CN113012833A - Preparation method of uranium nitride composite uranium dioxide fuel pellet - Google Patents
Preparation method of uranium nitride composite uranium dioxide fuel pellet Download PDFInfo
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- CN113012833A CN113012833A CN201911325486.5A CN201911325486A CN113012833A CN 113012833 A CN113012833 A CN 113012833A CN 201911325486 A CN201911325486 A CN 201911325486A CN 113012833 A CN113012833 A CN 113012833A
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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
- 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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Abstract
The invention belongs to the technical field of preparation of uranium nitride composite fuel pellets, and particularly relates to a preparation method of a uranium nitride composite uranium dioxide fuel pellet. Preparing metal uranium powder through cyclic hydrogenation and dehydrogenation, and nitriding to obtain a uranium nitrogen compound; placing a uranium nitrogen compound in a graphite mold for prepressing, performing high-temperature denitrification in a tungsten-molybdenum sintering furnace together with the mold and the uranium nitrogen compound, obtaining a massive UN material after denitrification, and preparing UN powder which can stably exist at room temperature after crushing and ball milling; mixing UN powder with 5-80 wt% of UO2Powder is subjected to dry three-dimensional mixing or wet ball milling mixing by taking ethanol as a medium to obtain UN-UO2Mixing the powder; taking UN-UO2Placing the mixed powder in a graphite die for hot-pressing sintering to obtain solid UN-UO2A composite fuel pellet. The UN powder which can stably exist in the air is prepared by the invention, and the UN powder and the UO can be stably existed in the air under the atmospheric environment2The mixing of the powder reduces the difficulty of the process operation and shortens the process period.
Description
Technical Field
The invention belongs to the technical field of preparation of uranium nitride composite fuel pellets, and particularly relates to a preparation method of a uranium nitride composite uranium dioxide fuel pellet.
Background
And UO2Compared with fuel pellet, UN pellet has higher uranium density and heat conductivity coefficient, can obviously improve the economic benefit of nuclear fuel, because UN has poor water decay resistance and can react with water when working in a reactor, and in order to reduce the reactivity of UN, a certain amount of UO can be added into UN2Currently, internationally for UN-UO2The preparation method of the composite material mainly comprises the steps of preparing UN powder through hydrogenation dehydrogenation and nitrogenization denitrification, and adding a certain amount of UO2After the powder is mixed, the UN-UO is prepared by hot pressing and sintering2A composite material. However, in the process, the prepared UN is very easy to oxidize, all the procedures need to be carried out in a glove box, the process operation difficulty is improved, and the process period is prolonged.
Disclosure of Invention
The invention aims to provide a preparation method of a uranium nitride composite uranium dioxide fuel pellet, which can prepare UN powder capable of stably existing in air and realize the purpose of mixing with UO in atmospheric environment2The mixing of the powder reduces the difficulty of the process operation and shortens the process period.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a method for preparing a uranium nitride composite uranium dioxide fuel pellet,
(1) preparing metal uranium powder through cyclic hydrogenation and dehydrogenation, and nitriding to obtain a uranium nitrogen compound;
(2) placing a uranium nitrogen compound in a graphite mold for prepressing, performing high-temperature denitrification in a tungsten-molybdenum sintering furnace together with the mold and the uranium nitrogen compound, obtaining a massive UN material after denitrification, and preparing UN powder which can stably exist at room temperature after crushing and ball milling;
(3) mixing UN powder with 5-80 wt% of UO2Powder is subjected to dry three-dimensional mixing or wet ball milling mixing by taking ethanol as a medium to obtain UN-UO2Mixing the powder;
(4) taking UN-UO2Placing the mixed powder in a graphite die for hot-pressing sintering to obtain solid UN-UO2A composite fuel pellet.
And (1) preparing metal uranium powder through 1-5 times of circulating hydrogenation and dehydrogenation.
In the step (1), the uranium nitrogen compound is UNx，1＜X≤2。
And (2) heating the die and the uranium nitrogen compound together in a tungsten-molybdenum sintering furnace to 1360-1460 ℃ for denitrification.
And (4) carrying out spraying or brushing of yttrium oxide on the inner cavity of the graphite mold.
And (4) hot pressing pressure is 40-80 MPa, hot pressing temperature is 1500-1600 ℃, and hot pressing time is 1.5-3 hours.
