CN116564562B - High-uranium-density dispersion fuel containing ZrC coating layer and preparation method thereof - Google Patents
High-uranium-density dispersion fuel containing ZrC coating layer and preparation method thereof Download PDFInfo
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- 239000000446 fuel Substances 0.000 title claims abstract description 101
- 239000006185 dispersion Substances 0.000 title claims abstract description 52
- 229910052770 Uranium Inorganic materials 0.000 title claims abstract description 39
- 239000011247 coating layer Substances 0.000 title description 24
- 238000002360 preparation method Methods 0.000 title description 20
- 239000002245 particle Substances 0.000 claims abstract description 61
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims abstract description 37
- 238000011068 loading method Methods 0.000 claims abstract description 12
- 239000002296 pyrolytic carbon Substances 0.000 claims description 80
- 239000000843 powder Substances 0.000 claims description 23
- 239000011159 matrix material Substances 0.000 claims description 18
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 claims description 13
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 claims description 13
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 9
- 229910007926 ZrCl Inorganic materials 0.000 claims description 9
- 239000001257 hydrogen Substances 0.000 claims description 9
- 229910052739 hydrogen Inorganic materials 0.000 claims description 9
- 238000005253 cladding Methods 0.000 claims description 8
- 239000011248 coating agent Substances 0.000 claims description 7
- 238000000576 coating method Methods 0.000 claims description 7
- 238000000034 method Methods 0.000 claims description 7
- 238000006243 chemical reaction Methods 0.000 claims description 2
- 230000035484 reaction time Effects 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims 1
- 241000013033 Triso Species 0.000 abstract description 39
- 239000008188 pellet Substances 0.000 abstract description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 5
- 238000011160 research Methods 0.000 abstract description 2
- 238000012360 testing method Methods 0.000 abstract description 2
- 239000010410 layer Substances 0.000 description 103
- 238000005245 sintering Methods 0.000 description 24
- 229910010271 silicon carbide Inorganic materials 0.000 description 21
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 18
- VKYKSIONXSXAKP-UHFFFAOYSA-N hexamethylenetetramine Chemical compound C1N(C2)CN3CN1CN2C3 VKYKSIONXSXAKP-UHFFFAOYSA-N 0.000 description 18
- 239000000243 solution Substances 0.000 description 17
- 229910002804 graphite Inorganic materials 0.000 description 15
- 239000010439 graphite Substances 0.000 description 15
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 9
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 9
- 239000004202 carbamide Substances 0.000 description 9
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 9
- 239000003292 glue Substances 0.000 description 9
- 239000011259 mixed solution Substances 0.000 description 9
- 238000001816 cooling Methods 0.000 description 7
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 6
- 229910000831 Steel Inorganic materials 0.000 description 6
- 235000010299 hexamethylene tetramine Nutrition 0.000 description 6
- 239000004312 hexamethylene tetramine Substances 0.000 description 6
- 239000000203 mixture Substances 0.000 description 6
- 238000004806 packaging method and process Methods 0.000 description 6
- 230000001681 protective effect Effects 0.000 description 6
- 239000010959 steel Substances 0.000 description 6
- 239000000463 material Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 238000007599 discharging Methods 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 3
- 230000032683 aging Effects 0.000 description 3
- 229910052786 argon Inorganic materials 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 238000000227 grinding Methods 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 229910017604 nitric acid Inorganic materials 0.000 description 3
- 229910002007 uranyl nitrate Inorganic materials 0.000 description 3
- 238000005406 washing Methods 0.000 description 3
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000011049 filling Methods 0.000 description 2
- 230000004992 fission Effects 0.000 description 2
- 238000005243 fluidization Methods 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000011946 reduction process Methods 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 1
- 229910021431 alpha silicon carbide Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 230000001627 detrimental effect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000003758 nuclear fuel Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Classifications
-
- 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
- G21C3/02—Fuel elements
- G21C3/04—Constructional details
- G21C3/06—Casings; Jackets
- G21C3/07—Casings; Jackets characterised by their material, e.g. alloys
-
- 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
-
- 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
Abstract
The invention relates to the technical fields of pressurized water reactors, gas cooled reactors and research and test reactors, and aims at solving the problems that the uranium loading of the existing dispersion fuel pellets is low and the extremely high temperature tolerance capability of the dispersion fuel containing TRISO particles is poor.
