CN108249925A - A kind of preparation method of complete ceramic microencapsulated fuel pellet - Google Patents

A kind of preparation method of complete ceramic microencapsulated fuel pellet Download PDF

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CN108249925A
CN108249925A CN201711384305.7A CN201711384305A CN108249925A CN 108249925 A CN108249925 A CN 108249925A CN 201711384305 A CN201711384305 A CN 201711384305A CN 108249925 A CN108249925 A CN 108249925A
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fuel pellet
silicon carbide
carbide powder
sintering
preparation
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CN108249925B (en
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刘文涛
马渊
刘业光
魏东波
孟莹
赵瑞瑞
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China North Nuclear Fuel Co Ltd
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    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
    • C04B35/56—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
    • C04B35/565—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
    • C—CHEMISTRY; METALLURGY
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    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/628—Coating the powders or the macroscopic reinforcing agents
    • C04B35/62892—Coating the powders or the macroscopic reinforcing agents with a coating layer consisting of particles
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/64—Burning or sintering processes
    • C04B35/645—Pressure sintering
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G21C3/58—Solid reactor fuel Pellets made of fissile material
    • G21C3/62—Ceramic fuel
    • G21C3/64—Ceramic dispersion fuel, e.g. cermet
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
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    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
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    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
    • C04B2235/3225—Yttrium oxide or oxide-forming salts thereof
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    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/74—Physical characteristics
    • C04B2235/77—Density
    • 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
    • Y02E30/30—Nuclear fission reactors

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Abstract

The invention belongs to fuel pellet preparing technical fields, and in particular to a kind of preparation method of complete ceramic microencapsulated fuel pellet includes the following steps：Step 1, silicon carbide powder and sintering aid addition；Step 2, TRISO SiC p surface platings silicon carbide powder；Step 3, fuel pellet is preforming；Step 4, fuel pellet hot pressed sintering.Complete ceramic microencapsulated fuel pellet produced by the present invention is cylindrical shape, density >=3.1g/cm3, pellet inside TRISO grain structures keep complete, and are uniformly distributed in silicon carbide-based internal.

