CN108039210A - Fuel pellet and its manufacture method - Google Patents

Fuel pellet and its manufacture method Download PDF

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Publication number
CN108039210A
CN108039210A CN201711059000.9A CN201711059000A CN108039210A CN 108039210 A CN108039210 A CN 108039210A CN 201711059000 A CN201711059000 A CN 201711059000A CN 108039210 A CN108039210 A CN 108039210A
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CN
China
Prior art keywords
urania
powder
fuel pellet
manufacture method
oxide
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.)
Pending
Application number
CN201711059000.9A
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Chinese (zh)
Inventor
黄华伟
刘彤
李锐
任啟森
孙茂州
马赵丹丹
高思宇
薛佳祥
龚星
彭振驯
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
China General Nuclear Power Corp
China Nuclear Power Technology Research Institute Co Ltd
CGN Power Co Ltd
China Nuclear Power Institute Co Ltd
Original Assignee
China General Nuclear Power Corp
China Nuclear Power Technology Research Institute Co Ltd
CGN Power Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by China General Nuclear Power Corp, China Nuclear Power Technology Research Institute Co Ltd, CGN Power Co Ltd filed Critical China General Nuclear Power Corp
Priority to CN201711059000.9A priority Critical patent/CN108039210A/en
Publication of CN108039210A publication Critical patent/CN108039210A/en
Priority to PCT/CN2018/101364 priority patent/WO2019085592A1/en
Pending legal-status Critical Current

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Classifications

    • 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
    • G21C21/10Manufacture of fuel elements or breeder elements contained in non-active casings by extrusion, drawing, or stretching by rolling, e.g. "picture frame" technique
    • 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
    • G21C21/16Manufacture of fuel elements or breeder elements contained in non-active casings by casting or dipping techniques
    • 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
    • G21C3/62Ceramic fuel
    • G21C3/623Oxide fuels
    • 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)
  • Chemical & Material Sciences (AREA)
  • Ceramic Engineering (AREA)
  • Monitoring And Testing Of Nuclear Reactors (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Compositions Of Oxide Ceramics (AREA)

Abstract

The invention discloses a kind of fuel pellet and its manufacture method, the manufacture method of fuel pellet includes:S1, weigh raw material:Chromium oxide 0 2%, aluminium oxide 0 2%, silica 0 2%, niobium oxide 0 2%, surplus is urania;Raw material ball milling, be uniformly mixed by S2, forms mixed-powder;S3, suppress mixed-powder to form urania biscuit and high temperature pre-burning;S4, crushed urania biscuit, sieved, and wears into urania particle;S5, mix beryllium oxide powder in urania particle, is mixed to form and treats press-powder material;Each urania particle surface is coated with the clad of beryllium oxide powder formation;S6, will treat that simultaneously densification sintering is pressed in press-powder material, and fuel pellet is made.The present invention is by the way of secondary addition compound, double sintering, sintering aid is set to be dissolved or be distributed in urania matrix, reduce sintering aid diffusion or be solid-solution in beryllium oxide, it is ensured that on the premise of sintering aid does not influence the capacity of heat transmission of BeO phases, effectively increase pellet crystallite dimension and improve sintering activity.