Description
Technical Field
The invention relates to the technical field of dispersion fuels for pressurized water reactors, gas cooled reactors and research test reactors, in particular to a high uranium density dispersion fuel containing a ZrC coating layer and a preparation method thereof.
Background
An important direction of the current nuclear power technology development is to improve the safety and reliability of a nuclear power system and avoid the rutting of nuclear power accidents such as Japanese Fudao. At present, the internationally proposed structure of the universal accident-resistant fuel is that TRISO particles with three-way isotropy are dispersed in a SiC matrix material, a containing space is provided for fission gas by utilizing four layers of cladding layers of the TRISO particles, and the SiC matrix material which has good thermal conductivity, small thermal expansion coefficient, low neutron absorption section and excellent compatibility with cladding and fuel is adopted to improve the safety characteristic of the fuel.
TRISO particles dispersed in SiC matrix, despite their high safety characteristics, can lead to a significant reduction in uranium loading in the fuel, affecting the economic applicability of the overall dispersed fuel.
The four-layer coating structure of the TRISO particles at present comprises a loose pyrolytic carbon layer, an inner compact pyrolytic carbon layer, a SiC layer and an outer compact pyrolytic carbon layer from inside to outside. The third SiC layer is a key for bearing internal and external pressure and guaranteeing the integrity of the fuel core, but in order to further improve the economy of the reactor, the improvement of the outlet temperature of the reactor is an important means. The SiC can be transformed into hexagonal alpha-SiC from face-centered cubic beta-SiC at 1800 ℃ and is released by irradiation 137 The amount of Cs is also high. This would be detrimental to increasing the operating temperature of the reactor, affecting further popularization of the deep application of TRISO particle dispersion fuel.
Disclosure of Invention
The invention aims to provide a high uranium density dispersion fuel containing a ZrC coating layer and a preparation method thereof, which solve the problem of low uranium loading of dispersion fuel pellets, improve the uranium loading in the dispersion fuel by 7% -30%, and solve the problem of poor capability of the dispersion fuel containing TRISO particles in tolerating extremely high temperature (more than or equal to 1800 ℃).
In order to achieve the above object, the present invention provides the following technical solutions:
the high uranium density dispersion fuel comprises coated fuel particles, a matrix and a fuel-free region, wherein the coated fuel particles comprise a fuel core and a loose pyrolytic carbon layer, an inner dense pyrolytic carbon layer, a ZrC layer and an outer dense pyrolytic carbon layer which are sequentially coated outside the fuel core, the thickness of the ZrC layer is 17-45 mu m, and the thickness of the outer dense pyrolytic carbon layer is 0-30 mu m.
Further, the fuel core is UCO core with diameter of 500-800 μm.
Further, the thickness of the loose pyrolytic carbon layer is 50-120 mu m, and the thickness of the inner compact pyrolytic carbon layer is 30-60 mu m.
Further, the thickness of the loose pyrolytic carbon layer was 90.7 μm, the thickness of the inner dense pyrolytic carbon layer was 38.6 μm, the thickness of the ZrC layer was 17.6 μm, and the thickness of the outer dense pyrolytic carbon layer was 20.9 μm.
Further, the fuel core is a UN core with a diameter of 500-800 μm.
Further, the thickness of the loose pyrolytic carbon layer is 50-120 mu m, the thickness of the inner dense pyrolytic carbon layer is 30-60 mu m, and the thickness of the outer dense pyrolytic carbon layer is 0 mu m.
Further, the thickness of the loose pyrolytic carbon layer was 52.2 μm, the thickness of the inner dense pyrolytic carbon layer was 36 μm, and the thickness of the ZrC layer was 44.7. Mu.m.
Further, the matrix is a SiC matrix.
Further, after an inner dense pyrolytic carbon layer is prepared in a fluidized bed, hydrogen and ZrCl are introduced 4 Powder, wherein the flow rate of hydrogen is 70-380L/min, zrCl 4 The powder is introduced at a speed of 70-190 g/min until hydrogen and ZrCl are introduced 4 After the powder is input stably, propylene and ZrCl are introduced 4 The powder is reacted, the propylene flow is 3-10L/min, the reaction time is 30-80 min, and the ZrC layer is obtained after the reaction.
