CN115740463A - Method for producing fuel pellets - Google Patents
Method for producing fuel pellets Download PDFInfo
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- CN115740463A CN115740463A CN202211383644.4A CN202211383644A CN115740463A CN 115740463 A CN115740463 A CN 115740463A CN 202211383644 A CN202211383644 A CN 202211383644A CN 115740463 A CN115740463 A CN 115740463A
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- 239000000446 fuel Substances 0.000 title claims abstract description 91
- 239000008188 pellet Substances 0.000 title claims abstract description 78
- 238000004519 manufacturing process Methods 0.000 title claims description 8
- 239000000843 powder Substances 0.000 claims abstract description 191
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 72
- 238000000498 ball milling Methods 0.000 claims abstract description 66
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 53
- 229910052770 Uranium Inorganic materials 0.000 claims abstract description 52
- 239000011812 mixed powder Substances 0.000 claims abstract description 50
- 238000005245 sintering Methods 0.000 claims abstract description 37
- 238000002156 mixing Methods 0.000 claims abstract description 20
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims abstract description 20
- 238000007731 hot pressing Methods 0.000 claims abstract description 15
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 14
- XOOUIPVCVHRTMJ-UHFFFAOYSA-L zinc stearate Chemical compound [Zn+2].CCCCCCCCCCCCCCCCCC([O-])=O.CCCCCCCCCCCCCCCCCC([O-])=O XOOUIPVCVHRTMJ-UHFFFAOYSA-L 0.000 claims abstract description 14
- 239000001257 hydrogen Substances 0.000 claims abstract description 13
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 9
- 238000000034 method Methods 0.000 claims description 44
- 239000002245 particle Substances 0.000 claims description 23
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 22
- 150000002431 hydrogen Chemical class 0.000 claims description 5
- 238000002360 preparation method Methods 0.000 abstract description 7
- 229910003468 tantalcarbide Inorganic materials 0.000 description 41
- 239000012535 impurity Substances 0.000 description 15
- 229910052760 oxygen Inorganic materials 0.000 description 10
- 230000008569 process Effects 0.000 description 10
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 8
- 239000001301 oxygen Substances 0.000 description 8
- 229910052751 metal Inorganic materials 0.000 description 6
- 239000002184 metal Substances 0.000 description 6
- 238000004321 preservation Methods 0.000 description 6
- 230000006872 improvement Effects 0.000 description 5
- 230000009286 beneficial effect Effects 0.000 description 4
- 239000002994 raw material Substances 0.000 description 4
- 239000007789 gas Substances 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- CSJDCSCTVDEHRN-UHFFFAOYSA-N methane;molecular oxygen Chemical compound C.O=O CSJDCSCTVDEHRN-UHFFFAOYSA-N 0.000 description 3
- 238000003825 pressing Methods 0.000 description 3
- 239000007791 liquid phase Substances 0.000 description 2
- UNASZPQZIFZUSI-UHFFFAOYSA-N methylidyneniobium Chemical compound [Nb]#C UNASZPQZIFZUSI-UHFFFAOYSA-N 0.000 description 2
- NFFIWVVINABMKP-UHFFFAOYSA-N methylidynetantalum Chemical compound [Ta]#C NFFIWVVINABMKP-UHFFFAOYSA-N 0.000 description 2
- 239000002105 nanoparticle Substances 0.000 description 2
- 239000010955 niobium Substances 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 230000009257 reactivity Effects 0.000 description 2
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 238000009770 conventional sintering Methods 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005262 decarbonization Methods 0.000 description 1
- QRKOGTOMYRGNOR-UHFFFAOYSA-N methane;uranium Chemical compound C.[U] QRKOGTOMYRGNOR-UHFFFAOYSA-N 0.000 description 1
- 238000009740 moulding (composite fabrication) Methods 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 239000003758 nuclear fuel Substances 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
The application provides a preparation method of a fuel pellet, which comprises the following steps: mixing nanoscale TaC powder, nanoscale NbC powder, nanoscale UC powder, zinc stearate and uranium powder, and then performing ball milling treatment to obtain UC-NbC-TaC-U mixed powder; carrying out hot-pressing sintering treatment on the UC-NbC-TaC-U mixed powder to obtain an initial fuel pellet; reacting the initial fuel pellets at a first temperature for a first time period with flowing hydrogen to remove free carbon to obtain (U, nb, ta) C quaternary fuel pellets, wherein the first temperature is greater than 1200 ℃.