Description

Fuel pellet and its manufacture method
Technical field
The present invention relates to nuclear fuel element technical field, more particularly to a kind of fuel pellet and its manufacture method.
Background technology
Due to UO2Have the advantages that fusing point is high, stability is good, irradiation behaviour is good, the commercial nuclear reactor of the whole world overwhelming majority Fuel element all use UO2As fuel pellet.However, UO2Ceramic thermal conductivity is low, and fuel pellet is formed during military service Larger temperature gradient, core temperature reach more than 1500 DEG C.Big temperature gradient causes pellet to produce thermal stress, high pellet Temperature causes fission gas release rate to increase, this is unfavorable for the increase of fuel element burnup, affects the security and warp of nuclear power Ji property.
In order to reduce pellet thermal stress, fission gas release rate is reduced, the second phase of high heat conductance is added in pellet Compound, such as BeO, SiC, Nano diamond, become the hot spot for improving fuel pellet performance.Meanwhile fission gas release also by The influence of crystallite dimension, adds micro sintering aid, and it is the important research for reducing fission gas release to promote pellet crystal grain to grow up Direction.
BeO chemical stabilities are good, and neutron absorption cross-section is small, with UO2There is good compatibility, be to improve UO2Pellet thermal conductivity Important candidate compound.BeO and UO2It is oxide, UO2The technique of/BeO pellets is similar to UO2 pellets, industrial applications Prospect is good.It is however, uniform, continuously distributed in UO2The BeO of matrix suppresses ion diffusion to a certain extent, hinders pellet fine and close Grow up with crystal grain.Cr is directly added using conventional2O3、Al2O3Powder sintered activity can be improved etc. sintering aid, but may be with BeO reacts, and influences heat conductivility and the distribution of BeO phases, is unfavorable for the raising of pellet thermal conductivity.
Therefore, in order to obtain the UO of high heat conductance, big crystal grain2Pellet, the addition manner of sintering aid become urgent need to resolve Key issue.
The content of the invention
The technical problem to be solved in the present invention is, there is provided a kind of combustion for increasing pellet crystallite dimension and improving sintering activity Expect the manufacture method of pellet and obtained fuel pellet.
The technical solution adopted by the present invention to solve the technical problems is:A kind of manufacture method of fuel pellet is provided, is wrapped Include following steps:
S1, according to mass percent weigh following raw material:Chromium oxide 0-2%, aluminium oxide 0-2%, silica 0-2%, Niobium oxide 0-2%, surplus are urania;At least one of the chromium oxide, aluminium oxide, silica and niobium oxide quality is not 0;
The raw material ball milling, be uniformly mixed by S2, forms mixed-powder;
S3, suppress the mixed-powder to form urania biscuit and carry out high temperature pre-burning;
S4, crushed the urania biscuit after high temperature pre-burning, sieved, and ball milling forms urania particle;
S5, mix beryllium oxide powder in urania particle, is mixed to form and treats press-powder material;Urania described in each of which The surface of particle is coated with the clad that the beryllium oxide powder is formed;
S6, by described treat that press-powder material is pressed and carries out densification sintering, and fuel pellet is made.
Preferably, in step S1, the particle diameter of the chromium oxide is 20nm-20 μm;The particle diameter of the aluminium oxide is 10nm-30 μm;The particle diameter of the silica is 10nm-50 μm;The particle diameter of the niobium oxide is 10nm-30 μm;The particle diameter of the urania is 0.5μm-50μm。
Preferably, in step S3, the pressure of compacting is 50-300Mpa.
Preferably, in step S3, the urania biscuit radius of formation is 10mm-100mm, is highly 10-100mm.
Preferably, in step S3, the temperature of high temperature pre-burning is 600 DEG C -1500 DEG C, soaking time 1-8h.
