CN109994223A - A kind of novel dispersion fuel and its manufacturing method - Google Patents

A kind of novel dispersion fuel and its manufacturing method Download PDF

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Publication number
CN109994223A
CN109994223A CN201711498475.8A CN201711498475A CN109994223A CN 109994223 A CN109994223 A CN 109994223A CN 201711498475 A CN201711498475 A CN 201711498475A CN 109994223 A CN109994223 A CN 109994223A
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fuel
sic
dispersion
green compact
pellet
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Inventor
刘仕超
焦拥军
陈平
李文杰
涂腾
李伟
高士鑫
何梁
欧大鹏
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Nuclear Power Institute of China
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Nuclear Power Institute of China
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    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21CNUCLEAR REACTORS
    • G21C21/00Apparatus or processes specially adapted to the manufacture of reactors or parts thereof
    • G21C21/02Manufacture of fuel elements or breeder elements contained in non-active casings
    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21CNUCLEAR REACTORS
    • G21C3/00Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42Selection of substances for use as reactor fuel
    • G21C3/58Solid reactor fuel Pellets made of fissile material
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00Energy generation of nuclear origin
    • Y02E30/30Nuclear fission reactors

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Manufacturing & Machinery (AREA)
  • Ceramic Products (AREA)

Abstract

The invention belongs to reactor fuel technical fields, and in particular to a kind of novel dispersion fuel and its manufacturing method.A kind of novel dispersion fuel, involucrum are wrapped in outside column pellet, and column pellet includes fuel region and without fuel bed, and no fuel bed is wrapped in outside fuel region, and fuel region includes TRISO particle and SiC matrix, and TRISO particle dispersion is in SiC ceramic matrix.A kind of manufacturing method of dispersion fuel includes the following steps: step 1, preparation column pellet green compact;Step 2 makes to prepare SiC/SiC short fiber composite material green tape;Step 3 obtains cylindrical shape without fuel region green compact;Step 4 is prepared into disc-shaped without fuel region green compact;Rod fuel area green compact are placed in cylindrical shape without in fuel region green compact by step 5, are prepared into column pellet through hot pressed sintering;Step 6 carries out grinding to column pellet, obtains novel dispersion fuel pellet.The present invention is able to solve that dispersion fuel TRISO distribution of particles in the prior art is unreasonable and the defect of poor processability.