Further, after the ZrC layer is prepared, acetylene and propylene are introduced to react to obtain an outer compact pyrolytic carbon layer, and the outer compact pyrolytic carbon layer is cooled to room temperature in a particle fluidization state and then discharged to obtain coated fuel particles; or after the ZrC layer is prepared, directly cooling to room temperature in a particle fluidization state, and discharging to obtain the coated fuel particles.
Compared with the prior art, the high uranium density dispersion fuel containing the ZrC coating layer and the preparation method thereof have the following beneficial effects:
according to the invention, the thickness of the dense pyrolytic carbon layer of the outermost layer of the TRISO particles is reduced from 40 mu m to 0-30 mu m, so that the diameter size of the TRISO particles can be reduced, and the uranium loading amount of the dispersion fuel can be improved under the condition of the same loading volume.
In UO of 500 μm 2 The core is exemplified by a porous pyrolytic carbon having a thickness of 95 μm, an inner dense pyrolytic carbon having a thickness of 40 μm, a SiC having a thickness of 35 μm, and an outer dense pyrolytic carbon having a thickness of both 40 μm and 0 μm. Both TRISO particles are filled in pellets with phi of 8.43mm x 10.92mm, and when the filling volume of the TRISO particles is 40%, the uranium content of the fuel pellets with the thickness of the outer dense pyrolytic carbon layer of 0 μm is increased by 30% compared with the uranium content of the fuel pellets with the thickness of the outer dense pyrolytic carbon layer of 40 μm.
According to the invention, the SiC layer in the TRISO particles is changed into the ZrC layer, so that the running temperature and the outlet temperature of the reactor can be improved, the ZrC layer does not generate phase change below 3540 ℃ (the melting point of the ZrC layer), and the integrity of the TRISO particles can be better protected; at the same time, the ZrC layer and palladium hardly react, has good capacity of containing fission products.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments will be briefly described below.
FIG. 1 is a schematic view of coated fuel particles according to example 1 of the present invention;
fig. 2 is a schematic view of a dispersion fuel according to embodiment 1 of the present invention.
Reference numerals illustrate:
1. a fuel core; 2. loosening the pyrolytic carbon layer; 3. an inner dense pyrolytic carbon layer; 4. a ZrC layer; 5. an outer dense pyrolytic carbon layer; 6. TRISO particles; 7. a SiC matrix; 8. and a fuel-free zone.
Detailed Description
Further details are provided below with reference to the specific embodiments.
The invention provides a high uranium density dispersion fuel containing a ZrC coating layer, which improves the uranium loading in the dispersion fuel and improves the high temperature resistance of the dispersion fuel.
According to the invention, the ZrC layer is adopted to replace a third SiC layer in the TRISO particles, so that the excellent oxidation resistance and high temperature resistance of the ZrC material are fully exerted, the high temperature resistance of the TRISO particle dispersion fuel at a higher operating temperature (more than 1800 ℃) is further improved, and the application of the TRISO particle dispersion fuel in a harsher environment is promoted.
The main function of the dense pyrolytic carbon layer of the outermost layer of the TRISO particles (coated fuel particles) is to protect the third layer and provide supporting force for the third layer, and the design is mainly due to the fact that the initial application of the TRISO particles is that pyrolytic carbon and graphite are of homologous materials on a graphite matrix, so that the outer dense pyrolytic carbon layer of the outermost layer can have good compatibility with the graphite matrix. According to the invention, after the ZrC layer is adopted to replace the SiC layer, the great difference between the thermal expansion coefficient of the outermost pyrolytic carbon layer and the ZrC layer is considered, so that the invention provides two schemes for solving, namely, the thickness of the outer dense pyrolytic carbon layer of the outermost layer is thinned to be less than 0 mu m and less than or equal to 30 mu m, and the uranium loading in the dispersion fuel can be effectively improved. The outmost dense pyrolytic carbon layer with the thickness of 30 mu m is the standard thickness dimension of TRISO particle dressing, and in the invention, the outmost dense pyrolytic carbon layer with the thickness of 30 mu m can be used as a spacing layer among TRISO particles for preventing deformation caused by mutual extrusion in the filling and forming process of the TRISO particles. And secondly, the outermost outer dense pyrolytic carbon layer is removed, that is to say, the thickness of the outer dense pyrolytic carbon layer is 0 mu m, so that the uranium loading in the dispersion fuel is improved, and meanwhile, the compatibility of the TRISO particles and the heat conducting performance of the SiC matrix can be improved. Therefore, the thickness of the outer dense pyrolytic carbon layer of the outermost layer of the high uranium density dispersion fuel containing the ZrC coating layer is 0-30 mu m, namely, the thickness of the outer dense pyrolytic carbon layer is more than or equal to 0 mu m and less than or equal to 30 mu m.