Preferably, in step S5, the particle diameter of the beryllium oxide powder is 500nm-100 μm.
Preferably, in step S5, the mass percent of the beryllium oxide powder is 1-5%.
Preferably, in step S6, compressing pressure is 100-300MPa.
Preferably, in step S6, densification sintering carries out under inertia or reducing atmosphere, the temperature of sintering for 1600 DEG C- 1800℃。
The present invention also provides a kind of fuel pellet, is made using above-mentioned manufacture method.
Beneficial effects of the present invention:By the way of secondary addition compound, double sintering so that the sintering aid of addition is consolidated It is molten or be distributed in urania matrix, reduce sintering aid and diffuse to or be solid-solution in beryllium oxide, it is ensured that sintering aid does not influence BeO phases The capacity of heat transmission on the premise of, it is effective to increase pellet crystallite dimension and improve sintering activity.
Brief description of the drawings
Below in conjunction with accompanying drawings and embodiments, the invention will be further described, in attached drawing:
Fig. 1 is the manufacture method flow chart of the fuel pellet of the present invention;
Fig. 2 is the structure figure of the fuel pellet of embodiment 1 in the present invention.
Embodiment
In order to which the technical features, objects and effects of the present invention are more clearly understood, now compare attached drawing and describe in detail The embodiment of the present invention.
With reference to figure 1, the manufacture method of fuel pellet of the invention, it may include following steps:
S1, according to mass percent weigh following raw material:Chromium oxide (Cr2O3) 0-2%, aluminium oxide (Al2O3) 0-2%, Silica (SiO2) 0-2%, niobium oxide (Nb2O5) 0-2%, surplus is urania (UO2);Chromium oxide, aluminium oxide, silica and At least one of niobium oxide quality is not 0.
Each raw material is powdered, and wherein the particle diameter of chromium oxide is 20nm-20 μm, and the particle diameter of aluminium oxide is 10nm-30 μm, The particle diameter of silica is 10nm-50 μm, and the particle diameter of niobium oxide is 10nm-30 μm, and the particle diameter of urania is 0.5 μm -50 μm.Oxidation Uranium is major ingredient, the main component as matrix;Chromium oxide, aluminium oxide, silica and niobium oxide are sintering aid.
Raw material ball milling, be uniformly mixed by S2, forms mixed-powder.
Ball milling mixing can carry out on tumbling ball mill or planetary ball mill.
S3, suppress mixed-powder to form urania biscuit and carry out high temperature pre-burning.
Wherein, the pressure of compacting is 50-300Mpa.High temperature pre-burning may be selected to carry out in high-temperature atmosphere furnace;High temperature pre-burning Temperature be 600 DEG C -1500 DEG C, soaking time 1-8h.The urania biscuit radius of formation can be 10mm-100mm, highly be 10-100mm。
S4, crushed the urania biscuit after high temperature pre-burning, sieved, and ball milling forms approximate sphericity or spherical oxidation Uranium particle.
Ball-milling Time can according to circumstances depending on, such as 1-20h (hour).
S5, will mix beryllium oxide (BeO) powder in urania particle, be mixed to form and treat press-powder material.
Wherein, the surface of each urania particle is coated with the clad of beryllium oxide powder formation.
The mass percent of beryllium oxide powder is the 1-5% of urania particle total amount.The particle diameter of beryllium oxide powder is 500nm-100μm。
S6, will treat that press-powder material is pressed and carries out densification sintering, and fuel pellet is made.
In step S6, compressing pressure is 100-300Mpa, is suppressed using compression molding mode.
Densification sintering is make it that compressing pellet base substrate is fine and close using pressureless sintering;The densification sintering be Carried out under inertia or reducing atmosphere, the temperature of sintering is 1600 DEG C -1800 DEG C.The inert gases such as argon gas may be selected in inert atmosphere, The reducing gas such as hydrogen may be selected in reducing atmosphere.