Description
Technical Field
The application relates to the technical field of nuclear fuel, in particular to a preparation method of a fuel pellet.
Background
The quaternary (U, nb, ta) C fuel as a special carbide fuel has the advantages of high specific impulse, high thrust and the like, and can supply energy to a high-power nuclear propulsion reactor for deep space exploration and cargo transportation.
In the related art, a method for preparing a quaternary (U, nb, ta) C fuel includes: mixing UO 2 Powder, nb 2 O 5 Powder, ta 2 O 5 Mixing with C powderThe quaternary (U, nb, ta) C fuel pellet is prepared by ball milling, pressing and sintering the quaternary (U, nb, ta) C raw material powder.
However, the quaternary (U, nb, ta) C fuel pellets prepared by the preparation method in the related art have problems of high content of free carbon and oxygen impurities and low pellet density.
Disclosure of Invention
In view of the above, in order to reduce the content of free carbon and oxygen impurities in the quaternary (U, nb, ta) C fuel pellet and increase the density of the fuel pellet, the present application proposes a method for preparing the fuel pellet, so as to at least partially solve the above existing technical problems.
In order to solve the above technical problems, the present application proposes a method for preparing a fuel pellet, comprising:
mixing nanoscale TaC powder, nanoscale NbC powder, nanoscale UC powder, zinc stearate and uranium powder, and then performing ball milling treatment to obtain UC-NbC-TaC-U mixed powder;
carrying out hot-pressing sintering treatment on the UC-NbC-TaC-U mixed powder to obtain an initial fuel pellet;
reacting the initial fuel pellets for a first length of time at a first temperature with flowing hydrogen to remove free carbon to obtain (U, nb, ta) C quaternary fuel pellets, wherein the first temperature is greater than 1200 ℃.
According to the embodiment of the application, the mass ratio of the nanoscale TaC powder to the nanoscale NbC powder to the nanoscale UC powder is 1 (3-5) to (6-4); the adding amount of the zinc stearate is 0.3 to 0.5 percent of the total mass of the nano TaC powder, the nano NbC powder and the nano UC powder; the adding amount of the uranium powder is 1-3% of the total mass of the nano TaC powder, the nano NbC powder and the nano UC powder.
According to the embodiment of the application, the particle size of the nano UC powder is in the range of 500-900 nm; the particle size range of the nano NbC powder is 700-900 nm; the particle size range of the nano-scale TaC powder is 800-900 nm.
According to an embodiment of the present application, a method for preparing a nanoscale UC powder includes:
will U 3 O 8 Mixing the powder and carbon powder and then carrying out ball milling treatment to obtain U 3 O 8 And carbon, wherein U 3 O 8 The particle size range of the mixed powder of the carbon and the carbon is 500-900 nm;
to U 3 O 8 And sintering the mixed powder of the carbon and the mixed powder to obtain the nanoscale UC powder.
According to an embodiment of the present application, U 3 O 8 The molar ratio of the powder to the carbon powder is 1 (7-9).
According to an embodiment of the application, U 3 O 8 Mixing the powder and carbon powder and then carrying out ball milling treatment to obtain U 3 O 8 And carbon, the mixed powder comprising: will U 3 O 8 Mixing the powder and carbon powder, and ball-milling for 1-3 h by adopting an ethanol wet method under the condition that the ball-milling rotating speed is 300-500 rpm to obtain U 3 O 8 And mixed powder of carbon.
According to the embodiment of the application, for U 3 O 8 And sintering the mixed powder of the carbon to obtain the nanoscale UC powder, wherein the nanoscale UC powder comprises the following components: to U 3 O 8 Reacting the mixed powder with carbon for 2-4 h at 1500-1700 ℃ to obtain the nanoscale UC powder.
According to an embodiment of the present application, a method of preparing nanoscale NbC powder comprises: nbC powder with the granularity of 10-20 mu m is subjected to ball milling treatment to obtain nanoscale NbC powder.
According to an embodiment of the present application, a method of preparing a nanoscale TaC powder comprises: and carrying out ball milling treatment on the TaC powder with the granularity of 20-40 mu m to obtain the nano-scale TaC powder.
