified radioactive waste 9 is stored as a waste body at a prescribed storage place (not shown).
  • any one of the glasses described in the first embodiment may be used as the glass raw materials 6.
  • the radioactive waste 4 solidified with the glass raw material 6 may be clinoptilolite, mordenitem, chabazite, an insoluble ferrocyanide compound, or a titanate compound, besides zeolite.

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  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Processing Of Solid Wastes (AREA)
EP15158743.3A 2014-03-14 2015-03-12 Radioactive waste solidification method Active EP2919237B1 (en)

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JP2014052245A JP6126031B2 (ja) 2014-03-14 2014-03-14 放射性廃棄物の固化処理方法

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JP6423194B2 (ja) * 2014-07-23 2018-11-14 日立Ｇｅニュークリア・エナジー株式会社 放射性廃棄物の固化処理方法
GB2570971A (en) * 2016-06-23 2019-08-14 Nippon Chemical Ind Method for manufacturing solidified body of radioactive waste

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US3365578A (en) * 1962-08-10 1968-01-23 Atomic Energy Authority Uk Glass composition comprising radioactive waste oxide material contained within a steel vessel
US4351749A (en) * 1978-11-18 1982-09-28 Vitrex Corporation Molecular glasses for nuclear waste encapsulation
JPS6013295A (ja) * 1983-07-04 1985-01-23 株式会社東芝 放射性廃棄物の固化処理方法
JPS62124499A (ja) 1985-11-26 1987-06-05 株式会社東芝 放射性廃棄物の固化処理方法
JPS62165198A (ja) * 1986-01-17 1987-07-21 株式会社新来島どっく 高レベル放射性廃棄物の水熱固化処理法
JP4772459B2 (ja) 2005-11-10 2011-09-14 株式会社東芝 放射性廃棄物の固化処理方法
US8525085B2 (en) * 2006-05-10 2013-09-03 Massachusetts Institute Of Technology Directed energy melter
JP5472704B2 (ja) 2009-08-26 2014-04-16 三菱マテリアル株式会社 高レベル放射性廃棄物ガラス固化処理のための電気溶融炉用Ｃｏ基合金製部材および電気溶融炉

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