Obtained fuel pellet, can require according to size, using centerless grinder, obtain the pellet for meeting size requirement.
Fuel pellet made from the manufacturing method of the present invention, pellet crystallite dimension of the pellet crystallite dimension compared with the prior art Greatly.
Below by way of specific embodiment, the present invention is further described.
Embodiment 1
Weigh the Cr of 1 μm of particle diameter2O3Powder 0.5wt.%;Surplus is the UO of 0.5 μm of particle diameter2Powder.Each powder is inserted into ball In grinding jar, uniformly mixed on tumbling ball mill or planetary ball mill.By mixed-powder it is compressing be urania biscuit, pressure 100MPa, molding UO2Biscuit radius φ 50mm, height 20mm.By UO2Biscuit pre-burning in high-temperature atmosphere furnace, sintering temperature 100 DEG C, soaking time 4h.Pellet after pre-burning is crushed, is sieved, the UO of almost spherical is then obtained by the way of autogenous grinding2 Particle;In UO2The BeO powder of 2.5wt.%, mixing, in UO are added in particle2Particle surface coats one layer of BeO powder.Using mould Molded mode, pressing pressure 200MPa, will be coated with the UO of BeO powder2Particle is pressed into pellet;In inertia or reducing atmosphere Under, make pellet fine and close using pressureless sintering, 1700 DEG C of sintering temperature, obtains fuel pellet.
The metallograph of obtained fuel pellet is as shown in Fig. 2, component is uniform in pellet, density >=96%T.D, oxygen metal raw Son is than being 1.99~2.01, and impurity content meets the requirements, and the thermal conductivity and intensive properties of pellet are good.
Embodiment 2
Weigh the Cr of 1 μm of particle diameter2O3Powder 0.5wt.%;The Al that 1 μm of particle diameter2O3Powder 0.2wt.%;Surplus is particle diameter 0.5 μm of UO2Powder.Each powder is inserted in ball grinder, is uniformly mixed on tumbling ball mill or planetary ball mill.Will mixing Powder pressing forming is UO2Biscuit, pressure 100MPa, molding UO2Biscuit radius φ 50mm, height 20mm.By urania biscuit The pre-burning in high-temperature atmosphere furnace, 100 DEG C of sintering temperature, soaking time 4h.Pellet after pre-burning is crushed, is sieved, is then used The mode of autogenous grinding obtains the UO of almost spherical2Particle;In UO2The BeO powder of 2.5wt.%, mixing, in UO are added in particle2 Grain surface coats one layer of BeO powder.Using compression molding mode, pressing pressure 200MPa, will be coated with the UO of BeO powder2 Grain is pressed into pellet;Under inertia or reducing atmosphere, make pellet fine and close using pressureless sintering, 1700 DEG C of sintering temperature, is fired Expect pellet.
Embodiment 3
Weigh the Nb of 1 μm of particle diameter2O5Powder 0.5wt.%, the Al that 1 μm of particle diameter2O3Powder 0.2wt.%;Surplus is particle diameter 0.5 μm of UO2Powder.Each powder is inserted in ball grinder, is uniformly mixed on tumbling ball mill or planetary ball mill.Will mixing Powder pressing forming is urania biscuit, pressure 100MPa, molding urania biscuit radius φ 50mm, height 20mm.By oxygen Change the pre-burning in high-temperature atmosphere furnace of uranium biscuit, 100 DEG C of sintering temperature, soaking time 4h.Pellet after pre-burning is crushed, is sieved, Then the UO of almost spherical is obtained by the way of autogenous grinding2Particle;In UO2The BeO powder of 2.5wt.% is added in particle, is mixed, In UO2Particle surface coats one layer of BeO powder.Using compression molding mode, pressing pressure 200MPa, will be coated with BeO powder UO2Particle is pressed into pellet;Under inertia or reducing atmosphere, make pellet fine and close using pressureless sintering, 1700 DEG C of sintering temperature, Obtain fuel pellet.
The metallograph of the fuel pellet of embodiment 2 and embodiment 3 refers to Fig. 2.
The foregoing is merely the embodiment of the present invention, is not intended to limit the scope of the invention, every to utilize this hair The equivalent structure or equivalent flow shift that bright specification and accompanying drawing content are made, is directly or indirectly used in other relevant skills Art field, is included within the scope of the present invention.

