CN111326265A - Uranium dioxide-carbide composite fuel pellet and preparation method thereof - Google Patents
Uranium dioxide-carbide composite fuel pellet and preparation method thereof Download PDFInfo
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- CN111326265A CN111326265A CN202010127901.2A CN202010127901A CN111326265A CN 111326265 A CN111326265 A CN 111326265A CN 202010127901 A CN202010127901 A CN 202010127901A CN 111326265 A CN111326265 A CN 111326265A
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- 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
- G21C3/623—Oxide fuels
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C21/00—Apparatus or processes specially adapted to the manufacture of reactors or parts thereof
- G21C21/02—Manufacture of fuel elements or breeder elements contained in non-active casings
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- 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
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- 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
Abstract
The invention discloses a uranium dioxide-carbide composite fuel pellet and a preparation method thereof. According to the invention, the uranium dioxide is separated from the carbide by coating the surface of the uranium dioxide microsphere with a layer of molybdenum for inhibiting the interface reaction layer, so that the problem that the thermal conductivity of the carbide to the uranium dioxide is reduced due to the fact that other compounds are generated by the high-temperature reaction of the uranium dioxide and the carbide is avoided, and the problem of the interface reaction of the uranium dioxide-carbide composite fuel pellet is effectively solved. In addition, the metal molybdenum has nuclear properties such as high heat conductivity, high melting point, proper neutron absorption cross section and the like, and also has excellent high-temperature chemical compatibility with uranium dioxide and carbide, so that the metal molybdenum in the interface reaction layer is inhibited from further improving the thermal conductivity of the uranium dioxide.
Description
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
The sudden occurrence of a nuclear power station accident of Fudao 3 months and days in 2011 leads to the active commercial nuclear reactor fuel element UO2The safety reliability of-Zr is in serious question. Under the new situation of rapid development of nuclear energy and higher intrinsic safety requirement, UO2Zr fuel elements have not been able to meet the requirements of future nuclear power for higher intrinsic safety and multi-application stack type development. The Fukushicata nuclear power accident exposes the disadvantage of low thermal conductivity of the existing uranium dioxide fuel, namely the hidden danger of reactor melting exists because the residual heat of the reactor core can not be effectively dissipated under the accident working condition. Therefore, the most effective way to add some highly thermally conductive second phase material to the uranium dioxide matrix is currently. Among these, carbide (XC, X ═ Si, Zr) has excellent heat conductivity, 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, because the interface reaction of the uranium dioxide and the carbide can occur at high temperature to generate a U-C-X compound, the effect of enhancing the thermal conductivity of the uranium dioxide by the carbide is reduced, and the thermal stability and the chemical stability of the uranium dioxide under the high-temperature near-accident working condition 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, to improve the thermal conductivity of the uranium dioxide-carbide composite fuel pellet and to be suitable for the more severe high-temperature accident working condition, the development of a preparation method of the thermal conductivity enhanced composite fuel pellet for inhibiting the interface reaction between uranium dioxide and carbide is urgently needed, so as to solve the problem.
Disclosure of Invention
Based on the above, the invention aims to solve the problem that the effect of enhancing the thermal conductivity of uranium dioxide by carbide is reduced due to the interface reaction between uranium dioxide and carbide at high temperature, and provides a uranium dioxide-carbide composite fuel pellet, wherein the surface of uranium dioxide in the uranium dioxide-carbide composite fuel pellet is coated with a layer of interface reaction inhibiting layer metal molybdenum formed by low-temperature pre-sintering 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 comprises the following steps:
step S1: firstly, pre-pressing or pre-sintering a uranium dioxide raw material, and then sequentially grinding, crushing, screening and physically micro-balling to prepare uranium dioxide microspheres with the particle size of 100-1000 microns;
step S2: mixing the uranium dioxide microspheres obtained in the step S1 with metal molybdenum powder according to a 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 pre-sintering the uranium dioxide microspheres coated with the metal molybdenum powder at a low temperature to obtain the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer;
step S3: and (5) mixing the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer on the surface and obtained in the step (S2) with carbide particles with the particle size of 0.1-20 mu m 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 sintering the mixture obtained in the step S3 by adopting any one of discharge plasma sintering, hot-pressing sintering and pressureless 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 mold pressing, the pressure is 100 to 600MPa, and the pressure maintaining time is 0.5 to 30 min.