Description

A kind of preparation method of complete ceramic microencapsulated fuel pellet
Technical field
The invention belongs to fuel pellet preparing technical fields, and in particular to a kind of preparation of complete ceramic microencapsulated fuel pellet Method.
Background technology
At present commercialization nuclear power fuel using ceramic UO pellet, main preparation method be by compacting, Ceramic pellet is made in the uranium dioxide of certain degree of enrichment by the powder metallurgy process such as sintering, shape grinding.Although in opening for many years More mature application can be formed in hair, but is still had some disadvantages under specific use condition, is mainly manifested in matrix With relatively low thermal conductivity, fault freedom in the event of an accident is poor, therefore the safety guarantee of nuclear fuel is poor.
As promoted nuclear plant safety performance important measure, research and development fault tolerant fuel (Accident Tolerant Fuel, ATF) becoming the new direction of nuclear fuel field Overseas Development, accident can be contained to a certain degree and there is inherent safety Fuel.
Full ceramics microencapsulated fuel pellet is designed by the high burnup U that is used in light water reactor, is by uranium dioxide fuel Particle is encapsulated in silicon carbide substrate, and silicon carbide substrate stability is high and has both very high thermal conductivity, has had with cooling agent simultaneous Capacitive.The fission gas and corrosivity fission product that the fuel of full ceramic matrix cladding releases are seldom, hold in the event of an accident Mistake is high, and safety is guaranteed.
Invention content
The technical problem to be solved by the present invention is to TRISO (Tristructural Isotropic (TRISO) Coated Fuel Particles) particle and silicon carbide powder be raw material, TRISO particles even dispersion be distributed by powder metallurgical technique It is silicon carbide-based in vivo, prepare a kind of complete ceramic microencapsulated fuel pellet.
In order to realize the purpose, the technical solution adopted by the present invention is that：
A kind of preparation method of complete ceramic microencapsulated fuel pellet, includes the following steps：
Step 1, silicon carbide powder and sintering aid addition
Step 1.1, raw material is determined
Average grain diameter≤1 μm of silicon carbide powder, specific surface area >=20m2/g；
Sintering aid is aluminium oxide and the mixture of rare earth oxide, and average grain diameter is 0.9~1.1 μm；
Step 1.2, sintering aid is added
Sintering aid is added in into silicon carbide powder, sintering aid additive amount is the 6%~10% of silicon carbide powder quality；
Sintering aid and silicon carbide powder are mixed using wet ball grinding technique, dispersant is organic solvent；
Screening is dried after the completion of wet ball grinding as silicon carbide powder matrix material；
Step 2, TRISO SiC p surface platings silicon carbide powder
Step 2.1, it uniformly coats bonding system in TRISO particle surfaces and impregnates setting time, bonding system is viscosity Organic solvent；
Step 2.2, it is former in the silicon carbide powder matrix that particle surface one layer of step 1 of bonding obtains using surface bonding technology Material；
Step 2.3, TRISO particles are uniformly mixed with silicon carbide powder；
Step 3, fuel pellet is preforming
Fuel pellet is preforming using compression molding, and green compact pellet is cylinder, using zinc stearate mixing carbon tetrachloride As molding lubricant, pellet typed pressure is 10~50MPa, 5~20s of dwell time；
Step 4, fuel pellet hot pressed sintering
Fuel pellet sintering belongs to liquid-phase sintering, and sintering processing is hot pressed sintering, using high-density graphite as hot pressing die, heat Pressing temperature control, in 30~100min, hot pressing pressure is 15~50MPa for soaking time control at 1850~2000 DEG C.
Further, the preparation method of a kind of complete ceramic microencapsulated fuel pellet as described above in step 1.1, helps burning Agent is aluminium oxide and Y2O3Mixture, aluminium oxide and Y2O3Mass ratio be 2：8、4：6、3：One kind in 7.
Further, the preparation method of a kind of complete ceramic microencapsulated fuel pellet as described above in step 1.1, helps burning Agent is aluminium oxide and Gd2O3Mixture, aluminium oxide and Gd2O3Mass ratio be 2：8、4：6、3：One kind in 7.
Further, the preparation method of a kind of complete ceramic microencapsulated fuel pellet as described above, in step 1.2, dispersion Agent is absolute ethyl alcohol, one kind in carbon tetrachloride.
Further, the preparation method of a kind of complete ceramic microencapsulated fuel pellet as described above in step 2.1, bonds System is the glycerine ethanol solution that mass concentration is 5~30%, and glycerine is as binding agent, and absolute ethyl alcohol is as diluent.
Further, the preparation method of a kind of complete ceramic microencapsulated fuel pellet as described above, in step 2.2, TRISO The quality of particle is 20~50wt% of silicon carbide powder matrix material quality.
Further, the preparation method of a kind of complete ceramic microencapsulated fuel pellet as described above in step 4, is sintered gas Atmosphere is vacuum, one kind in argon gas atmosphere.
The advantageous effect of technical solution of the present invention is：It is circle by complete ceramic microencapsulated fuel pellet produced by the present invention Post shapes, density >=3.1g/cm3, the TRISO grain structures holding of pellet inside is complete, and is uniformly distributed in silicon carbide substrate It is interior.
Specific embodiment
Technical solution of the present invention is described in detail with reference to specific embodiment.
A kind of preparation method of complete ceramic microencapsulated fuel pellet of the present invention, includes the following steps：
Step 1, silicon carbide powder and sintering aid addition
Step 1.1, raw material is determined
Average grain diameter≤1 μm of silicon carbide powder, specific surface area >=20m2/g；
Sintering aid is aluminium oxide and the mixture of rare earth oxide, and average grain diameter is 0.9~1.1 μm；
Specifically, the scheme of sintering aid have it is following two：1. aluminium oxide and Y2O3Mixture, aluminium oxide and Y2O3Matter Amount is than being 2：8、4：6、3：One kind in 7；2. sintering aid is aluminium oxide and Gd2O3Mixture, aluminium oxide and Gd2O3Quality Than being 2：8、4：6、3：One kind in 7；
Step 1.2, sintering aid is added
Sintering aid is added in into silicon carbide powder, sintering aid additive amount is the 6%~10% of silicon carbide powder quality；
Sintering aid and silicon carbide powder are mixed using wet ball grinding technique, dispersant is absolute ethyl alcohol, four chlorinations The organic solvents such as carbon；
Screening is dried after the completion of wet ball grinding as silicon carbide powder matrix material；
Step 2, TRISO SiC p surface platings silicon carbide powder
Step 2.1, it uniformly coats bonding system in TRISO particle surfaces and impregnates setting time, bonding system is viscosity Organic solvent；Specifically, bonding system is the glycerine ethanol solution that mass concentration is 5~30%, glycerine as binding agent, Absolute ethyl alcohol is as diluent；
Step 2.2, it is former in the silicon carbide powder matrix that particle surface one layer of step 1 of bonding obtains using surface bonding technology Material；The quality of TRISO particles is 20~50wt% of silicon carbide powder matrix material quality；
Step 2.3, TRISO particles are uniformly mixed with silicon carbide powder；
Step 3, fuel pellet is preforming
Fuel pellet is preforming using compression molding, and green compact pellet is cylinder, using zinc stearate mixing carbon tetrachloride As molding lubricant, pellet typed pressure is 10~50MPa, 5~20s of dwell time；
Step 4, fuel pellet hot pressed sintering
Fuel pellet sintering belongs to liquid-phase sintering, and sintering processing is hot pressed sintering, using high-density graphite as hot pressing die, burns It is vacuum or argon gas atmosphere to tie atmosphere, and hot pressing temperature control is at 1850~2000 DEG C, and soaking time control is in 30~100min, heat Pressure pressure is 15~50MPa.