Therefore, the thickness of the outer compact pyrolytic carbon layer is reduced, the SiC layer in the TRISO particles is changed into the ZrC layer, and the integral uranium loading and high temperature resistance of the TRISO particle dispersion fuel can be improved through the combined design, so that the TRISO particle dispersion fuel can be favorably popularized and applied to special-purpose reactors with high burnup and high outlet temperature, the efficient and safe operation of the fuel is realized, and the wider application is promoted.
In the invention, the thickness of the loose pyrolytic carbon layer is 50-120 mu m, the thickness of the inner compact pyrolytic carbon layer is 30-60 mu m, and the thickness of the ZrC layer is 17-45 mu m.
Example 1
The high uranium density dispersion fuel containing the ZrC coating layer is shown in a figure 1, wherein the coated fuel particles are a fuel core 1, a loose pyrolytic carbon layer 2, an inner dense pyrolytic carbon layer 3, a ZrC layer 4 and an outer dense pyrolytic carbon layer 5 from inside to outside in sequence.
The material composition of the fuel core 1 was UCO, and the diameter of the fuel core 1 was 500 μm. The thickness of the loose pyrolytic carbon layer 2 is 90.7 mu m, the thickness of the inner compact pyrolytic carbon layer 3 is 38.6 mu m, the thickness of the ZrC layer 4 is 17.6 mu m, and the thickness of the outer compact pyrolytic carbon layer 5 is 20.9 mu m. The coated fuel particles were dispersed in a SiC matrix, the overall pellet size being Φ 8.566mm× 12.979mm. As shown in fig. 2, the composition of the dispersion fuel is TRISO particles 6, siC matrix 7 and fuel-free zone 8, respectively.
A preparation method of high uranium density dispersion fuel containing ZrC coating layer comprises the following steps:
step 1: UCO core preparation. The UCO core is prepared by an external gel and carbothermic reduction process, and the process flow is as follows: 5000 to 5000gU 3 O 8 Slowly adding the powder into a mixed solution of 2200mL of concentrated nitric acid and 4100mL of deionized water to obtain uranyl nitrate solution (HMTA); 2.3 to 2.5g of hexamethylenetetramine and 1g of urea are mixed to prepare a mixed solution of hexamethylenetetramine and urea; adding the HMTA/urea mixed solution and 640g of carbon powder into the prepared ADUN solution to prepare a glue solution. Dispersing the mixed glue solution after standing through a dispersing head, wherein the flow rate of the glue solution is 12mL/min, and the vibration frequency is 100-120 Hz to prepare UO 3 And (3) aging, washing and drying the gel ball, and finally roasting the gel ball at 1700 ℃ in a CO atmosphere to obtain the UCO core.
Step 2: preparing TRISO particles. Placing 3000g UCO core into a fluidized bed, heating the fluidized bed to 1150 ℃, introducing argon (67L/min flow) and acetylene (175L/min flow) for 2min,obtaining loose pyrolytic carbon; introducing acetylene (flow is 60L/min) and propylene (60L/min), and reacting for 10min to obtain the internal compact pyrolytic carbon; introducing hydrogen (flow is 72L/min) and ZrCl 4 Powder (70 g/min) and propylene (flow 3L/min) for 30min to obtain ZrC layer; introducing acetylene (flow is 30L/min) and propylene (flow is 30L/min) for 5min to obtain the outer compact pyrolytic carbon layer. And after coating, cooling the TRISO particles along with a furnace in a fluidized state, and discharging from the bottom after cooling to room temperature to obtain the TRISO particles.