Preferably, when the uranium dioxide raw material in 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 to 1500 ℃, the heat preservation time is 0.5 to 12 hours, the atmosphere is argon, the temperature of the discharge plasma sintering is 200 to 1100 ℃, the heat preservation time is 0.2 to 30 minutes, and the atmosphere is argon or vacuum.
Preferably, the uranium dioxide microspheres and the metal molybdenum powder in the step S2 are mixed for 0.2-8 hours in negative pressure equipment with the rotating speed of 50-300 r/min.
Preferably, in the step S3, a circulation mode of forward rotation for 20min, intermittent stop for 1min, and reverse rotation for 20min is adopted for mixing, and then the mixture is mixed in a ball mill with a rotation speed of 150 to 400r/min for 1 to 24 hours, wherein a grinding medium and grinding balls are not added in the mixing process, and the inert gas is one of nitrogen, helium and argon.
Preferably, when the mixture in step S4 is sintered by using discharge plasma, the discharge plasma sintering conditions are as follows: the sintering temperature is 1000-1500 ℃, the heating rate is 50-300 ℃/min, the heat preservation time is 0.5-30 min, the pressure is 30-70 MPa, and the vacuum degree is 0.5-20 Pa.
Preferably, when the mixture in 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 fired in a pressureless atmosphere, the pressureless sintering includes the following steps:
step B1: performing compression molding on the mixture obtained in the step S3 under the conditions that the pressure is 100-500 MPa and the pressure maintaining time is 0.5-10 min to obtain a blank body;
step B2: b, subjecting the blank obtained in the step B1 to H at the flow rate of 0.2-2L/min2Heating to 1150-17 deg.C at a heating rate of 1-10 deg.C/minAnd keeping the temperature at 80 ℃ 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 a layer of molybdenum metal for inhibiting an interface reaction layer through low-temperature pre-sintering, and the uranium dioxide and the carbide are separated by the molybdenum metal for inhibiting the interface reaction layer, so that the reduction of the effect of the carbide on the thermal conductivity of the uranium dioxide caused by the generation of other compounds through the high-temperature reaction of the uranium dioxide and the carbide is avoided. In addition, as the metal molybdenum has nuclear properties of high heat conduction, high melting point, proper neutron absorption cross section and the like, and also has excellent high-temperature chemical compatibility with uranium dioxide and carbide, the uranium dioxide heat conductivity effect can be further improved, and the uranium dioxide-carbide composite fuel pellet prepared by the invention can meet the more harsh high-temperature service environment of the fuel pellet material under the normal working condition and the accident working condition of a reactor.
(2) The composite fuel pellet containing the molybdenum metal for inhibiting the interface reaction layer between the uranium dioxide and the carbide, which is prepared by the invention, effectively solves the problem of the interface reaction of the uranium dioxide-carbide composite fuel pellet, improves the thermal stability and the chemical stability of the uranium dioxide-carbide composite pellet as the thermal conductivity enhanced uranium dioxide fuel, and greatly improves the safety of the uranium dioxide nuclear fuel pellet, thereby improving the safety and the economical efficiency of an active commercial pressurized water reactor, particularly the thermal stability and the chemical stability under the working condition of high-temperature accidents, and finally improving the safety margin of the reactor under the working condition of accidents. Meanwhile, the invention can meet the requirements of industrial large-scale 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 the preparation process of the uranium dioxide-carbide composite fuel pellet.
Detailed Description
The technical solution of the present invention is further clearly and completely described in the following examples using SiC as carbide, wherein the raw materials used in the examples of the present invention are all commercially available.
Example 1
A preparation method of a uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, pre-pressing a uranium dioxide raw material axially for 10min under the condition of 250MPa of pressure, and then sequentially carrying out grinding, crushing, screening and physical micro-spheroidizing treatment to obtain the uranium dioxide microspheres with the particle size of 150-400 mu m.
Step 2: and (2) putting the uranium dioxide microspheres prepared in the step (1) and 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 rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder on the surfaces to 300-phase-change 1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, and preserving the temperature for 2-24 hours for low-temperature pre-sintering to finally obtain the uranium dioxide microspheres coated with the metal molybdenum on the surfaces of the inhibition interface reaction layers.