Claims (8)

1. a kind of preparation method of complete ceramic microencapsulated fuel pellet, which is characterized in that include the following steps：
Step 1, silicon carbide powder and sintering aid addition
Step 1.1, raw material is determined
Average grain diameter≤1 μm of silicon carbide powder, specific surface area >=20m2/g；
Sintering aid is aluminium oxide and the mixture of rare earth oxide, and average grain diameter is 0.9~1.1 μm；
Step 1.2, sintering aid is added
Sintering aid is added in into silicon carbide powder, sintering aid additive amount is the 6%~10% of silicon carbide powder quality；
Sintering aid and silicon carbide powder are mixed using wet ball grinding technique, dispersant is organic solvent；
Screening is dried after the completion of wet ball grinding as silicon carbide powder matrix material；
Step 2, TRISO SiC p surface platings silicon carbide powder
Step 2.1, it uniformly coats bonding system in TRISO particle surfaces and impregnates setting time, bonding system is that viscosity is organic Solvent；
Step 2.2, the silicon carbide powder matrix material obtained using surface bonding technology in particle surface one layer of step 1 of bonding；
Step 2.3, TRISO particles are uniformly mixed with silicon carbide powder；
Step 3, fuel pellet is preforming
Fuel pellet is preforming using compression molding, and green compact pellet is cylinder, using zinc stearate mixing carbon tetrachloride conduct Molding lubricant, pellet typed pressure are 10~50MPa, 5~20s of dwell time；
Step 4, fuel pellet hot pressed sintering
Fuel pellet sintering belongs to liquid-phase sintering, and sintering processing is hot pressed sintering, using high-density graphite as hot pressing die, hot pressing temperature Degree control is at 1850~2000 DEG C, and in 30~100min, hot pressing pressure is 15~50MPa for soaking time control.
2. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：Step 1.1 In, sintering aid is aluminium oxide and Y2O3Mixture, aluminium oxide and Y2O3Mass ratio be 2：8、4：6、3：One kind in 7.
3. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：Step 1.1 In, sintering aid is aluminium oxide and Gd2O3Mixture, aluminium oxide and Gd2O3Mass ratio be 2：8、4：6、3：One kind in 7.
4. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：Step 1.2 In, dispersant is absolute ethyl alcohol, one kind in carbon tetrachloride.
5. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：Step 2.1 In, bonding system is the glycerine ethanol solution that mass concentration is 5~30%, and glycerine is as binding agent, absolute ethyl alcohol conduct Diluent.
6. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：Step 2.2 In, the quality of TRISO particles is 20~50wt% of silicon carbide powder matrix material quality.
7. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：In step 4, Sintering atmosphere is vacuum, one kind in argon gas atmosphere.
8. a kind of preparation method of complete ceramic microencapsulated fuel pellet as described in claim 1, it is characterised in that：Step 1.1 In, the scheme of sintering aid has following two：1. aluminium oxide and Y2O3Mixture, aluminium oxide and Y2O3Mass ratio be 2：8、4： 6、3：One kind in 7；2. sintering aid is aluminium oxide and Gd2O3Mixture, aluminium oxide and Gd2O3Mass ratio be 2：8、4：6、 3：One kind in 7；
In step 1.2, dispersant is absolute ethyl alcohol, one kind in carbon tetrachloride；
In step 2.1, bonding system is the glycerine ethanol solution that mass concentration is 5~30%, and glycerine is as binding agent, nothing Water-ethanol is as diluent；
In step 2.2, the quality of TRISO particles is 20~50wt% of silicon carbide powder matrix material quality；
In step 4, sintering atmosphere is vacuum, one kind in argon gas atmosphere.
CN201711384305.7A 2017-12-20 2017-12-20 Preparation method of all-ceramic micro-packaging fuel pellet Active CN108249925B (en)