Step 3: preparation of fuel pellets. The particles containing ZrC coating layer are mixed with SiC powder and 3 to 7 percent of sintering aid powder (Al 2 O 3 And Y 2 O 3 ) Uniformly mixing, wherein the volume ratio of the particles of the ZrC coating layer is 41%. And (3) preparing the composite powder filled into the steel die into a green body under the condition of 1-1.5 KN by using a unidirectional press matched with the steel die. Packaging the prepared green compact into a graphite mold, and after packaging, placing the graphite mold into a hot-press sintering furnace, wherein the temperature of the hot-press sintering furnace is controlled to be 1650-1750 ℃, and sintering is performed under protective atmosphere or vacuum; or placing the graphite mould into a discharge plasma sintering furnace, controlling the temperature of the discharge plasma sintering furnace to 1750-1850 ℃, and sintering under protective atmosphere or vacuum. And taking out the graphite mold after sintering, taking out the dispersion fuel in a demolding or disintegration mode, and finally obtaining the high uranium density dispersion fuel containing the ZrC coating layer in an outer surface grinding mode.
Example 2
The high uranium density dispersion fuel containing the ZrC coating layer comprises a fuel core, a loose pyrolytic carbon layer, an inner dense pyrolytic carbon layer, a ZrC layer and an outer dense pyrolytic carbon layer from inside to outside.
The material composition of the fuel core was UCO, and the diameter of the fuel core was 650. Mu.m. The thickness of the loose pyrolytic carbon layer is 111.3 mu m, the thickness of the inner compact pyrolytic carbon layer is 41.4 mu m, the thickness of the ZrC layer is 27.8 mu m, and the thickness of the outer compact pyrolytic carbon layer is 29.5 mu m. The coated fuel particles were dispersed in a SiC matrix, the overall pellet size being Φ 8.566mm× 12.979mm. The composition of the dispersion fuel is TRISO particles, siC matrix and fuel-free zone respectively.
A preparation method of high uranium density dispersion fuel containing ZrC coating layer comprises the following steps:
step 1: UCO core preparation. The UCO core is prepared by an external gel and carbothermic reduction process, and the process flow is as follows: 5000 to 5000gU 3 O 8 Slowly adding the powder into a mixed solution of 2200mL of concentrated nitric acid and 4100mL of deionized water to obtain uranyl nitrate solution (HMTA); 2.3 to 2.5g of hexamethylenetetramine and 1g of urea are mixed to prepare a mixed solution of hexamethylenetetramine and urea; adding the HMTA/urea mixed solution and 640g of carbon powder into the prepared ADUN solution to prepare a glue solution. Dispersing the mixed glue solution after standing through a dispersing head, wherein the flow rate of the glue solution is 12mL/min, and the vibration frequency is 100-120 Hz to prepare UO 3 And (3) aging, washing and drying the gel ball, and finally roasting the gel ball at 1700 ℃ in a CO atmosphere to obtain the UCO core.
Step 2: preparing TRISO particles. Placing 3000g of UCO core into a fluidized bed, heating the fluidized bed to 1150 ℃, introducing argon (with the flow of 60L/min) and acetylene (with the flow of 171L/min), and reacting for 2min to obtain loose pyrolytic carbon; introducing acetylene (with the flow of 84L/min) and propylene (with the flow of 88L/min) for 10min to obtain the internal compact pyrolytic carbon; introducing hydrogen (flow rate is 216L/min) and ZrCl 4 Powder (123 g/min) and propylene (flow 5L/min) for 40min to obtain ZrC layer; introducing acetylene (flow is 75L/min) and propylene (96L/min) for 7min to obtain the outer compact pyrolytic carbon layer. And after coating, cooling the TRISO particles along with a furnace in a fluidized state, and discharging from the bottom after cooling to room temperature to obtain the TRISO particles.
