CN111326265B - Uranium dioxide-carbide composite fuel pellet and preparation method thereof - Google Patents

Uranium dioxide-carbide composite fuel pellet and preparation method thereof Download PDF

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CN111326265B
CN111326265B CN202010127901.2A CN202010127901A CN111326265B CN 111326265 B CN111326265 B CN 111326265B CN 202010127901 A CN202010127901 A CN 202010127901A CN 111326265 B CN111326265 B CN 111326265B
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uranium dioxide
fuel pellet
composite fuel
sintering
carbide composite
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CN111326265A (en
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程亮
张鹏程
严彪杰
高瑞
杨振亮
李冰清
褚明福
王志毅
黄奇奇
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Institute of Materials of CAEP
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    • 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
    • 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
    • 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

Abstract

The invention discloses a uranium dioxide-carbide composite fuel pellet and a preparation method thereof. According to the invention, the uranium dioxide and the carbide are separated by coating the uranium dioxide microsphere surface with the interface reaction inhibiting layer metal molybdenum, so that the reduction of the thermal conductivity of the carbide to the uranium dioxide caused by the high-temperature reaction of the uranium dioxide and the carbide to other compounds is avoided, and the interface reaction problem of the uranium dioxide-carbide composite fuel pellet is more effectively solved. In addition, the metal molybdenum has high heat conduction, high melting point, proper neutron absorption section and other nuclear properties, and has excellent high-temperature chemical compatibility with uranium dioxide and carbide, so that the interface reaction layer is inhibited from further improving the thermal conductivity of uranium dioxide.

Description

Uranium dioxide-carbide composite fuel pellet and preparation method thereof
Technical Field
The invention belongs to the field of powder metallurgy technology, advanced composite materials and reactor fission energy, and particularly relates to a uranium dioxide-carbide composite fuel pellet and a preparation method thereof.
Background
Sudden accident of the Japan Fudao Nuclear Power station of 3 months 2011, which causes the active commercial Nuclear reactor Fuel element UO 2 The safety reliability of Zr is severely questioned. UO under the new situation of rapid development of nuclear energy and higher intrinsic safety requirements 2 Zr fuel elements have failed to meet the requirements of higher intrinsic safety of the nuclear energy and of multi-application stack development in the future. The defect of low heat conductivity of the existing uranium dioxide fuel is exposed by the catastrophic nuclear power accident of the Fudawn, namely, the core waste heat cannot be effectively dissipated under the accident condition, so that the hidden danger of a molten pile exists. Thus, the most efficient way to date is to add a certain amount of highly thermally conductive second phase material to the uranium dioxide matrix. Among these, carbide (XC, x=si, zr) has excellent heat conductive properties, and has both a low neutron absorption cross section and a high melting point, and is preferably a second phase material.
However, in the high-temperature sintering densification process of the uranium dioxide-carbide composite fuel pellet, the uranium dioxide and the carbide can generate an interface reaction at high temperature to generate a U-C-X compound, so that the effect of the carbide on enhancing the thermal conductivity of the uranium dioxide is reduced, and the thermal stability and the chemical stability of the uranium dioxide under the working condition of high temperature near accidents are obviously influenced.
Therefore, in order to solve the problem of interface reaction between uranium dioxide and carbide in the high-temperature sintering preparation process and under the high-temperature near-accident working condition, so as to improve the thermal conductivity of the uranium dioxide-carbide composite fuel pellet, and be suitable for the more severe high Wen Shigu working condition, the development of a preparation method of the thermal conductivity enhanced composite fuel pellet for inhibiting the uranium dioxide-carbide interface reaction is urgently needed to solve the above problems.
Disclosure of Invention
Based on the above, the invention aims to solve the problem that the effect of carbide on enhancing the thermal conductivity of uranium dioxide is reduced because the uranium dioxide and carbide can undergo an interface reaction at high temperature, and provides the uranium dioxide-carbide composite fuel pellet, wherein the uranium dioxide surface in the uranium dioxide-carbide composite fuel pellet is coated with a layer of interface reaction inhibiting layer metal molybdenum formed by low-temperature presintering of metal molybdenum powder with the particle size of 20-800 nm.