Description

A kind of novel dispersion fuel and its manufacturing method
Technical field
The invention belongs to reactor fuel technical fields, and in particular to a kind of novel dispersion fuel and its manufacturing method.
Background technique
Traditional reactor fuel element is stacked in zirconium alloy cladding by uranium dioxide pellet to be formed.It is mentioned now with burnup It rises and the refulling cycle is elongated, fuel element performance declines under high burnup, including involucrum corrosion aggravation, the release of fuel fission gas Increase, internal pressure becomes larger.Since involucrum is unique barrier that fission gas is discharged into primary Ioops, high burnup operation improves involucrum Risk that is damaged and then causing radioactive substance to discharge, especially under accident conditions.
In recent years, dispersion fuel is used for high temperature gas cooled reactor, i.e., by TRISO particle dispersion in graphite matrix.TRISO Grain is successively coated loose pyrolytic carbon layer, inside solid pyrolytic carbon layer (IPyC), SiC layer and external fine and close pyrolysis by cartridge in vitro Carbon-coating (OPyC) is constituted.In consideration of it, proposing the concept that dispersion fuel is applied to water cooled reator in the world, i.e., by TRISO particle Disperse is in being prepared into fuel pellet in SiC matrix, as shown in Figure 2.The SiC matrix and TRISO particle SiC of the fuel pellet coat Layer can play the role of fission product containing, can effectively limit fission gas and be discharged into pellet-cladding gap, so as to mention The safety of high fuel rod, and increase fuel high burnup operation potentiality.
But there are following technological deficiencies for the above dispersion fuel pellet:
1) TRISO fuel particle is also distributed in above-mentioned dispersion fuel pellet periphery or even some particle is exposed to core Block surface is easy to cause under accident conditions to weaken function of the SiC matrix as second fission product barrier TRISO particle and matrix separation, destroy pellet structural intergrity;
2) sintered pellet size is generally unsatisfactory for drawing requirement, needs to carry out grinding.Above-mentioned pellet is being ground When be easily destroyed the TRISO particle for being distributed in pellet periphery, the fuel core even resulted in inside TRISO particle is exposed, thus Pellet is caused to be scrapped.
Document " Progress on matrix SiC processing and properties for fully ceramic microencapsulated fuel form.K.A.Terrani,J.O.Kiggans,C.M.Silva.Journal 457 (2015) 9-17 " of of Nuclear Materials describes two kinds of preparation methods without fuel protective layer: one is use SiC powder dry-pressing at sleeve, later with dispersion fuel pellet hot pressed sintering, however due in sintering process TRISO particle it is outside Migration, so that there is also fuel particles for pellet periphery, can not play a protective role;Two is using the windings of long SiC fibrage body On the outside of pellet, NITE-SiC suspension is impregnated, later hot pressed sintering together, during the sintering process due to the resistance of long SiC fiber Hinder effect, TRISO particle cannot migrate, and pellet be can effectively protect, but there is problems in that 1) long SiC fibrage Body is expensive, and pellet is at high cost;2) long SiC fibrage body sintering activity is poor, and densification is difficult, leads to no fuel particle layer (i.e. protective layer) consistency is lower, weak to fission gas entrapments power;3) long SiC fibrage body and dispersion fuel pellet property are poor It is different larger, it is difficult to which that synchronous sintering, the fuel pellet internal stress of preparation is big, and application risk is high.
Summary of the invention
Present invention solves the technical problem that: the present invention provides a kind of novel dispersion fuel and its manufacturing method, is able to solve Dispersion fuel TRISO distribution of particles is unreasonable in the prior art and the defect of poor processability.
The technical solution adopted by the present invention:
A kind of novel dispersion fuel, including column pellet and involucrum, involucrum are wrapped in outside column pellet, column pellet packet It including fuel region and without fuel bed, no fuel bed is wrapped in outside fuel region, fuel region includes TRISO particle and SiC matrix, TRISO particle dispersion is in SiC ceramic matrix.
The TRISO particle is spherical structure, is followed successively by fuel core, loose pyrolytic carbon layer, inside solid from inside to outside Pyrolytic carbon layer, compact silicon carbide layer, external fine and close pyrolytic carbon layer.