The beneficial effects obtained by the invention are as follows:
the UN material which can stably exist in the atmosphere and the UO are prepared by a method of prepressing a uranium nitrogen compound in a graphite mould and heating the mould and the uranium nitrogen compound in a tungsten-molybdenum sintering furnace for denitrification2After the powders are mixed, UN-UO with certain water-decay resistance is prepared2The composite fuel pellet has wide application foreground in light water reactor.
Detailed Description
The present invention will be described in detail with reference to specific examples.
The preparation method of the uranium nitride composite uranium dioxide fuel pellet comprises the following steps:
preparing metal uranium powder through 1-5 times of cyclic hydrogenation and dehydrogenation, and nitriding to obtain uranium nitride compound (UN)xAnd X is more than 1 and less than or equal to 2), placing the uranium nitrogen compound in a graphite mold for prepressing, heating the mold and the uranium nitrogen compound in a tungsten-molybdenum sintering furnace to 1360-1460 ℃ for high-temperature denitrification, obtaining a blocky UN material after denitrification, and preparing the UN powder which can stably exist at room temperature after crushing and ball milling. Mixing UN powder with 5-80 wt% of UO2Powder is subjected to dry three-dimensional mixing or wet ball milling mixing by taking ethanol as a medium to obtain UN-UO2And mixing the powders. Taking UN-UO2The mixed powder is placed in a graphite mold for hot-press sintering in consideration of UO2The problem of reaction with graphite at high temperature is that the inner cavity of a graphite die is sprayed or brushed with yttrium oxide, the hot pressing pressure is 40-80 MPa, the hot pressing temperature is 1500-1600 ℃, the hot pressing time is 1.5-3 hours, and the solid UN-UO is prepared2A composite fuel pellet.
Examples
Cleaning an oxide layer of 1kg of metal uranium sheet by nitric acid, soaking the metal uranium sheet in alcohol to remove residual impurities on the surface, wiping the metal uranium sheet dry, placing the metal uranium sheet in a hydrogenation dehydrogenation furnace, introducing hydrogen with the pressure of 0.03-0.07 MPa, hydrogenating the metal uranium sheet at the temperature of 265-280 ℃ for 1-3 hours, vacuumizing and heating to the temperature of 530-570 ℃ for dehydrogenation for 3-5 hours, vacuumizing and cooling to the room temperature, and repeating the hydrogenation dehydrogenation process for 3 times to obtain metal uranium powder with a certain particle size;
continuously introducing nitrogen with the pressure of 0.03-0.07 MPa into the hydrogenation and dehydrogenation furnace, heating the metal uranium powder to 450-500 ℃, nitriding for 6-10 hours, and keeping the positive pressure in the furnace and cooling to room temperature to obtain a uranium nitrogen compound;
loading a uranium nitrogen compound into a phi 40mm steel die in a glove box, wrapping the uranium nitrogen compound with a plastic film after primary prepressing, taking out the glove box, placing the glove box on a four-column hydraulic press, removing the plastic film after 30-50 MPa secondary prepressing, placing the uranium nitrogen compound subjected to secondary prepressing and the die in a tungsten-molybdenum sintering furnace, heating to 1360-1460 ℃ for high-temperature denitrification to obtain a blocky UN material, and crushing and ball-milling for 10-30 min to prepare UN powder capable of stably existing at room temperature;
taking 10-20 gUN powder and 10 wt% of UO2Mixing the powder for 3-6 hours by using ethanol as a medium through a wet method, drying and sieving by using a standard sieve of 80-120 meshes to obtain uniformly mixed UN-UO2And mixing the powders.
Taking a certain amount of UN-UO2The mixed powder is placed in a graphite mold of a certain size for hot-pressing sintering in consideration of UO2The problem of reaction with graphite at high temperature is solved by adopting yttrium oxide to carry out spray brushing treatment on an inner cavity of a graphite die, wherein the hot pressing pressure is 40-80 MPa, the hot pressing temperature is 1500-1600 ℃, the hot pressing time is 1.5-3 hours, and solid UN-UO with a certain size is prepared2A composite fuel pellet.