According to the embodiment of the application, after mixing the nanoscale TaC powder, the nanoscale NbC powder, the nanoscale UC powder, zinc stearate and uranium powder, performing ball milling treatment to obtain UC-NbC-TaC-U mixed powder, wherein the conditions of the ball milling treatment comprise: an ethanol wet method is adopted, the ball milling rotating speed is 400-600 rpm, and the ball milling time is 6-10 h.
According to the embodiment of the application, in the step of carrying out hot-pressing sintering treatment on the UC-NbC-TaC-U mixed powder to obtain the initial fuel pellet, the conditions of the hot-pressing sintering treatment comprise that: the pressure is 60-100 MPa, the temperature is 1550-1755 ℃, and the heat preservation time is 1-3 h.
According to an embodiment of the application, reacting the initial fuel pellets at a first temperature for a first time period with flowing hydrogen to remove free carbon to obtain (U, nb, ta) C quaternary fuel pellets comprises: under the vacuum degree of (1-3) × 10 - 3 Pa, and introducing flowing hydrogen, and reacting the initial fuel pellet for 1-3 h at a first temperature of 1600-1755 ℃ to remove free carbon, thereby obtaining the (U, nb, ta) C quaternary fuel pellet.
According to the embodiment of the application, the UC-NbC-TaC-U mixed powder is prepared by mixing nanoscale TaC powder, nbC powder, UC powder, zinc stearate and uranium powder, then the mixed powder is subjected to hot-pressing sintering to obtain an initial fuel pellet, and then the initial fuel pellet is subjected to decarbonization treatment to obtain a quaternary (U, nb, ta) C pellet. The process can solve the problem that C and O impurities cannot be reduced by carbothermal reaction, so that the content of free C and O impurities in the quaternary (U, nb, ta) C fuel pellet can be reduced, and the density of the fuel pellet is improved.
According to the embodiment of the application, metal uranium powder is adopted as a sintering aid, and two beneficial effects can be generated on pellet sintering: firstly, the metal uranium powder can be melted into a liquid phase at the temperature of more than 1200 ℃, the formed liquid phase sintering can promote the improvement of pellet density, and meanwhile, the metal uranium can also improve the heat conductivity of the fuel, so that the improvement of the fuel thermophysical property is positively influenced; and secondly, the metal uranium can also increase the density of (U, nb, ta) C fuel uranium, increase the fuel consumption depth of the fuel and play a double beneficial effect.
Drawings
FIG. 1 is a flow chart of the present application for the preparation of fuel pellets.
Detailed Description
In order to make the objects, technical solutions and advantages of the present application more apparent, the technical solutions of the present application will be described clearly and completely in conjunction with the embodiments of the present application. It should be apparent that the described embodiment is one embodiment of the present application, and not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the described embodiments of the application without any inventive step, are within the scope of protection of the application.
It is to be noted that, unless otherwise defined, technical or scientific terms used herein shall have the ordinary meaning as understood by those of ordinary skill in the art to which this application belongs. If the description "first", "second", etc. is referred to throughout, the description of "first", "second", etc. is used only for distinguishing similar objects, and is not to be construed as indicating or implying a relative importance, order or number of technical features indicated, it being understood that the data described in "first", "second", etc. may be interchanged where appropriate. If "and/or" is presented throughout, it is meant to include three juxtapositions, exemplified by "A and/or B" and including either scheme A, or scheme B, or schemes in which both A and B are satisfied.
The maximum service temperature of the fuel of the nuclear propulsion reactor is approximately 3500K, the melting point of Uranium Carbide (UC) fuel is 2803K, the pure UC fuel cannot meet the ultra-high temperature requirement of the nuclear propulsion reactor, and meanwhile, the UC fuel also faces the problem of thermochemical corrosion in a hot hydrogen environment. Therefore, there is a need for optimized improvements in fuel performance by the addition of other elements (such as niobium Nb and tantalum Ta, etc.).
In the aspect of hot material performance, a second phase with high melting point and high heat conductivity, such as niobium carbide NbC and tantalum carbide TaC, is added to form a net bridging structure, so that the melting point and the heat conductivity of the carbide fuel are improved; in terms of mechanical properties, second phases such as niobium carbide NbC, tantalum carbide TaC and the like are dispersed and precipitated in a fuel grain boundary, and the mechanical properties of the fuel are enhanced in terms of hardness and bending strength.
By doping and modifying the carbide (UC) fuel, the formed multi-element carbide fuel is greatly improved in the aspects of thermal property and mechanical property. The quaternary (U, nb, ta) C fuel as a special carbide fuel has the advantages of high specific impulse, high thrust and the like, and can supply energy to a high-power nuclear propulsion reactor for deep space exploration and cargo transportation.