The fuel core is uranium nitride core or UO2-PuO2Core;The diameter of fuel core is 800 μm -1000 μm.
The column pellet contains chamfering and butterfly structure, and can according to need disperse in column pellet has erbium oxide flammable Poisonous substance.
The material of the no fuel region is SiC/SiC short fiber composite material, with a thickness of 0.1mm~2mm.
A kind of manufacturing method of dispersion fuel, includes the following steps:
Step 1 mixes TRISO particle with nano grade Sic powder, 5wt% sintering aid, prepares column pellet green compact;
Step 2 prepares SiC/SiC short fiber composite material green tape using casting molding processes;
SiC/SiC short fiber composite material green tape is wound in solid core rod iron surface by step 3, and winding layer number is 2~5 layers, Rodlike solid core steel surface is smooth, no significant defect, and surface is coated with dimethicone as release agent, has SiC raw surface wrap The columnar core of band does isostatic pressing, and waiting the pressure of static pressure is 80~200MPa, and the dwell time is 20~200s, the static pressure such as general Green compact afterwards, take off from columnar core, obtain cylindrical shape without fuel region green compact;
Step 4, by SiC/SiC short fiber composite material green tape multiple-layer stacked, being superimposed the number of plies is 2~10 layers, stamped system It is standby at disc-shaped without fuel region green compact;
Rod fuel area green compact are placed in cylindrical shape without in fuel region green compact by step 5, and placement disc-shaped is without fuel bed up and down Green compact are prepared into column pellet through hot pressed sintering, and sintering atmosphere is argon gas, and pressure 15MPa, sintering temperature is 1850 DEG C, is burnt The knot time is 1h;
Step 6 carries out grinding to column pellet, obtains novel dispersion fuel pellet.
In the step 2, the tape casting manufacturing method of SiC/SiC short fiber composite material green tape, specific steps are such as Under:
SiC fiber is cut to the staple fiber that length is 4~8mm by step 2.1, and SiC powder and sintering aid, sintering Auxiliary agent A l2O3:Y2O3Molar ratio be 3:2, ball milling mixing, wherein the volume ratio of SiC fiber and SiC particulate be 35:65, sintering Auxiliary agent accounts for 4~8wt.% of whole SiC total amounts, and ball-milling medium is dehydrated alcohol, incorporation time 8h, ratio of grinding media to material 5:1, mixing By 60 DEG C of dry acquisition mixed powders;
Step 2.2, by 50~60wt.% mixed powder, with 30~45wt.% organic solvent, wherein alcohol and toluene Volume ratio is 2:3 and 0.5~2wt.% dispersing agent tetramethylammonium hydroxide mixes, and ball milling 8h obtains the suspension of stable dispersion;
Step 2.3, into the suspension of acquisition, addition 4~8wt.% bonding agent, 2~6wt.% plasticizer and 1wt.% disappear Infusion, ball milling mixing 2h, 10~40min of de-bubble, obtains the SiC/SiC short fiber composite material of stable dispersion under vacuum conditions Slurry;
Step 2.4 pours into the SiC/SiC short fiber composite material slurry of acquisition in the slurry funnel of casting machine, carries out Tape casting, curtain coating speed are 20cm/min~40cm/min, and drying temperature is 50 DEG C, and edge height can for 30 μm~50 μm It adjusts, dry SiC/SiC short fiber composite material green tape is removed from casting machine, obtain the green tape with a thickness of 30-50 μm.
Beneficial effects of the present invention:
A kind of novel dispersion fuel provided by the invention and its manufacturing method, are able to solve dispersion fuel in the prior art TRISO distribution of particles is unreasonable and the defect of poor processability.
Detailed description of the invention
Fig. 1 is a kind of novel dispersion fuel structural schematic diagram provided by the invention;
Fig. 2 is that background technique is related to dispersion fuel structural schematic diagram;
Fig. 3 is TRISO particle schematic diagram;
In figure: 1- includes inner fuel area and external column pellet, 2- involucrum, 11-TRISO particle, 12- without fuel bed SiC matrix, 13- do not include the external column pellet without fuel bed, 31- disperse at TRISO of intrinsic silicon without fuel bed, 3- Grain, 32- are destroyed and are exposed to the TRISO particle on surface, 33-SiC matrix, 111- fuel core, 112- due to centerless grinding Loose pyrolytic carbon layer, 113- inside solid pyrolytic carbon layer (IPyC), 114- compact silicon carbide layer, the fine and close pyrolytic carbon layer in the outside 115- (OPyC)。
Specific embodiment
A kind of novel dispersion fuel provided by the invention and its manufacturing method are made in the following with reference to the drawings and specific embodiments It is further described.
Embodiment 1