Further, another object of the present invention is to provide a method for preparing a uranium dioxide-carbide composite fuel pellet, which specifically includes the following steps:
step S1: firstly, pre-pressing or presintering a uranium dioxide raw material, and then sequentially grinding, crushing, screening and physically micro-spheroidizing to obtain uranium dioxide microspheres with the particle size of 100-1000 mu m;
step S2: mixing uranium dioxide microspheres obtained in the step S1 with metal molybdenum powder according to the volume ratio of (80-95): 20-5, coating the metal molybdenum powder on the surfaces of the uranium dioxide microspheres through physical action, and then carrying out low-temperature presintering on the uranium dioxide microspheres coated with the metal molybdenum powder to obtain uranium dioxide microspheres coated with metal molybdenum of an interface reaction inhibiting layer;
step S3: uranium dioxide microspheres coated with the interface reaction inhibiting layer metal molybdenum and obtained in the step S2 and carbide particles with the particle size of 0.1-20 mu m are mixed according to the volume ratio of (75-98): (25-2) uniformly mixing under the protection of inert gas to obtain a mixture;
step S4: and (3) sintering the mixture obtained in the step (S3) by adopting any one mode of spark plasma sintering, hot-press sintering and pressureless atmosphere sintering to obtain the uranium dioxide-carbide composite fuel pellet.
Preferably, when the uranium dioxide raw material in the step S1 is pre-pressed, the pre-pressing is axial molding, the pressure is 100-600 MPa, and the dwell time is 0.5-30 min.
Preferably, when the uranium dioxide raw material in the step S1 is pre-sintered, the pre-sintering is non-pressure atmosphere sintering or discharge plasma sintering, wherein the temperature of the non-pressure atmosphere sintering is 600-1500 ℃, the heat preservation time is 0.5-12 h, the atmosphere is argon, the temperature of the discharge plasma sintering is 200-1100 ℃, the heat preservation time is 0.2-30 min, and the atmosphere is argon or vacuum.
Preferably, the uranium dioxide microspheres and the metallic molybdenum powder in the step S2 are mixed for 0.2 to 8 hours in a negative pressure device with the rotating speed of 50 to 300 r/min.
Preferably, in the step S3, a circulation mode of forward rotation for 20 min-intermittent stop for 1 min-reverse rotation for 20min is adopted for mixing, then the mixture is mixed in a ball mill with the rotating speed of 150-400 r/min for 1-24 h, no grinding medium or grinding balls are added in the mixing process, and the inert gas is one of nitrogen, helium and argon.
Preferably, when the mixture in the step S4 is sintered by using spark plasma, the spark plasma sintering conditions are as follows: sintering temperature 1000-1500 deg.c, heating rate 50-300 deg.c/min, heat maintaining time 0.5-30 min, pressure 30-70 MPa and vacuum degree 0.5-20 Pa.
Preferably, when the mixture in the step S4 is hot pressed and sintered, the hot pressed and sintered conditions are as follows: the sintering temperature is 1050-1550 ℃, the heating rate is 5-50 ℃/min, the heat preservation time is 1-5 h, the pressure is 30-150 MPa, and the vacuum degree is 10-50 Pa.
Preferably, when the mixture in the step S4 is burned in a pressureless atmosphere, the pressureless atmosphere sintering includes the following steps:
step B1: the mixture obtained in the step S3 is molded under the conditions that the pressure is 100-500 MPa and the dwell time is 0.5-10 min, so as to obtain a blank;
step B2: h, the blank obtained in the step B1 is subjected to H flow of 0.2-2L/min 2 The temperature is increased to 1150-1780 ℃ at a heating rate of 1-10 ℃/min, and the temperature is kept for 2-15 h.
Preferably, the carbide is SiC or ZrC.
Compared with the prior art, the invention has the following beneficial effects:
(1) According to the invention, the surface of the uranium dioxide microsphere is coated with the interface reaction layer metal molybdenum by low-temperature presintering, and the interface reaction layer metal molybdenum is inhibited to separate uranium dioxide from carbide, so that the effect of the carbide on the thermal conductivity of uranium dioxide is prevented from being reduced due to the fact that the uranium dioxide reacts with the carbide at a high temperature to generate other compounds. In addition, the metal molybdenum has high heat conduction, high melting point, proper neutron absorption section and other nuclear properties, and meanwhile, the metal molybdenum also has excellent high-temperature chemical compatibility with uranium dioxide and carbide, so that the effect of the uranium dioxide heat conductivity can be further improved.