In the related art, the preparation method of the quaternary (U, nb, ta) C fuel pellet is to use UO 2 Powder, nb 2 O 5 Powder, ta 2 O 5 And mixing the powder with the C powder, performing high-temperature reaction treatment to obtain quaternary (U, nb, ta) C raw material powder, and performing ball milling, pressing and sintering on the quaternary (U, nb, ta) C raw material powder to obtain the quaternary (U, nb, ta) C fuel pellet. However, due to UO 2 Powder, nb 2 O 5 Powder, ta 2 O 5 The reaction temperature and reaction time are different from those of C powder, so that the content of free carbon and oxygen impurities in the finally prepared (U, nb, ta) C quaternary fuel pellet is high (generally higher than 500 ppm), and the impurities can reduce the hot material performance of the fuel; meanwhile, the conventional sintering process has the problem of low density of the core block.
Fig. 1 schematically shows a flow chart of the present application for the preparation of fuel pellets.
As shown in fig. 1, the present application proposes a method for preparing fuel pellets, which includes operations S101 to S103.
In operation S101, mixing the nanoscale TaC powder, the nanoscale NbC powder, the nanoscale UC powder, zinc stearate, and uranium powder, and then performing ball milling to obtain UC-NbC-TaC-U mixed powder;
in operation S102, performing hot-pressing sintering on the UC-NbC-TaC-U mixed powder to obtain an initial fuel pellet;
in operation S103, the initial fuel pellets are reacted at a first temperature for a first time period with flowing hydrogen gas to remove free carbon, resulting in (U, nb, ta) C quaternary fuel pellets, wherein the first temperature is greater than 1200 ℃.
According to the embodiment of the application, the TaC powder, the NbC powder and the UC powder which are in the nanometer level are respectively prepared and then mixed, so that oxygen impurities are effectively reduced, free carbon is removed by utilizing flowing hydrogen, carbon impurities are reduced, and the purity of the fuel pellet is improved.
According to the embodiment of the application, the metal uranium powder is used as the sintering aid, so that the density of the pellets can be improved, the thermal conductivity of the fuel can be improved, and the improvement on the thermal physical property of the fuel is positively influenced.
According to the embodiment of the application, the mass ratio of the nanoscale TaC powder to the nanoscale NbC powder to the nanoscale UC powder is 1 (3-5) to (4-6); the adding amount of the zinc stearate is 0.3 to 0.5 percent of the total mass of the nano TaC powder, the nano NbC powder and the nano UC powder; the adding amount of the uranium powder is 1-3% of the total mass of the nano TaC powder, the nano NbC powder and the nano UC powder.
According to the examples of the present application, the nanoscale UC powder has a particle size in the range of 500 to 900nm.
According to the embodiments of the present application, the particle size of the nano-sized UC powder may be selected to be 500nm, 700nm, 900nm, etc.
According to embodiments of the present application, the nanoscale NbC powder has a particle size in the range of 700 to 900nm.
According to embodiments of the present application, the nanoscale NbC powder may be selected to have a particle size of 700nm, 800nm, 900nm, and the like.
According to the examples of the present application, the nanoscale TaC powder has a particle size in the range of 800 to 900nm.
According to the embodiments of the present application, the particle size of the nano-sized TaC powder may be selected to be 800nm, 850nm, 900nm, etc.
According to the examples of the present application, the mass ratio of the nanoscale TaC powder, nanoscale NbC powder and nanoscale UC powder can be selected from 1.
According to the embodiment of the present application, the added amount of zinc stearate may be selected to be 0.3%, 0.4%, 0.5%, etc. of the total mass of the nanoscale TaC powder, nanoscale NbC powder, and nanoscale UC powder.
According to the embodiment of the application, the adding amount of the uranium powder can be selected to be 1%, 2%, 3% and the like of the total mass of the nanoscale TaC powder, the nanoscale NbC powder and the nanoscale UC powder.
According to the embodiment of the application, the oxygen impurity content in the raw material can be effectively reduced by adding the nanoscale TaC powder, the nanoscale NbC powder and the nanoscale UC powder.
According to the embodiment of the application, the zinc stearate can increase the cohesiveness among different powders, and is beneficial to the agglomeration, pressing and forming treatment among the powders.