And step 3: and (3) adding the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer and prepared in the step (2) and SiC particles with the particle size of 0.1-20 microns into a stainless steel ball milling tank filled with argon gas according to the volume ratio of 90:10, mixing for 18 hours in a ball mill with the rotating speed of 220r/min by adopting a circulation mode of forward rotation for 20min, stopping for 1min and reversely rotating for 20min, and not adding any grinding medium and grinding balls in the mixing process to obtain a mixture.
And 4, step 4: and (3) loading the mixture prepared in the step (3) into a graphite mold, heating to 1500 ℃ at a heating rate of 300 ℃/min in vacuum with the pressure of 30MPa and the vacuum degree of 20Pa for discharge plasma sintering, keeping the temperature for 0.5min during sintering, and cooling and demolding 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 more than 180% of that of the standard uranium dioxide fuel pellet (600-1200 ℃).
Example 2
A preparation method of a uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, pre-pressing a uranium dioxide raw material axially for 30min under the condition of 100MPa of pressure, and then sequentially carrying out grinding, crushing, screening and physical micro-spheroidizing treatment to obtain the uranium dioxide microspheres with the particle size of 100-250 mu m.
Step 2: and (2) putting the uranium dioxide microspheres prepared in the step (1) and metal molybdenum powder into a negative pressure container according to the volume ratio of 95:5, rotating for 8 hours under the condition that the rotating speed is 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 rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder on the surfaces to 300-phase addition of 1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, and preserving the temperature for 2-24 hours for low-temperature pre-sintering to finally obtain the uranium dioxide microspheres coated with the metal molybdenum on the surfaces of the inhibition interface reaction layers.
And step 3: and (3) adding the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer and prepared in the step (2) and SiC particles with the particle size of 0.1-20 microns into a stainless steel ball milling tank filled with argon gas according to the volume ratio of 98:2, mixing for 24 hours in a ball mill with the rotating speed of 150r/min by adopting a circulation mode of forward rotation for 20 min-intermittent stop for 1 min-reverse rotation for 20min, and not adding any grinding medium and grinding balls in the mixing process to obtain a mixture.
And 4, step 4: and (3) loading the mixture prepared in the step (3) into a graphite mold, heating to 1000 ℃ at a heating rate of 50 ℃/min in vacuum with the pressure of 70MPa and the vacuum degree of 0.5Pa to perform discharge plasma sintering, preserving heat for 30min at the temperature during sintering, and cooling and demolding 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 more than 140% (600-1200 ℃) of that of the standard uranium dioxide fuel pellet.
Example 3
A preparation method of a uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, performing discharge 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 performing grinding, crushing, screening and physical micro-spheroidizing on the sintered uranium dioxide raw material to obtain uranium dioxide microspheres with the particle size of 250-600 mu m.
Step 2: and (2) putting the uranium dioxide microspheres prepared in the step (1) and 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 rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder on the surfaces to 300-phase-change 1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, and preserving the temperature for 2-24 hours for low-temperature pre-sintering to finally obtain the uranium dioxide microspheres coated with the metal molybdenum on the surfaces of the inhibition interface reaction layers.
And step 3: and (3) adding the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer and prepared in the step (2) and SiC particles with the particle size of 0.1-20 microns into a stainless steel ball milling tank filled with argon gas according to the volume ratio of 80:20, mixing for 12 hours in a ball mill with the rotating speed of 260r/min by adopting a circulation mode of forward rotation for 20 min-intermittent stop for 1 min-reverse rotation for 20min, and not adding any grinding medium and grinding balls in the mixing process to obtain a mixture.
And 4, step 4: and (3) loading the mixture prepared in the step (3) into a graphite mold, heating to 1050 ℃ at a heating rate of 5 ℃/min in vacuum with the pressure of 150MPa and the vacuum degree of 10Pa for spark plasma sintering, preserving heat for 0.5min at the temperature during sintering, and cooling and demolding 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 more than 220% of that of the standard uranium dioxide fuel pellet (600-1200 ℃).
Example 4
A preparation method of a uranium dioxide-carbide composite fuel pellet comprises the following steps:
step 1: firstly, performing discharge plasma sintering on a uranium dioxide raw material in vacuum, wherein the sintering temperature is 1100 ℃, and the heat preservation time is 0.5min, and then sequentially performing grinding, crushing, screening and physical micro-spheroidizing on the sintered uranium dioxide raw material to obtain the uranium dioxide microspheres with the particle size of 400-plus-one 1000 mu m.