(2) The composite fuel pellet containing the interface reaction inhibiting layer metallic molybdenum between uranium dioxide and carbide prepared by the method effectively solves the interface reaction problem of the uranium dioxide-carbide composite fuel pellet, improves the thermal stability and chemical stability of the uranium dioxide-carbide composite pellet serving as a heat conductivity enhanced uranium dioxide fuel, and greatly improves the safety of the uranium dioxide nuclear fuel pellet, thereby improving the safety and economical efficiency of the commercial pressurized water reactor in service, particularly the thermal stability and chemical stability under the high-temperature accident condition, and finally improving the safety margin of the reactor under the accident condition. Meanwhile, the invention can meet the requirements of industrial mass production and application, has higher application value and better application prospect, and is worthy of large-scale popularization and application.
Drawings
FIG. 1 is a schematic diagram of a process flow for preparing uranium dioxide-carbide composite fuel pellets according to the present invention.
Detailed Description
The following examples further describe the technical scheme of the present invention in a clear and complete manner using carbide as SiC, wherein the raw materials used in the examples of the present invention are all commercially available.
Example 1
The preparation method of the uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, axially pre-pressing a uranium dioxide raw material for 10min under the pressure of 250MPa, and then sequentially carrying out grinding, crushing, screening and physical micro-spheroidization to obtain uranium dioxide microspheres with the particle size of 150-400 mu m.
Step 2: and (2) loading the uranium dioxide microspheres prepared in the step (1) and the metal molybdenum powder into a negative pressure container according to the volume ratio of 90:10, rotating for 6 hours under the condition that the rotating speed is 100r/min, coating the metal molybdenum powder with the particle size of 20-800nm on the surfaces of the uranium dioxide microspheres under the physical action of negative pressure generated by the rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder to 300-1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, preserving heat for 2-24 hours, and performing low-temperature presintering to obtain the uranium dioxide microspheres coated with the interface reaction layer metal molybdenum.
Step 3: adding uranium dioxide microspheres coated with metal molybdenum for inhibiting an interface reaction layer and SiC particles with the particle size of 0.1-20 mu m prepared in the step 2 into a stainless steel ball milling tank filled with argon protection according to the volume ratio of 90:10, and mixing for 18h in a ball mill with the rotating speed of 220r/min by adopting a circulation mode of forward rotation of 20 min-intermittent 1 min-reverse rotation of 20min, wherein no grinding medium or grinding ball is added in the mixing process, so as to obtain the mixture.
Step 4: and (3) filling the mixture prepared in the step (3) into a graphite die, heating to 1500 ℃ in vacuum with the pressure of 30MPa and the vacuum degree of 20Pa at a heating rate of 300 ℃/min, and carrying out discharge plasma sintering, wherein the temperature is required to be kept for 0.5min during sintering, and cooling and demoulding after sintering to obtain the uranium dioxide-carbide composite fuel pellet.
The thermal conductivity of the uranium dioxide-carbide composite fuel pellet sample prepared in the embodiment is determined to be more than 180% of that of a standard uranium dioxide fuel pellet (600-1200 ℃).
Example 2
The preparation method of the uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, axially pre-pressing a uranium dioxide raw material for 30min under the pressure of 100MPa, and then sequentially carrying out grinding, crushing, screening and physical micro-spheroidization to obtain uranium dioxide microspheres with the particle size of 100-250 mu m.
Step 2: and (2) loading the uranium dioxide microspheres prepared in the step (1) and the metal molybdenum powder into a negative pressure container according to the volume ratio of 95:5, rotating for 8 hours under the condition of the rotating speed of 50r/min, coating the metal molybdenum powder with the particle size of 20-800nm on the surfaces of the uranium dioxide microspheres under the physical action of negative pressure generated by the rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder to 300-1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, preserving heat for 2-24 hours, and performing low-temperature presintering to obtain the uranium dioxide microspheres coated with the interface reaction layer metal molybdenum.
Step 3: adding uranium dioxide microspheres coated with metal molybdenum for inhibiting an interface reaction layer and SiC particles with the particle size of 0.1-20 mu m prepared in the step 2 into a stainless steel ball milling tank filled with argon protection according to the volume ratio of 98:2, and adopting a circulation mode of forward rotation for 20 min-intermittent 1 min-reverse rotation for 20min to mix for 24h in a ball mill with the rotating speed of 150r/min, wherein no grinding medium or grinding balls are added in the mixing process, so as to obtain the mixture.