According to the embodiment of the application, the metal uranium powder is used as a sintering aid, so that the density and the heat conductivity of the pellets can be improved, and the positive influence on the improvement of the fuel thermophysical performance is realized.
According to an embodiment of the present application, a method for preparing a nanoscale UC powder includes: will U 3 O 8 Mixing the powder and carbon powder and then carrying out ball milling treatment to obtain U 3 O 8 Mixed powder with carbon, for U 3 O 8 And sintering the mixed powder of the carbon and the mixed powder to obtain the nanoscale UC powder.
According to an embodiment of the present application, U 3 O 8 The particle size range of the mixed powder with carbon is 500-900 nm.
According to an embodiment of the present application, U 3 O 8 The particle size of the mixed powder with carbon may be selected from 500nm, 700nm, 900nm, etc.
According to an embodiment of the present application, U 3 O 8 The molar ratio of the powder to the carbon powder is 1 (7-9).
According to an embodiment of the present application, U 3 O 8 The molar ratio of powder to carbon powder can be selected from 1:7, 1:8, 1:9, etc.
According to the embodiment of the application, the U can be enabled by adding excessive carbon powder 3 O 8 The complete reactive removal of the O in the powder helps to reduce the O impurities of the fuel pellets.
According to the embodiment of the application, U 3 O 8 Mixing the powder and carbon powder and then carrying out ball milling treatment to obtain U 3 O 8 And carbon, the mixed powder comprising: will U 3 O 8 Mixing the powder and carbon powder, and ball-milling for 1-3 h by adopting an ethanol wet method under the condition that the ball-milling rotating speed is 300-500 rpm to obtain U 3 O 8 And mixed powder of carbon.
According to an embodiment of the present application, U 3 O 8 When the powder and the carbon powder are mixed for ball milling treatment, the ball milling rotation speed can be 300nm, 400nm, 500nm and the like.
According to an embodiment of the present application, U 3 O 8 Mixing the powder and carbon powder and ball-millingDuring treatment, the ball milling treatment time can be selected from 1h, 2h, 3h and the like.
According to an embodiment of the application, to U 3 O 8 And sintering the mixed powder of the carbon to obtain the nanoscale UC powder, wherein the nanoscale UC powder comprises the following components: to U 3 O 8 Reacting the mixed powder with carbon for 2-4 h at 1500-1700 ℃ to obtain the nanoscale UC powder.
According to the embodiment of the application, for U 3 O 8 The sintering temperature of the mixed powder with carbon is 1500 deg.C, 1600 deg.C, 1700 deg.C, etc.
According to the embodiment of the application, for U 3 O 8 The sintering time for sintering the mixed powder with carbon may be selected from 2 hours, 3 hours, 4 hours, and the like.
According to an embodiment of the present application, a method of preparing nanoscale NbC powder comprises: nbC powder with the granularity of 10-20 mu m is subjected to ball milling treatment to obtain nanoscale NbC powder.
According to embodiments of the present application, the particle size of the NbC powder may be selected to be 10 μm, 15 μm, 20 μm, and the like.
According to an embodiment of the present application, a method of preparing a nanoscale TaC powder comprises: and carrying out ball milling treatment on the TaC powder with the granularity of 20-40 mu m to obtain the nano-scale TaC powder.
According to the examples of the present application, the particle size of the TaC powder may be chosen to be 20 μm, 30 μm, 40 μm, etc.
According to the embodiment of the application, after mixing nanoscale TaC powder, nanoscale NbC powder, nanoscale UC powder, zinc stearate and uranium powder, performing ball milling treatment to obtain UC-NbC-TaC-U mixed powder, wherein the conditions of the ball milling treatment comprise: an ethanol wet method is adopted, the ball milling rotating speed is 400-600 rpm, and the ball milling time is 6-10 h.
According to the embodiment of the application, when the ball milling treatment is performed after the nano-scale TaC powder, the nano-scale NbC powder, the nano-scale UC powder, the zinc stearate and the uranium powder are mixed, the ball milling rotating speed can be selected from 400rpm, 500rpm, 600rpm and the like.
According to the embodiment of the application, when the ball milling treatment is carried out after the nano-scale TaC powder, the nano-scale NbC powder, the nano-scale UC powder, the zinc stearate and the uranium powder are mixed, the ball milling time can be selected to be 6h, 8h, 10h and the like.