Step 3: preparation of fuel pellets. The particles containing ZrC coating layer are mixed with SiC powder and 3 to 7 percent of sintering aid powder (Al 2 O 3 And Y 2 O 3 ) Uniformly mixing, wherein the volume ratio of the particles of the ZrC coating layer is 41%. And (3) preparing the composite powder filled into the steel die into a green body under the condition of 1-1.5 KN by using a unidirectional press matched with the steel die. Packaging the prepared green body into a graphite mold, and after packaging, placing the graphite mold into a hot-press sintering furnaceThe temperature of (2) is controlled between 1650 and 1750 ℃, and sintering is carried out under protective atmosphere or vacuum; or placing the graphite mould into a discharge plasma sintering furnace, controlling the temperature of the discharge plasma sintering furnace to 1750-1850 ℃, and sintering under protective atmosphere or vacuum. And taking out the graphite mold after sintering, taking out the dispersion fuel in a demolding or disintegration mode, and finally obtaining the high uranium density dispersion fuel containing the ZrC coating layer in an outer surface grinding mode.
Example 3
A high uranium density dispersion fuel containing a ZrC coating layer comprises a fuel core, a loose pyrolytic carbon layer, an inner compact pyrolytic carbon layer and a ZrC layer from inside to outside. Example 3 the outer dense pyrolytic carbon layer was not coated with the ZrC layer.
The material composition of the fuel core was UN, and the diameter of the fuel core was 800 μm. The thickness of the loose pyrolytic carbon layer is 52.2 mu m, the thickness of the inner compact pyrolytic carbon layer is 36 mu m, and the thickness of the ZrC layer is 44.7 mu m. The coated fuel particles were dispersed in a SiC matrix with the overall pellet size Φ21.6mm×22.2mm. The composition of the dispersion fuel is TRISO particles, siC matrix and fuel-free zone respectively.
A preparation method of high uranium density dispersion fuel containing ZrC coating layer comprises the following steps:
step 1: UN core preparation. The preparation of the UN core is carried out through an external gel, carbothermic reduction and nitridation process, and the process flow is as follows: 5000 to 5000gU 3 O 8 Slowly adding the powder into a mixed solution of 2200mL of concentrated nitric acid and 4100mL of deionized water to obtain uranyl nitrate solution (HMTA); 2.3 to 2.5g of hexamethylenetetramine and 1g of urea are mixed to prepare a mixed solution of hexamethylenetetramine and urea; adding the HMTA/urea mixed solution and 530g of carbon powder into the prepared ADUN solution to prepare a glue solution. Dispersing the mixed glue solution after standing through a dispersing head, wherein the flow rate of the glue solution is 12mL/min, and the vibration frequency is 100-120 Hz to prepare UO 3 Gel ball/C, aging, washing and drying, and finally adding into N 2 Roasting at 1900 ℃ in the atmosphere to prepare the UN core.
Step 2: preparing TRISO particles. 3000g of UN cores were placed in a fluidized bed, which was warmed to 11Introducing argon (with the flow of 20L/min) and acetylene (with the flow of 60L/min) at 50 ℃ for 2min to obtain loose pyrolytic carbon; introducing acetylene (flow is 35L/min) and propylene (flow is 35L/min) for 7min to obtain the internal compact pyrolytic carbon; introducing hydrogen (flow is 380L/min) and ZrCl 4 Powder (185 g/min) and propylene (flow 10L/min) for 75min to obtain ZrC layer. And after coating, cooling the TRISO particles along with a furnace in a fluidized state, and discharging from the bottom after cooling to room temperature to obtain the TRISO particles.
Step 3: preparation of fuel pellets. The particles containing ZrC coating layer are mixed with SiC powder and 3 to 7 percent of sintering aid powder (Al 2 O 3 And Y 2 O 3 ) Uniformly mixing, wherein the volume ratio of the particles of the ZrC coating layer is 41%. And (3) preparing the composite powder filled into the steel die into a green body under the condition of 1-1.5 KN by using a unidirectional press matched with the steel die. Packaging the prepared green compact into a graphite mold, and after packaging, placing the graphite mold into a hot-press sintering furnace, wherein the temperature of the hot-press sintering furnace is controlled to be 1650-1750 ℃, and sintering is performed under protective atmosphere or vacuum; or placing the graphite mould into a discharge plasma sintering furnace, controlling the temperature of the discharge plasma sintering furnace to 1750-1850 ℃, and sintering under protective atmosphere or vacuum. And taking out the graphite mold after sintering, taking out the dispersion fuel in a demolding or disintegration mode, and finally obtaining the high uranium density dispersion fuel containing the ZrC coating layer in an outer surface grinding mode.