Step 4: and (3) filling the mixture prepared in the step (3) into a graphite die, heating to 1000 ℃ in vacuum with the pressure of 70MPa and the vacuum degree of 0.5Pa at the heating rate of 50 ℃/min, and carrying out discharge plasma sintering, wherein the temperature is required to be kept for 30min during sintering, and cooling and demoulding after sintering to obtain the uranium dioxide-carbide composite fuel pellet.
The thermal conductivity of the uranium dioxide-carbide composite fuel pellet sample prepared in the embodiment is measured to be more than 140% of that of a standard uranium dioxide fuel pellet (600-1200 ℃).
Example 3
The preparation method of the uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, carrying out spark plasma sintering on a uranium dioxide raw material under the protection of argon, wherein the sintering temperature is 200 ℃ and the heat preservation time is 30min, and then sequentially carrying out grinding crushing, screening and physical microsphere treatment on the sintered uranium dioxide raw material to obtain the uranium dioxide microsphere with the particle size of 250-600 mu m.
Step 2: and (2) loading the uranium dioxide microspheres prepared in the step (1) and the metal molybdenum powder into a negative pressure container according to the volume ratio of 85:15, rotating for 4 hours under the condition that the rotating speed is 150r/min, coating the metal molybdenum powder with the particle size of 20-800nm on the surfaces of the uranium dioxide microspheres under the physical action of negative pressure generated by the rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder to 300-1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, preserving heat for 2-24 hours, and performing low-temperature presintering to obtain the uranium dioxide microspheres coated with the interface reaction layer metal molybdenum.
Step 3: adding uranium dioxide microspheres coated with metal molybdenum for inhibiting an interface reaction layer and SiC particles with the particle size of 0.1-20 mu m prepared in the step 2 into a stainless steel ball milling tank filled with argon protection according to the volume ratio of 80:20, and adopting a circulation mode of forward rotation for 20 min-intermittent 1 min-reverse rotation for 20min to mix for 12h in a ball mill with the rotating speed of 260r/min, wherein no grinding medium or grinding balls are added in the mixing process, so as to obtain the mixture.
Step 4: and (3) filling the mixture prepared in the step (3) into a graphite die, heating to 1050 ℃ in vacuum with the pressure of 150MPa and the vacuum degree of 10Pa at a heating rate of 5 ℃/min, and carrying out discharge plasma sintering, wherein the temperature is required to be kept for 0.5min during sintering, and cooling and demoulding after sintering to obtain the uranium dioxide-carbide composite fuel pellet.
The thermal conductivity of the uranium dioxide-carbide composite fuel pellet sample prepared in the embodiment is measured to be more than 220% of that of a standard uranium dioxide fuel pellet (600-1200 ℃).
Example 4
The preparation method of the uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, carrying out spark plasma sintering on a uranium dioxide raw material in vacuum, wherein the sintering temperature is 1100 ℃, the heat preservation time is 0.5min, and then sequentially carrying out grinding crushing, screening and physical microsphere treatment on the sintered uranium dioxide raw material to obtain the uranium dioxide microsphere with the particle size of 400-1000 mu m.
Step 2: and (2) loading the uranium dioxide microspheres prepared in the step (1) and the metal molybdenum powder into a negative pressure container according to the volume ratio of 80:20, rotating for 2 hours under the condition that the rotating speed is 250r/min, coating the metal molybdenum powder with the particle size of 20-800nm on the surfaces of the uranium dioxide microspheres under the physical action of negative pressure generated by the rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder to 300-1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, preserving heat for 2-24 hours, and performing low-temperature presintering to obtain the uranium dioxide microspheres coated with the interface reaction layer metal molybdenum.
Step 3: adding uranium dioxide microspheres coated with metal molybdenum for inhibiting an interface reaction layer and SiC particles with the particle size of 0.1-20 mu m prepared in the step 2 into a stainless steel ball milling tank filled with argon protection according to the volume ratio of 75:25, and adopting a circulation mode of forward rotation for 20 min-intermittent 1 min-reverse rotation for 20min to mix for 4h in a ball mill with the rotating speed of 300r/min, wherein no grinding medium or grinding ball is added in the mixing process, so as to obtain the mixture.