According to the embodiment of the application, the nano-scale powder material has small particle size and high reactivity, can effectively improve the reactivity and is beneficial to improving the density of the fuel pellet.
According to the embodiment of the application, in the hot-pressing sintering treatment of the UC-NbC-TaC-U mixed powder to obtain the initial fuel pellet, the conditions of the hot-pressing sintering treatment comprise: the pressure is 60-100 MPa, the temperature is 1550-1755 ℃, and the heat preservation time is 1-3 h.
According to the embodiment of the application, when the UC-NbC-TaC-U mixed powder is subjected to hot-pressing sintering treatment, the pressure can be selected from 60MPa, 80MPa, 100MPa and the like.
According to the embodiment of the application, when the UC-NbC-TaC-U mixed powder is subjected to hot-pressing sintering treatment, the temperature can be selected to be 1550 ℃, 1650 ℃, 1750 ℃ and the like.
According to the embodiment of the application, when the UC-NbC-TaC-U mixed powder is subjected to hot-pressing sintering treatment, the heat preservation time can be selected to be 1h, 2h, 3h and the like.
According to an embodiment of the present application, reacting an initial fuel pellet at a first temperature for a first length of time with flowing hydrogen to remove free carbon, resulting in a (U, nb, ta) C quaternary fuel pellet comprising: under the vacuum degree of (1-3) × 10 - 3 Pa, and under the condition of introducing flowing hydrogen, reacting the initial fuel pellet for 1-3 h at a first temperature of 1600-1755 ℃ to remove free carbon, thus obtaining the (U, nb, ta) C quaternary fuel pellet.
According to the embodiment of the present application, the degree of vacuum may be selected to be 1 × 10 -3 Pa、2×10 -3 Pa、3×10 -3 Pa, and the like.
According to an embodiment of the present application, the first temperature may be selected to be 1600 ℃, 1700 ℃, 1755 ℃, and the like.
According to the embodiment of the application, the first time period can be selected to be 1h, 2h, 3h and the like.
According to embodiments of the present application, the introduction of hydrogen at high temperatures may remove free carbon from the initial fuel pellets, wherein the hydrogen decarbonizersIs considered to be C and H 2 Reaction to form CH 4 ，C+H 2 →CH 4 。
According to the examples of the present application, the relative density of the pellet obtained by applying the preparation method for preparing the (U, nb, ta) C quaternary fuel pellet proposed by the present application can reach more than 92% TD, the content of C impurities is less than 0.3wt%, the content of O impurities is less than 0.1wt%, and the pellet has excellent thermophysical properties.
According to embodiments of the present application, the relative density is equal to the true density divided by the theoretical density.
In order to make the objects, technical solutions and advantages of the present application more apparent, the present application is further described in detail with reference to specific embodiments below. It should be noted that the described embodiments are only a part of the embodiments of the present application, and not all embodiments. Other embodiments, which can be derived by one of ordinary skill in the art from the embodiments given herein without making any creative effort, shall fall within the scope of the present disclosure.
Example 1
A method of making a fuel pellet comprising:
s1: u is respectively measured according to the molar ratio of 1:7 3 O 8 Putting the powder and carbon powder into a ball mill for ball milling treatment to obtain nano-scale U 3 O 8 And mixed powder of carbon. Nano-scale U 3 O 8 And placing the mixed powder with carbon into a vacuum sintering furnace, and carrying out heat preservation treatment for 2 hours at the temperature of 1500 ℃ to obtain the nanoscale UC powder.
NbC powder with the initial particle size of 10-20 mu m is taken and put into a ball mill for ball milling treatment, so as to obtain nano NbC powder with the particle size of 700-900 nm.
TaC powder with the initial granularity of 20-40 mu m is taken and put into a ball mill for ball milling treatment, and nanoscale TaC powder with the granularity of 800-900 nm is obtained.
S2: respectively measuring nanoscale TaC powder, nbC powder and UC powder according to the mol ratio of 1.
Wherein, the ball milling process is an ethanol wet method, the ball milling rotating speed is preferably 300rpm, and the ball milling time is 1h.
S3: and (3) loading the nanoscale UC-NbC-TaC-U mixed powder prepared in the step (S2) into a graphite die, and carrying out heat preservation for 1 hour by adopting a hot-pressing sintering process under the conditions that the pressure is 60MPa and the temperature is 1550 ℃ to prepare an initial fuel pellet.
Wherein, the ball milling process is an ethanol wet method, the ball milling rotating speed is preferably 400rpm, and the ball milling time is 6h.