Step 2: and (2) putting the uranium dioxide microspheres prepared in the step (1) and metal molybdenum powder into a negative pressure container according to the volume ratio of 80:20, rotating for 2h 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 rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder on the surfaces to 300-phase-change 1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, and preserving the temperature for 2-24h for low-temperature pre-sintering to finally obtain the uranium dioxide microspheres coated with the metal molybdenum on the surfaces of the inhibition interface reaction layers.
And step 3: and (3) adding the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer and prepared in the step (2) and SiC particles with the particle size of 0.1-20 microns into a stainless steel ball milling tank filled with argon protection according to the volume ratio of 75:25, mixing for 4 hours in a ball mill with the rotating speed of 300r/min by adopting a circulation mode of forward rotation for 20min, stopping for 1min and reversely rotating for 20min, and not adding any grinding medium and grinding balls in the mixing process to obtain a mixture.
And 4, step 4: performing 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 to obtain a blank body; then the blank is placed in a graphite die at the flow rate of 0.2L/min H2In the protection, the temperature is increased to 1780 ℃ at the heating rate of 10 ℃/min for pressureless sintering, the temperature is kept for 2h at the temperature during pressureless sintering, and the uranium dioxide-carbide composite fuel pellet is obtained after cooling and demoulding after sintering.
The thermal conductivity of the uranium dioxide-carbide composite fuel pellet sample prepared in the embodiment is more than 250% (600-1200 ℃) of that of the standard uranium dioxide fuel pellet.
Example 5
A preparation method of a 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 ℃, and the heat preservation time is 12min, and then sequentially carrying out grinding, crushing, screening and physical micro-spheroidizing on the sintered uranium dioxide raw material to obtain uranium dioxide microspheres with the particle size of 300-800 microns.
Step 2: and (2) putting the uranium dioxide microspheres prepared in the step (1) and metal molybdenum powder into a negative pressure container according to the volume ratio of 92:8, rotating for 0.2h under the condition that the rotating speed is 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 rotation of negative pressure equipment, heating the uranium dioxide microspheres coated with the metal molybdenum powder on the surfaces to 300-1000 ℃ at the heating rate of 2-50 ℃/min under the vacuum condition, and preserving heat for 2-24h for low-temperature pre-sintering to finally obtain the uranium dioxide microspheres coated with the metal molybdenum with the surface inhibiting interface reaction layer.
And step 3: and (3) adding the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer and prepared in the step (2) and SiC particles with the particle size of 0.1-20 microns into a stainless steel ball milling tank filled with argon gas according to the volume ratio of 90:10, mixing for 1h in a ball mill with the rotating speed of 400r/min by adopting a circulation mode of forward rotation for 20min, stopping for 1min and reverse rotation for 20min, and not adding any grinding medium and grinding balls in the mixing process to obtain a mixture.
And 4, step 4: and (3) putting the mixture prepared in the step (3) into a graphite die, heating to 1550 ℃ at a heating rate of 50 ℃/min in vacuum with the pressure of 30MPa and the vacuum degree of 50Pa for hot-pressing sintering, preserving heat for 1h at the temperature during sintering, cooling after sintering, and demolding 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 more than 190% (600-1200 ℃) of that of the standard uranium dioxide fuel pellet.
The preparation process of the uranium dioxide-carbide composite fuel pellet in all the embodiments is shown in fig. 1, and is characterized in that 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, low-temperature sintering is carried out, so that the surfaces of the uranium dioxide microspheres are coated with the interface reaction inhibiting layer of metal molybdenum, then the uranium dioxide microspheres coated with the interface reaction inhibiting layer of metal molybdenum on the surfaces are mixed with carbide and sintered, and the uranium dioxide-carbide composite fuel pellet is obtained after cooling.
In summary, the present invention solves the technical deficiencies of the prior art. The invention aims to solve the technical problem that the effect of enhancing the thermal conductivity of uranium dioxide by carbide is reduced due to the fact that interface reaction can occur between uranium dioxide and carbide at high temperature. In addition, the effect of further improving the thermal conductivity of the uranium dioxide by adding the metal molybdenum for inhibiting the interface reaction layer can meet the more severe high-temperature service environment of the fuel pellet material under the normal working condition and the accident working condition of the reactor.