Step 4: carrying out compression molding on the mixture obtained in the step 3 under the conditions that the pressure is 200MPa and the pressure maintaining time is 5min, so as to obtain a blank; then placing the blank in a graphite mold at a flow rate of 0.2L/min H 2 In the protection of (2), the temperature is increased to 1780 ℃ at the heating rate of 10 ℃/min for pressureless sintering, the temperature is kept for 2 hours during pressureless sintering, and the uranium dioxide-carbide composite fuel pellets are obtained after sintering, cooling and demoulding.
The thermal conductivity of the uranium dioxide-carbide composite fuel pellet sample prepared in the embodiment is measured to be more than 250% of the thermal conductivity of a standard uranium dioxide fuel pellet (600-1200 ℃).
Example 5
The preparation method of the uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, carrying out pressureless sintering on a uranium dioxide raw material under the protection of argon, wherein the sintering temperature is 600 ℃, the heat preservation time is 12min, and then sequentially carrying out grinding crushing, screening and physical microsphere treatment on the sintered uranium dioxide raw material to obtain the uranium dioxide microsphere with the particle size of 300-800 mu m.
Step 2: and (2) loading the uranium dioxide microspheres prepared in the step (1) and the metal molybdenum powder into a negative pressure container according to the volume ratio of 92:8, rotating for 0.2h under the condition of the rotating speed of 300r/min, coating the metal molybdenum powder with the particle size of 20-800nm on the surfaces of the uranium dioxide microspheres under the physical action of negative pressure generated by the rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder to 300-1000 ℃ at the heating rate of 2-50 ℃/min under the condition of vacuum, preserving heat for 2-24h, and performing low-temperature presintering to obtain the uranium dioxide microspheres coated with the metal molybdenum with the interface reaction inhibiting layer.
Step 3: adding uranium dioxide microspheres coated with metal molybdenum for inhibiting an interface reaction layer and SiC particles with the particle size of 0.1-20 mu m prepared in the step 2 into a stainless steel ball milling tank filled with argon protection according to the volume ratio of 90:10, and adopting a circulation mode of forward rotation for 20 min-intermittent 1 min-reverse rotation for 20min to mix for 1h in a ball mill with the rotating speed of 400r/min, wherein no grinding medium or grinding ball is added in the mixing process, so as to obtain the mixture.
Step 4: and (3) filling the mixture prepared in the step (3) into a graphite die, heating to 1550 ℃ in vacuum with the pressure of 30MPa and the vacuum degree of 50Pa at the heating rate of 50 ℃/min, performing hot-pressing sintering, keeping the temperature for 1h during sintering, and cooling and demoulding after sintering to obtain the uranium dioxide-carbide composite fuel pellet.
The thermal conductivity of the uranium dioxide-carbide composite fuel pellet sample prepared in the embodiment is measured to be more than 190% of the thermal conductivity of a standard uranium dioxide fuel pellet (600-1200 ℃).
The preparation flow of the uranium dioxide-carbide composite fuel pellets in all the embodiments is shown in fig. 1, firstly, uranium dioxide raw material powder is processed into uranium dioxide microspheres, then metal molybdenum powder is coated on the surfaces of the uranium dioxide microspheres and subjected to low-temperature sintering to enable the surfaces of the uranium dioxide microspheres to be coated with interface reaction inhibiting layers of metal molybdenum, and then the uranium dioxide microspheres with the interface reaction inhibiting layers of the metal molybdenum coated on the surfaces are mixed with carbide and sintered, and the uranium dioxide-carbide composite fuel pellets are obtained after cooling.
In summary, the present invention solves the technical drawbacks of the prior art. The invention aims to solve the technical problem that the effect of carbide on enhancing the thermal conductivity of uranium dioxide is reduced because the uranium dioxide and carbide can undergo an interface reaction at high temperature. In addition, the effect of inhibiting the interface reaction layer metallic molybdenum to further improve the thermal conductivity of uranium dioxide is achieved, and the severe high-temperature service environment of the fuel pellet material under the normal working condition and the accident working condition of the reactor can be met.