S4: putting the initial fuel pellets prepared in the step S3 into a high-temperature sintering furnace, and vacuumizing until the pressure is 1 multiplied by 10 -3 After Pa, flowing H is passed 2 And (3) preserving the temperature of the gas for 1h at 1600 ℃, and removing residual trace C to obtain the (U, nb, ta) C fuel pellet.
Among them, the (U, nb, ta) C fuel pellets produced in this example had an oxygen content of 50ppm, a carbon content of 85ppm, a density of 92.3% TD, and it was found that the pellets produced by the method provided herein had a relative density of 92% TD or more and a carbon-oxygen impurity content of less than 90ppm.
Example 2
A method of making a fuel pellet comprising:
s1: u is respectively measured according to the molar ratio of 1:8 3 O 8 Putting the powder and carbon powder into a ball mill for ball milling treatment to obtain nanoscale U 3 O 8 And mixed powder of carbon. Nano-scale U 3 O 8 And placing the mixed powder with carbon into a vacuum sintering furnace, and carrying out heat preservation treatment for 3 hours at the temperature of 1600 ℃ to obtain the nanoscale UC powder.
NbC powder with the initial particle size of 10-20 mu m is taken and put into a ball mill for ball milling treatment, so as to obtain nano NbC powder with the particle size of 700-900 nm.
TaC powder with the initial granularity of 20-40 mu m is taken and put into a ball mill for ball milling treatment, so as to obtain nano-scale TaC powder with the granularity of 800-900 nm.
S2: respectively measuring nanoscale TaC powder, nbC powder and UC powder according to the mol ratio of 1.
Wherein, the ball milling process is an ethanol wet method, the ball milling rotating speed is preferably 400rpm, and the ball milling time is 2h.
S3: and (3) loading the nano UC-NbC-TaC-U mixed powder prepared in the step (S2) into a graphite die, and preserving heat for 2 hours by adopting a hot-pressing sintering process under the conditions that the pressure is 80MPa and the temperature is 1650 ℃ to prepare an initial fuel pellet.
Wherein, the ball milling process is an ethanol wet method, the ball milling rotating speed is preferably 500rpm, and the ball milling time is 8h.
S4: putting the initial fuel pellets prepared in the step S3 into a high-temperature sintering furnace, and vacuumizing until the pressure is 2 multiplied by 10 -3 After Pa, flowing H is passed 2 And (3) preserving the temperature of the gas for 2h at 1700 ℃, and removing residual trace C to obtain the (U, nb, ta) C fuel pellet.
Among them, the (U, nb, ta) C fuel pellets produced in this example had an oxygen content of 48ppm, a carbon content of 76ppm, a density of 93.1% TD, and it was found that the pellets produced by the method provided herein had a relative density of 92% TD or more and a carbon-oxygen impurity content of less than 90ppm.
Example 3
A method of making a fuel pellet comprising:
s1: u is respectively measured according to the molar ratio 1:9 3 O8 powder and carbon powder are put into a ball mill for ball milling treatment to obtain nano-scale U 3 O 8 And mixed powder of carbon. And (3) putting the mixed powder into a vacuum sintering furnace, and preserving the heat for 4 hours at the temperature of 1700 ℃ to prepare the nanoscale UC powder.
NbC powder with the initial granularity of 10-20 mu m is taken and put into a ball mill for ball milling treatment, and the nano NbC powder with the granularity of 700-900 nm is obtained.
TaC powder with the initial granularity of 20-40 mu m is taken and put into a ball mill for ball milling treatment, and nanoscale TaC powder with the granularity of 800-900 nm is obtained.
S2: respectively measuring nanoscale TaC powder, nbC powder and UC powder according to the mol ratio of 1.
Wherein, the ball milling process is an ethanol wet method, the ball milling rotating speed is preferably 500rpm, and the ball milling time is 3h.
S3: and (3) loading the nano UC-NbC-TaC-U mixed powder prepared in the step (S2) into a graphite die, and preserving heat for 3 hours by adopting a hot-pressing sintering process under the conditions that the pressure is 100MPa and the temperature is 1755 ℃ to prepare an initial fuel pellet.
Wherein, the ball milling process is an ethanol wet method, the ball milling rotating speed is preferably 600rpm, and the ball milling time is 10 hours.