As shown in Figure 1, a kind of novel dispersion fuel provided by the invention, including column pellet 1 and involucrum 2, involucrum 2 wrap up Outside column pellet 1, including fuel region and without fuel bed 13, no fuel bed 13 is wrapped in outside fuel region column pellet 1, combustion Expect that area includes TRISO particle 11 and SiC matrix 12, TRISO particle dispersion is in SiC ceramic matrix 12;As shown in figure 3, TRISO Particle 11 is spherical structure, is followed successively by fuel core 111, loose pyrolytic carbon layer 112, inside solid pyrolytic carbon layer from inside to outside (IPyC) 113, compact silicon carbide layer 114, external fine and close pyrolytic carbon layer (OPyC) 115.
Fuel core 111 is uranium nitride core.The diameter of fuel core 111 is 800 μm.
The diameter of column pellet 1 is 8mm~9mm, is highly 10mm~15mm, contains chamfering and butterfly structure.Column core Disperse has erbium oxide burnable poison in block 1.
The material of no fuel region is SiC/SiC short fiber composite material, with a thickness of 0.1mm~2mm.
Embodiment 2
The present embodiment the difference from embodiment 1 is that:
Fuel core 111 is UO2-PuO2Core, UO2-PuO2Core diameter is 800 μm -1000 μm.
The diameter of column pellet 1 is 10mm~14mm, is highly 10mm~15mm, and erbium oxide is not contained in column pellet 1 Burnable poison.
Embodiment 3
The present embodiment provides a kind of manufacturing methods of dispersion fuel, include the following steps:
Step 1 mixes TRISO particle 11 with nano grade Sic powder, 5wt% sintering aid, and preparation column pellet 1 is raw Base, diameter 13mm are highly 15mm;
Step 2 prepares SiC/SiC short fiber composite material green tape using casting molding processes;
SiC/SiC short fiber composite material green tape is wound in solid core rod iron surface by step 3, and winding layer number is 2~5 layers, Rodlike solid core steel surface is smooth, no significant defect, and surface is coated with dimethicone as release agent, has SiC raw surface wrap The columnar core 1 of band does isostatic pressing, and waiting the pressure of static pressure is 80~200MPa, and the dwell time is 20~200s, and general etc. is quiet Green compact after pressure are taken off from columnar core 1, and acquisition cylindrical shape is without 13 green compact of fuel region, with a thickness of 200 μm, internal diameter 13.5mm, Height is 15mm;
Step 4, by SiC/SiC short fiber composite material green tape multiple-layer stacked, being superimposed the number of plies is 2~10 layers, stamped system It is standby at disc-shaped without 13 green compact of fuel region, with a thickness of 200 μm, diameter 13.5mm;
13 green compact of rod fuel area are placed in cylindrical shape without in fuel region green compact by step 5, and placement disc-shaped is without fuel up and down Layer green compact are prepared into column pellet 1 through hot pressed sintering, and sintering atmosphere is argon gas, and pressure 15MPa, sintering temperature is 1850 DEG C, Sintering time is 1h;
Step 6 carries out grinding to column pellet 1, obtains the novel dispersion fuel pellet of specific dimensions.
In step 2, the tape casting manufacturing method of SiC/SiC short fiber composite material green tape, the specific steps of which are as follows:
SiC fiber is cut to the staple fiber that length is 4~8mm by step 2.1, with SiC powder and sintering aid (Al2O3: Y2O3=3:2, molar ratio) ball milling mixing, wherein the volume ratio of SiC fiber and SiC particulate is 35:65, and sintering aid accounts for whole 4~8wt.% of SiC total amount, ball-milling medium are dehydrated alcohol, and incorporation time 8h, ratio of grinding media to material 5:1 are dry through 60 DEG C after mixing Dry acquisition mixed powder;
Step 2.2, by 50~60wt.% mixed powder, with the (mixing of alcohol and toluene of 30~45wt.% organic solvent Liquid, wherein alcohol is that 2:3) and 0.5~2wt.% dispersing agent (tetramethylammonium hydroxide) mix with the volume ratio of toluene, ball milling The suspension of 8h acquisition stable dispersion;
4~8wt.% bonding agent (PVB), 2~6wt.% plasticizer (adjacent benzene are added into the suspension of acquisition for step 2.3 Dibutyl carboxylic acid) and 1wt.% defoaming agent (n-butanol), ball milling mixing 2h, 10~40min of de-bubble, obtains under vacuum conditions The SiC/SiC short fiber composite material slurry of stable dispersion;
Step 2.4 pours into the SiC/SiC short fiber composite material slurry of acquisition in the slurry funnel of casting machine, carries out Tape casting, curtain coating speed are 20cm/min~40cm/min, and drying temperature is 50 DEG C, and edge height can for 30 μm~50 μm It adjusts, dry SiC/SiC short fiber composite material green tape is removed from casting machine, obtain the green tape with a thickness of 30-50 μm.