The foregoing is only a partial embodiment of the present invention, and it should be noted that it will be apparent to those skilled in the art that modifications and adaptations can be made without departing from the principles of the present invention, and such modifications and adaptations are intended to be comprehended within the scope of the present invention.

Claims (9)

1. The uranium dioxide-carbide composite fuel pellet is characterized in that the uranium dioxide surface in the uranium dioxide-carbide composite fuel pellet is coated with a layer of interface reaction inhibiting layer metal molybdenum formed by low-temperature presintering metal molybdenum powder with the particle size of 20-800 nm;
the preparation method of the uranium dioxide-carbide composite fuel pellet specifically comprises the following steps:
step S1: firstly, pre-pressing or presintering a uranium dioxide raw material, and then sequentially grinding, crushing, screening and physically micro-spheroidizing to obtain uranium dioxide microspheres with the particle size of 100-1000 mu m;
step S2: mixing uranium dioxide microspheres obtained in the step S1 with metal molybdenum powder according to the volume ratio of (80-95): 20-5, coating the metal molybdenum powder on the surfaces of the uranium dioxide microspheres through physical action, and then carrying out low-temperature presintering on the uranium dioxide microspheres coated with the metal molybdenum powder to obtain uranium dioxide microspheres coated with metal molybdenum of an interface reaction inhibiting layer;
step S3: uranium dioxide microspheres coated with the interface reaction inhibiting layer metal molybdenum and obtained in the step S2 and carbide particles with the particle size of 0.1-20 mu m are mixed according to the volume ratio of (75-98): (25-2) uniformly mixing under the protection of inert gas to obtain a mixture;
step S4: and (3) sintering the mixture obtained in the step (S3) by adopting any one mode of spark plasma sintering, hot-press sintering and pressureless atmosphere sintering to obtain the uranium dioxide-carbide composite fuel pellet.
2. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein when the uranium dioxide raw material in the step S1 is pre-pressed, the pre-pressing is an axial compression molding, the pressure is 100-600 MPa, and the dwell time is 0.5-30 min.
3. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein when the uranium dioxide raw material in the step S1 is pre-sintered, the pre-sintering is non-pressure atmosphere sintering or discharge plasma sintering, wherein the non-pressure atmosphere sintering is performed at a temperature of 600-1500 ℃, a heat preservation time of 0.5-12 h, an atmosphere is argon, the discharge plasma sintering is performed at a temperature of 200-1100 ℃, a heat preservation time of 0.2-30 min, and an atmosphere is argon or vacuum.
4. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein the uranium dioxide microspheres and the metal molybdenum powder in the step S2 are mixed in a negative pressure device with a rotation speed of 50-300 r/min for 0.2-8 h.
5. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein the step S3 is performed by mixing in a circulation mode of forward rotation for 20 min-intermittent stop for 1 min-reverse rotation for 20min, and then mixing in a ball mill with a rotation speed of 150-400 r/min for 1-24 h, wherein no grinding medium or grinding balls are added during mixing, and the inert gas is one of nitrogen, helium and argon.
6. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein when the mixture in step S4 is sintered using spark plasma, the spark plasma sintering conditions are: sintering temperature 1000-1500 deg.c, heating rate 50-300 deg.c/min, heat maintaining time 0.5-30 min, pressure 30-70 MPa and vacuum degree 0.5-20 Pa.
7. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein when the mixture in step S4 is hot pressed and sintered, the hot pressed and sintered conditions are: the sintering temperature is 1050-1550 ℃, the heating rate is 5-50 ℃/min, the heat preservation time is 1-5 h, the pressure is 30-150 MPa, and the vacuum degree is 10-50 Pa.
8. The uranium dioxide-carbide composite fuel pellet of claim 1, wherein when the mixture in step S4 is burned in a pressureless atmosphere, the pressureless atmosphere sintering includes the steps of:
step B1: the mixture obtained in the step S3 is molded under the conditions that the pressure is 100-500 MPa and the dwell time is 0.5-10 min, so as to obtain a blank;
step B2: h, the blank obtained in the step B1 is subjected to H flow of 0.2-2L/min 2 The temperature is increased to 1150-1780 ℃ at a heating rate of 1-10 ℃/min, and the temperature is kept for 2-15 h.
9. A uranium dioxide-carbide composite fuel pellet according to any of claims 1 to 8, wherein said carbide is SiC or ZrC.
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