The preparation method provided by the invention realizes the preparation of the high uranium density dispersion fuel pellet with the ZrC layer containing the ultra-high temperature coating layer. The purpose of preparing the core block is achieved through several key technological methods such as core preparation, TRISO particle preparation containing an ultra-high temperature coating layer, green body preparation, core block sintering and the like. The prepared core block can meet the technical condition requirements of core entering blocks in the aspects of out-of-core performance test of density, size, thermophysical performance, mechanical performance and the like, and is mainly applied to fuel stacks corresponding to the technical conditions, so that the use standard of nuclear fuel elements is met.
The invention can improve the problem of low uranium loading in the current dispersion fuel, improves the overall economic characteristic of the fuel, improves the high temperature resistance of the dispersion fuel, prolongs the fuel refueling period, accelerates the commercial application of the fuel and can popularize the application of the fuel in the directions of ultra-temperature gas cooled reactors, gas cooled micro-reactors, nuclear heat rocket engines and the like.
The foregoing is merely illustrative of the present invention, and the present invention is not limited thereto, and any changes or substitutions easily contemplated by those skilled in the art within the scope of the present invention should be included in the scope of the present invention. Therefore, the protection scope of the present invention shall be subject to the protection scope of the claims.
Claims (8)
1. The high uranium density dispersion fuel comprises coated fuel particles, a SiC matrix and a fuel-free region, and is characterized in that the coated fuel particles comprise a fuel core, a loose pyrolytic carbon layer, an inner dense pyrolytic carbon layer, a ZrC layer and an outer dense pyrolytic carbon layer which are sequentially coated outside the fuel core, the thickness of the ZrC layer is 17-45 mu m, and the thickness of the outer dense pyrolytic carbon layer is 0 mu m, so that uranium loading in the dispersion fuel is improved, and compatibility of the coated fuel particles and heat conducting performance of the SiC matrix is improved.
2. The high uranium density dispersion fuel containing a ZrC cladding according to claim 1, wherein the fuel core is a UCO core having a diameter of 500-800 μm.
3. The high uranium density dispersion fuel containing a ZrC cladding according to claim 2, wherein the loose pyrolytic carbon layer has a thickness of 50 to 120 μm and the inner dense pyrolytic carbon layer has a thickness of 30 to 60 μm.
4. The high uranium density dispersion fuel containing a ZrC cladding according to claim 1, wherein the fuel core is a UN core having a diameter of 500 to 800 μm.
5. The high uranium density dispersion fuel containing a ZrC cladding of claim 4, wherein the loose pyrolytic carbon layer is 50 to 120 μm thick, the inner dense pyrolytic carbon layer is 30 to 60 μm thick, and the outer dense pyrolytic carbon layer is 0 μm thick.
6. The high uranium density dispersion fuel containing a ZrC cladding of claim 5, wherein the loose pyrolytic carbon layer has a thickness of 52.2 μm, the inner dense pyrolytic carbon layer has a thickness of 36 μm, and the ZrC layer has a thickness of 44.7 μm.
7. A process for preparing a high uranium density dispersion fuel containing a ZrC cladding layer as claimed in any one of claims 1 to 6, characterized in that after preparing an inner dense pyrolytic carbon layer in a fluidized bed, hydrogen and ZrCl are introduced 4 Powder, wherein the flow rate of hydrogen is 70-380L/min, zrCl 4 The powder is introduced at a speed of 70-190 g/min until hydrogen and ZrCl are introduced 4 After the powder is input stably, propylene and ZrCl are introduced 4 The powder is reacted, the propylene flow is 3-10L/min, the reaction time is 30-80 min, and the ZrC layer is obtained after the reaction.
8. The method for preparing a high uranium density dispersion fuel containing a ZrC coating according to claim 7, wherein after the ZrC coating is prepared, the ZrC coating is directly cooled to room temperature in a fluidized state and then discharged to obtain coated fuel particles.
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