Claims (7)

1. a kind of novel dispersion fuel, it is characterised in that: including column pellet (1) and involucrum (2), involucrum (2) is wrapped in column Pellet (1) is external, and column pellet (1) includes fuel region and without fuel bed (13), and no fuel bed (13) is wrapped in outside fuel region, Fuel region includes TRISO particle (11) and SiC matrix (12), and TRISO particle dispersion is in SiC ceramic matrix (12).
2. a kind of novel dispersion fuel according to claim 1, it is characterised in that: the TRISO particle (11) is spherical shape Structure is followed successively by fuel core (111), loose pyrolytic carbon layer (112), inside solid pyrolytic carbon layer (113), densification from inside to outside Silicon carbide layer (114), external fine and close pyrolytic carbon layer (115).
3. a kind of novel dispersion fuel according to claim 2, it is characterised in that: the fuel core (111) is nitridation Uranium core or UO2-PuO2Core;The diameter of fuel core (111) is 800 μm -1000 μm.
4. a kind of novel dispersion fuel according to claim 1, it is characterised in that: the column pellet (1) contains chamfering And butterfly structure, can according to need disperse in column pellet (1) has erbium oxide burnable poison.
5. a kind of novel dispersion fuel according to claim 1, it is characterised in that: the material of the no fuel region is SiC/ SiC short fiber composite material, with a thickness of 0.1mm~2mm.
6. a kind of manufacturing method of dispersion fuel, characterized by the following steps:
Step (1) mixes TRISO particle (11) with nano grade Sic powder, 5wt% sintering aid, prepares column pellet (1) Green compact;
Step (2) prepares SiC/SiC short fiber composite material green tape using casting molding processes;
SiC/SiC short fiber composite material green tape is wound in solid core rod iron surface by step (3), and winding layer number is 2~5 layers, stick Shape solid core steel surface is smooth, no significant defect, and surface is coated with dimethicone as release agent, and surface wrap is had SiC green tape Columnar core (1) do isostatic pressing, wait static pressure pressure be 80~200MPa, the dwell time be 20~200s, will etc. it is quiet Green compact after pressure are taken off from columnar core (1), obtain cylindrical shape without fuel region (13) green compact;
Step (4), by SiC/SiC short fiber composite material green tape multiple-layer stacked, being superimposed the number of plies is 2~10 layers, stamped preparation At disc-shaped without fuel region (13) green compact;
Rod fuel area (13) green compact are placed in cylindrical shape without in fuel region green compact by step (5), and placement disc-shaped is without fuel up and down Layer green compact, are prepared into column pellet (1), sintering atmosphere is argon gas, pressure 15MPa, sintering temperature 1850 through hot pressed sintering DEG C, sintering time 1h;
Step (6) carries out grinding to column pellet (1), obtains novel dispersion fuel pellet.
7. a kind of manufacturing method of dispersion fuel according to claim 6, it is characterised in that: in the step (2), SiC/ The tape casting manufacturing method of SiC short fiber composite material green tape, the specific steps of which are as follows:
SiC fiber is cut to the staple fiber that length is 4~8mm by step (2.1), and SiC powder and sintering aid, sintering helps Agent Al2O3:Y2O3Molar ratio be 3:2, ball milling mixing, wherein the volume ratio of SiC fiber and SiC particulate is 35:65, and sintering helps Agent accounts for 4~8wt.% of whole SiC total amounts, and ball-milling medium is dehydrated alcohol, incorporation time 8h, ratio of grinding media to material 5:1, after mixing Through 60 DEG C of dry acquisition mixed powders;
Step (2.2), by 50~60wt.% mixed powder, with 30~45wt.% organic solvent, the wherein body of alcohol and toluene Product is than being 2:3 and the mixing of 0.5~2wt.% dispersing agent tetramethylammonium hydroxide, the suspension of ball milling 8h acquisition stable dispersion;
4~8wt.% bonding agent, 2~6wt.% plasticizer and 1wt.% defoaming are added into the suspension of acquisition for step (2.3) Agent, ball milling mixing 2h, 10~40min of de-bubble, obtains the SiC/SiC short fiber composite material slurry of stable dispersion under vacuum conditions Material;
Step (2.4) pours into the SiC/SiC short fiber composite material slurry of acquisition in the slurry funnel of casting machine, is flowed Prolong molding, curtain coating speed is 20cm/min~40cm/min, and drying temperature is 50 DEG C, and edge height is 30 μm~50 μm adjustable, Dry SiC/SiC short fiber composite material green tape is removed from casting machine, obtains the green tape with a thickness of 30-50 μm.
CN201711498475.8A 2017-12-29 2017-12-29 A kind of novel dispersion fuel and its manufacturing method Pending CN109994223A (en)