The foregoing is only a partial embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (10)
1. The uranium dioxide-carbide composite fuel pellet is characterized in that the surface of uranium dioxide in the uranium dioxide-carbide composite fuel pellet is coated with a layer of interface reaction inhibiting layer metal molybdenum formed by low-temperature pre-sintering metal molybdenum powder with the particle size of 20-800 nm.
2. The method for preparing a uranium dioxide-carbide composite fuel pellet according to claim 1, comprising the following steps:
step S1: firstly, pre-pressing or pre-sintering a uranium dioxide raw material, and then sequentially grinding, crushing, screening and physically micro-balling to prepare uranium dioxide microspheres with the particle size of 100-1000 microns;
step S2: mixing the uranium dioxide microspheres obtained in the step S1 with metal molybdenum powder according to a 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 pre-sintering the uranium dioxide microspheres coated with the metal molybdenum powder at a low temperature to obtain the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer;
step S3: and (5) mixing the uranium dioxide microspheres coated with the metal molybdenum for inhibiting the interface reaction layer on the surface and obtained in the step (S2) with carbide particles with the particle size of 0.1-20 mu m 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 sintering the mixture obtained in the step S3 by adopting any one of discharge plasma sintering, hot-pressing sintering and pressureless sintering to obtain the uranium dioxide-carbide composite fuel pellet.
3. The method for preparing a uranium dioxide-carbide composite fuel pellet according to claim 2, wherein when the uranium dioxide raw material is pre-pressed in the step S1, the pre-pressing is axial molding, the pressure is 100 to 600MPa, and the pressure holding time is 0.5 to 30 min.
4. The method for preparing a uranium dioxide-carbide composite fuel pellet according to claim 2, wherein when the uranium dioxide raw material is pre-sintered in step S1, the pre-sintering is pressureless sintering or spark plasma sintering, wherein the pressureless sintering is performed at a temperature of 600 to 1500 ℃, a holding time of 0.5 to 12 hours, an atmosphere of argon, the spark plasma sintering is performed at a temperature of 200 to 1100 ℃, a holding time of 0.2 to 30 minutes, and an atmosphere of argon or vacuum.
5. The method for preparing the uranium dioxide-carbide composite fuel pellet as claimed in claim 2, wherein the uranium dioxide microspheres and the metal molybdenum powder in the step S2 are mixed for 0.2-8 hours in a negative pressure device with a rotation speed of 50-300 r/min.
6. The method for preparing the uranium dioxide-carbide composite fuel pellet as claimed in claim 2, wherein the step S3 is performed by mixing in a circulation mode of forward rotation for 20min, intermittent rotation for 1min and 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 a grinding medium and a grinding ball are not added during mixing, and the inert gas is one of nitrogen, helium and argon.
7. The method for preparing uranium dioxide-carbide composite fuel pellets according to claim 2, wherein when the mixture in the step S4 is sintered by spark plasma, the spark plasma sintering conditions are as follows: the sintering temperature is 1000-1500 ℃, the heating rate is 50-300 ℃/min, the heat preservation time is 0.5-30 min, the pressure is 30-70 MPa, and the vacuum degree is 0.5-20 Pa.
8. The method for preparing uranium dioxide-carbide composite fuel pellets according to claim 2, wherein 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.
9. A method for the preparation of uranium dioxide-carbide composite fuel pellets according to claim 2, wherein, when the mixture in step S4 is fired in a pressureless atmosphere, the pressureless sintering comprises the following steps:
step B1: performing compression molding on the mixture obtained in the step S3 under the conditions that the pressure is 100-500 MPa and the pressure maintaining time is 0.5-10 min to obtain a blank body;
step B2: b, subjecting the blank obtained in the step B1 to H at the flow rate of 0.2-2L/min2The temperature is increased to 1150-1780 ℃ at a rate of 1-10 ℃/min in the atmosphere, and the temperature is kept for 2-15 h.
10. A method of producing a uranium dioxide-carbide composite fuel pellet according to any one of claims 2 to 9, wherein the carbide is SiC or ZrC.
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