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN110729064A (en) * 2019-10-24 2020-01-24 中国核动力研究设计院 Al for nuclear power2O3-Gd2O3Burnable poison ceramic material and preparation method thereof
CN112739664A (en) * 2018-09-28 2021-04-30 福吉米株式会社 Coated silicon carbide particle powder
CN113611435A (en) * 2021-08-17 2021-11-05 西北工业大学 Ceramic composite fuel pellet and preparation method and application thereof
CN115295198A (en) * 2022-08-04 2022-11-04 中国核动力研究设计院 Method for preparing all-ceramic micro-packaging dispersion fuel by oscillation sintering
WO2022241733A1 (en) * 2021-05-20 2022-11-24 中广核研究院有限公司 High-entropy ceramic inert matrix dispersion fuel pellet and preparation method therefor
CN116926399A (en) * 2023-07-05 2023-10-24 湖南昕昱科技有限公司 Special ceramic material and preparation method and application thereof

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WO2017019620A1 (en) * 2015-07-25 2017-02-02 Ultra Safe Nuclear Corporation Method for fabrication of fully ceramic microencapsulated nuclear fuel
CN106653126A (en) * 2016-12-28 2017-05-10 中核北方核燃料元件有限公司 Method and mould for preparing annular UO2 fuel pellet
CN106935297A (en) * 2015-12-30 2017-07-07 中核北方核燃料元件有限公司 A kind of preparation method of thorium anhydride paillon foil
CN106971765A (en) * 2017-04-13 2017-07-21 中国工程物理研究院材料研究所 A kind of preparation technology of high TRISO contents inertia base dispersion fuel pellet
CN106981318A (en) * 2017-04-13 2017-07-25 中国工程物理研究院材料研究所 A kind of inertia base disperse pellet fuel and its production and use

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Publication number Priority date Publication date Assignee Title
WO2017019620A1 (en) * 2015-07-25 2017-02-02 Ultra Safe Nuclear Corporation Method for fabrication of fully ceramic microencapsulated nuclear fuel
CN106935297A (en) * 2015-12-30 2017-07-07 中核北方核燃料元件有限公司 A kind of preparation method of thorium anhydride paillon foil
CN106653126A (en) * 2016-12-28 2017-05-10 中核北方核燃料元件有限公司 Method and mould for preparing annular UO2 fuel pellet
CN106971765A (en) * 2017-04-13 2017-07-21 中国工程物理研究院材料研究所 A kind of preparation technology of high TRISO contents inertia base dispersion fuel pellet
CN106981318A (en) * 2017-04-13 2017-07-25 中国工程物理研究院材料研究所 A kind of inertia base disperse pellet fuel and its production and use

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112739664A (en) * 2018-09-28 2021-04-30 福吉米株式会社 Coated silicon carbide particle powder
CN112739664B (en) * 2018-09-28 2023-07-21 福吉米株式会社 Coated silicon carbide particle powder
CN110729064A (en) * 2019-10-24 2020-01-24 中国核动力研究设计院 Al for nuclear power2O3-Gd2O3Burnable poison ceramic material and preparation method thereof
WO2022241733A1 (en) * 2021-05-20 2022-11-24 中广核研究院有限公司 High-entropy ceramic inert matrix dispersion fuel pellet and preparation method therefor
CN113611435A (en) * 2021-08-17 2021-11-05 西北工业大学 Ceramic composite fuel pellet and preparation method and application thereof
CN115295198A (en) * 2022-08-04 2022-11-04 中国核动力研究设计院 Method for preparing all-ceramic micro-packaging dispersion fuel by oscillation sintering
CN115295198B (en) * 2022-08-04 2024-03-19 中国核动力研究设计院 Method for preparing full ceramic micro-package dispersion fuel by oscillation sintering
CN116926399A (en) * 2023-07-05 2023-10-24 湖南昕昱科技有限公司 Special ceramic material and preparation method and application thereof
CN116926399B (en) * 2023-07-05 2024-04-09 湖南昕昱科技有限公司 Special ceramic material and preparation method and application thereof

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