S4: putting the initial fuel pellets prepared in the step S3 into a high-temperature sintering furnace, and vacuumizing until the pressure is 3 multiplied by 10 -3 After Pa, flowing H is passed 2 And (3) preserving the temperature of the gas for 3 hours at 1800 ℃, and removing residual trace C to obtain the (U, nb, ta) C fuel pellet.
Among them, the (U, nb, ta) C fuel pellets produced in this example had an oxygen content of 42ppm, a carbon content of 65ppm, a density of 93.5% td, and it was found that the pellets produced by the method provided herein had a relative density of 92% td or more and a carbon-oxygen impurity content of less than 90ppm.
The present invention is not limited to the above embodiments, and various changes can be made without departing from the spirit of the present invention within the knowledge of those skilled in the art. The prior art can be used for all the matters not described in detail in this application.
Claims (10)
1. A method of making a fuel pellet comprising:
mixing nanoscale TaC powder, nanoscale NbC powder, nanoscale UC powder, zinc stearate and uranium powder, and then performing ball milling treatment to obtain UC-NbC-TaC-U mixed powder;
carrying out hot-pressing sintering treatment on the UC-NbC-TaC-U mixed powder to obtain an initial fuel pellet;
reacting the initial fuel pellets for a first length of time at a first temperature with flowing hydrogen to remove free carbon to obtain (U, nb, ta) C quaternary fuel pellets, wherein the first temperature is greater than 1200 ℃.
2. The production method according to claim 1,
the mass ratio of the nanoscale TaC powder to the nanoscale NbC powder to the nanoscale UC powder is 1 (3-5) to 4-6;
the addition amount of the zinc stearate is 0.3-0.5% of the total mass of the nanoscale TaC powder, the nanoscale NbC powder and the nanoscale UC powder;
the added amount of the uranium powder is 1-3% of the total mass of the nanoscale TaC powder, the nanoscale NbC powder and the nanoscale UC powder.
3. The production method according to claim 1 or 2,
the granularity range of the nano UC powder is 500-900 nm;
the particle size range of the nano NbC powder is 700-900 nm;
the particle size range of the nano-scale TaC powder is 800-900 nm.
4. The method of claim 3, wherein the method of preparing the nanoscale UC powder comprises:
will U 3 O 8 Mixing the powder and carbon powder and then carrying out ball milling treatment to obtain U 3 O 8 And carbon, wherein the U is 3 O 8 The particle size range of the mixed powder of the carbon and the carbon is 500-900 nm;
for the U 3 O 8 And sintering the mixed powder of the carbon to obtain the nanoscale UC powder.
5. The method according to claim 4, wherein the U is 3 O 8 The molar ratio of the powder to the carbon powder is 1 (7-9).
6. The method according to claim 4, wherein the addition of U is carried out 3 O 8 Mixing the powder and the carbon powder and then carrying out ball milling treatment to obtain U 3 O 8 And carbon, the mixed powder comprising:
will be the U 3 O 8 Mixing the powder with the carbon powder, and performing ball milling treatment for 1-3 h by adopting an ethanol wet method under the condition that the ball milling rotating speed is 300-500 rpm to obtain the U 3 O 8 And mixed powder of carbon.
7. The method according to claim 4, wherein the pair of the U 3 O 8 And sintering the mixed powder of the carbon to obtain the nanoscale UC powder, wherein the nanoscale UC powder comprises the following components:
for the U 3 O 8 And reacting the mixed powder with carbon for 2 to 4 hours at the temperature of 1500 to 1700 ℃ to obtain the nanoscale UC powder.
8. The method of claim 3, wherein the nanoscale NbC powder is prepared by a method comprising:
and ball-milling NbC powder with the particle size of 10-20 mu m to obtain the nanoscale NbC powder.
9. The method of claim 3, wherein the method of preparing the nanoscale TaC powder comprises:
and carrying out ball milling treatment on the TaC powder with the granularity of 20-40 mu m to obtain the nano-scale TaC powder.
10. The method of claim 1 wherein reacting the initial fuel pellets at a first temperature for a first length of time with flowing hydrogen to remove free carbon to obtain (U, nb, ta) C quaternary fuel pellets comprises:
under the vacuum degree of (1-3) × 10 -3 Pa, and introducing flowing hydrogen, and reacting the initial fuel pellet for 1-3 h at a first temperature of 1600-1755 ℃ to remove free carbon, thereby obtaining the (U, nb, ta) C quaternary fuel pellet.
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