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CN113611435A (en) * 2021-08-17 2021-11-05 西北工业大学 Ceramic composite fuel pellet and preparation method and application thereof
CN113936818A (en) * 2021-09-02 2022-01-14 中国核电工程有限公司 Homogenized coated particle dispersed fuel and preparation method thereof
CN114038583A (en) * 2021-11-17 2022-02-11 中国核动力研究设计院 Full ceramic fuel rod
CN115132380A (en) * 2022-07-08 2022-09-30 中国核动力研究设计院 Dispersion micro-packaging rod-shaped fuel element and heat pipe reactor for combusting same
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CN111508628A (en) * 2020-04-17 2020-08-07 中国科学院合肥物质科学研究院 Preparation method of tungsten or molybdenum-based fuel pellet with uranium dioxide core balls dispersed and distributed
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CN112233820A (en) * 2020-10-15 2021-01-15 哈尔滨工程大学 Reactor fuel assembly and reactor core structure
CN113611435A (en) * 2021-08-17 2021-11-05 西北工业大学 Ceramic composite fuel pellet and preparation method and application thereof
CN113936818A (en) * 2021-09-02 2022-01-14 中国核电工程有限公司 Homogenized coated particle dispersed fuel and preparation method thereof
CN113936818B (en) * 2021-09-02 2022-11-25 中国核电工程有限公司 Homogenized coated particle dispersed fuel and preparation method thereof
WO2023029317A1 (en) * 2021-09-02 2023-03-09 中国核电工程有限公司 Homogenized coated particle dispersion fuel and preparation method theref
CN114038583A (en) * 2021-11-17 2022-02-11 中国核动力研究设计院 Full ceramic fuel rod
CN114038583B (en) * 2021-11-17 2023-11-21 中国核动力研究设计院 Full ceramic fuel rod
CN115132380A (en) * 2022-07-08 2022-09-30 中国核动力研究设计院 Dispersion micro-packaging rod-shaped fuel element and heat pipe reactor for combusting same
CN115132378A (en) * 2022-07-08 2022-09-30 中国核动力研究设计院 ODS (oxide dispersion strengthened) stainless steel-based dispersion micro-packaging rod-shaped fuel element and reactor
CN115132379A (en) * 2022-07-08 2022-09-30 中国核动力研究设计院 Dispersion micro-packaging rod-shaped fuel element adopting refractory metal base and reactor

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