Claims (10)

1. a kind of manufacture method of fuel pellet, it is characterised in that comprise the following steps:
S1, according to mass percent weigh following raw material:Chromium oxide 0-2%, aluminium oxide 0-2%, silica 0-2%, niobium oxide 0- 2%, surplus is urania;At least one of the chromium oxide, aluminium oxide, silica and niobium oxide quality is not 0;
The raw material ball milling, be uniformly mixed by S2, forms mixed-powder;
S3, suppress the mixed-powder to form urania biscuit and carry out high temperature pre-burning;
S4, crushed the urania biscuit after high temperature pre-burning, sieved, and ball milling forms urania particle;
S5, mix beryllium oxide powder in urania particle, is mixed to form and treats press-powder material;Urania particle described in each of which Surface be coated with the clad that the beryllium oxide powder is formed;
S6, by described treat that press-powder material is pressed and carries out densification sintering, and fuel pellet is made.
2. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S1, the chromium oxide Particle diameter is 20nm-20 μm;The particle diameter of the aluminium oxide is 10nm-30 μm;The particle diameter of the silica is 10nm-50 μm;It is described The particle diameter of niobium oxide is 10nm-30 μm;The particle diameter of the urania is 0.5 μm -50 μm.
3. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S3, the pressure of compacting is 50-300Mpa。
4. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S3, the urania of formation Biscuit radius is 10mm-100mm, is highly 10-100mm.
5. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S3, the temperature of high temperature pre-burning Spend for 600 DEG C -1500 DEG C, soaking time 1-8h.
6. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S5, the beryllium oxide powder The particle diameter at end is 500nm-100 μm.
7. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S5, the beryllium oxide powder The mass percent at end is 1-5%.
8. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S6, compressing pressure Power is 100-300MPa.
9. the manufacture method of fuel pellet according to claim 1, it is characterised in that in step S6, densification sintering exists Carried out under inertia or reducing atmosphere, the temperature of sintering is 1600 DEG C -1800 DEG C.
10. a kind of fuel pellet, it is characterised in that using the manufacture method of claim 1-9 any one of them fuel pellets It is made.
CN201711059000.9A 2017-11-01 2017-11-01 Fuel pellet and its manufacture method Pending CN108039210A (en)

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PCT/CN2018/101364 WO2019085592A1 (en) 2017-11-01 2018-08-20 Fuel pellet and manufacturing method therefor

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CN108806804A (en) * 2018-05-28 2018-11-13 广东核电合营有限公司 Fibre-reinforced fuel pellets of SiC and preparation method thereof
CN109300560A (en) * 2018-11-01 2019-02-01 中国原子能科学研究院 A kind of mixed oxide pellet sintering atmosphere oxygen gesture control device
WO2019085592A1 (en) * 2017-11-01 2019-05-09 中广核研究院有限公司 Fuel pellet and manufacturing method therefor
CN110827998A (en) * 2019-11-21 2020-02-21 中国核动力研究设计院 Beryllium oxide moderated metal cooling reactor miniaturization design method and reactor
CN112334991A (en) * 2018-06-21 2021-02-05 西屋电气公司瑞典分公司 Fuel pellet
CN112735618A (en) * 2020-12-30 2021-04-30 中核北方核燃料元件有限公司 Preparation method of SiC-based UCO core fuel pellet

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Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2019085592A1 (en) * 2017-11-01 2019-05-09 中广核研究院有限公司 Fuel pellet and manufacturing method therefor
CN108806804A (en) * 2018-05-28 2018-11-13 广东核电合营有限公司 Fibre-reinforced fuel pellets of SiC and preparation method thereof
CN112334991A (en) * 2018-06-21 2021-02-05 西屋电气公司瑞典分公司 Fuel pellet
CN112334991B (en) * 2018-06-21 2024-05-07 西屋电气公司瑞典分公司 Fuel pellet
CN109300560A (en) * 2018-11-01 2019-02-01 中国原子能科学研究院 A kind of mixed oxide pellet sintering atmosphere oxygen gesture control device
CN109300560B (en) * 2018-11-01 2024-05-14 中国原子能科学研究院 Mixed oxide pellet sintering atmosphere oxygen potential control device
CN110827998A (en) * 2019-11-21 2020-02-21 中国核动力研究设计院 Beryllium oxide moderated metal cooling reactor miniaturization design method and reactor
CN110827998B (en) * 2019-11-21 2021-05-18 中国核动力研究设计院 Beryllium oxide moderated metal cooling reactor miniaturization design method and reactor
CN112735618A (en) * 2020-12-30 2021-04-30 中核北方核燃料元件有限公司 Preparation method of SiC-based UCO core fuel pellet
CN112735618B (en) * 2020-12-30 2022-06-28 中核北方核燃料元件有限公司 Preparation method of SiC-based UCO core fuel pellet

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Application publication date: 20180515