Claims (6)
1. A preparation method of a uranium nitride composite uranium dioxide fuel pellet is characterized by comprising the following steps:
(1) preparing metal uranium powder through cyclic hydrogenation and dehydrogenation, and nitriding to obtain a uranium nitrogen compound;
(2) placing a uranium nitrogen compound in a graphite mold for prepressing, performing high-temperature denitrification in a tungsten-molybdenum sintering furnace together with the mold and the uranium nitrogen compound, obtaining a massive UN material after denitrification, and preparing UN powder which can stably exist at room temperature after crushing and ball milling;
(3) mixing UN powder with 5-80 wt% of UO2Powder is subjected to dry three-dimensional mixing or wet ball milling mixing by taking ethanol as a medium to obtain UN-UO2Mixing the powder;
(4) taking UN-UO2Placing the mixed powder in a graphite die for hot-pressing sintering to obtain solid UN-UO2A composite fuel pellet.
2. The method of preparing a uranium nitride composite uranium dioxide fuel pellet according to claim 1, wherein: and (1) preparing metal uranium powder through 1-5 times of circulating hydrogenation and dehydrogenation.
3. The method of preparing a uranium nitride composite uranium dioxide fuel pellet according to claim 1, wherein: in the step (1), the uranium nitrogen compound is UNx，1＜X≤2。
4. The method of preparing a uranium nitride composite uranium dioxide fuel pellet according to claim 1, wherein: and (2) heating the die and the uranium nitrogen compound together in a tungsten-molybdenum sintering furnace to 1360-1460 ℃ for denitrification.
5. The method of preparing a uranium nitride composite uranium dioxide fuel pellet according to claim 1, wherein: and (4) carrying out spraying or brushing of yttrium oxide on the inner cavity of the graphite mold.
6. The method of preparing a uranium nitride composite uranium dioxide fuel pellet according to claim 1, wherein: and (4) hot pressing pressure is 40-80 MPa, hot pressing temperature is 1500-1600 ℃, and hot pressing time is 1.5-3 hours.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201911325486.5A CN113012833A (en) | 2019-12-20 | 2019-12-20 | Preparation method of uranium nitride composite uranium dioxide fuel pellet |
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| CN201911325486.5A CN113012833A (en) | 2019-12-20 | 2019-12-20 | Preparation method of uranium nitride composite uranium dioxide fuel pellet |
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| CN113012833A true CN113012833A (en) | 2021-06-22 |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2023130356A1 (en) * | 2022-01-07 | 2023-07-13 | 岭澳核电有限公司 | High-uranium-density atf nuclear fuel pellet and preparation method therefor |
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| CN103466568A (en) * | 2013-09-09 | 2013-12-25 | 中国原子能科学研究院 | Preparation method of uranium nitride fuel powder and pellet |
| CN107256726A (en) * | 2017-07-03 | 2017-10-17 | 中国工程物理研究院材料研究所 | A kind of preparation method of metal reinforced uranium dioxide fuel ball |
| CN109903868A (en) * | 2019-01-02 | 2019-06-18 | 中国原子能科学研究院 | A kind of preparation method of UC fuel pellet |
| CN110156475A (en) * | 2019-07-02 | 2019-08-23 | 中国原子能科学研究院 | A kind of microwave synthesis method of uranium carbonitride zirconium powder |
| CN110415845A (en) * | 2019-08-06 | 2019-11-05 | 中国核动力研究设计院 | A kind of high uranium density hybrid fuel pellet and preparation method thereof |
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- 2019-12-20 CN CN201911325486.5A patent/CN113012833A/en active Pending
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103466568A (en) * | 2013-09-09 | 2013-12-25 | 中国原子能科学研究院 | Preparation method of uranium nitride fuel powder and pellet |
| CN107256726A (en) * | 2017-07-03 | 2017-10-17 | 中国工程物理研究院材料研究所 | A kind of preparation method of metal reinforced uranium dioxide fuel ball |
| CN109903868A (en) * | 2019-01-02 | 2019-06-18 | 中国原子能科学研究院 | A kind of preparation method of UC fuel pellet |
| CN110156475A (en) * | 2019-07-02 | 2019-08-23 | 中国原子能科学研究院 | A kind of microwave synthesis method of uranium carbonitride zirconium powder |
| CN110415845A (en) * | 2019-08-06 | 2019-11-05 | 中国核动力研究设计院 | A kind of high uranium density hybrid fuel pellet and preparation method thereof |
Non-Patent Citations (1)
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| JAE HO YANG.ET: "UO2 -UN composites with enhanced uranium density and thermal conductivity", 《JOURNAL OF NUCLEAR MATERIALS》 * |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2023130356A1 (en) * | 2022-01-07 | 2023-07-13 | 岭澳核电有限公司 | High-uranium-density atf nuclear fuel pellet and preparation method therefor |
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