RU2183867C2 - Method for recovering metal alloy of plutonium to produce composite uranium-plutonium oxide fuel - Google Patents
Method for recovering metal alloy of plutonium to produce composite uranium-plutonium oxide fuel Download PDFInfo
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- RU2183867C2 RU2183867C2 RU2000121276/06A RU2000121276A RU2183867C2 RU 2183867 C2 RU2183867 C2 RU 2183867C2 RU 2000121276/06 A RU2000121276/06 A RU 2000121276/06A RU 2000121276 A RU2000121276 A RU 2000121276A RU 2183867 C2 RU2183867 C2 RU 2183867C2
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- plutonium
- melt
- alloy
- uranium
- mixed
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- 229910052778 Plutonium Inorganic materials 0.000 title claims abstract description 9
- 239000000446 fuel Substances 0.000 title claims abstract description 9
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 title claims abstract description 9
- 229910001092 metal group alloy Inorganic materials 0.000 title claims abstract description 5
- 238000000034 method Methods 0.000 title claims description 6
- PSPBAKLTRUOTFX-UHFFFAOYSA-N [O-2].[Pu+4].[U+6].[O-2].[O-2].[O-2].[O-2] Chemical compound [O-2].[Pu+4].[U+6].[O-2].[O-2].[O-2].[O-2] PSPBAKLTRUOTFX-UHFFFAOYSA-N 0.000 title abstract 2
- 239000002131 composite material Substances 0.000 title abstract 2
- 229910045601 alloy Inorganic materials 0.000 claims abstract description 20
- 239000000956 alloy Substances 0.000 claims abstract description 20
- 238000004090 dissolution Methods 0.000 claims abstract description 13
- 239000000460 chlorine Substances 0.000 claims abstract description 12
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052801 chlorine Inorganic materials 0.000 claims abstract description 7
- 150000003839 salts Chemical class 0.000 claims abstract description 7
- 229910052770 Uranium Inorganic materials 0.000 claims abstract description 4
- 229910001514 alkali metal chloride Inorganic materials 0.000 claims abstract description 4
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 4
- 239000000203 mixture Substances 0.000 claims abstract description 4
- 238000003756 stirring Methods 0.000 claims abstract description 4
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims abstract description 4
- 125000005289 uranyl group Chemical group 0.000 claims abstract description 4
- FLDALJIYKQCYHH-UHFFFAOYSA-N plutonium(iv) oxide Chemical class [O-2].[O-2].[Pu+4] FLDALJIYKQCYHH-UHFFFAOYSA-N 0.000 claims abstract 2
- 239000000155 melt Substances 0.000 claims description 16
- 238000012545 processing Methods 0.000 claims description 4
- 239000008187 granular material Substances 0.000 claims description 3
- WJWSFWHDKPKKES-UHFFFAOYSA-N plutonium uranium Chemical compound [U].[Pu] WJWSFWHDKPKKES-UHFFFAOYSA-N 0.000 claims description 2
- 230000001376 precipitating effect Effects 0.000 claims 1
- 238000006243 chemical reaction Methods 0.000 abstract description 7
- 229910001066 Pu alloy Inorganic materials 0.000 abstract description 2
- 239000004615 ingredient Substances 0.000 abstract 1
- 239000000126 substance Substances 0.000 abstract 1
- 238000002156 mixing Methods 0.000 description 4
- OOAWCECZEHPMBX-UHFFFAOYSA-N oxygen(2-);uranium(4+) Chemical compound [O-2].[O-2].[U+4] OOAWCECZEHPMBX-UHFFFAOYSA-N 0.000 description 4
- FCTBKIHDJGHPPO-UHFFFAOYSA-N uranium dioxide Inorganic materials O=[U]=O FCTBKIHDJGHPPO-UHFFFAOYSA-N 0.000 description 4
- 238000011068 loading method Methods 0.000 description 3
- 239000002244 precipitate Substances 0.000 description 3
- 230000005587 bubbling Effects 0.000 description 2
- 239000003758 nuclear fuel Substances 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 229910000561 Plutonium–gallium alloy Inorganic materials 0.000 description 1
- QNJPYBOCFFOTGM-UHFFFAOYSA-J [Cl-].[Cl-].[Cl-].[Cl-].[Pu+4] Chemical class [Cl-].[Cl-].[Cl-].[Cl-].[Pu+4] QNJPYBOCFFOTGM-UHFFFAOYSA-J 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 150000001805 chlorine compounds Chemical class 0.000 description 1
- XOYLJNJLGBYDTH-UHFFFAOYSA-M chlorogallium Chemical compound [Ga]Cl XOYLJNJLGBYDTH-UHFFFAOYSA-M 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000004070 electrodeposition Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000012958 reprocessing Methods 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000000859 sublimation Methods 0.000 description 1
- 230000008022 sublimation Effects 0.000 description 1
- 239000002699 waste material Substances 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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- Electrolytic Production Of Metals (AREA)
Abstract
Description
Изобретение относится к области атомной энергетики и может быть использовано при конверсии оружейного плутония в МОКС - топливо. The invention relates to the field of nuclear energy and can be used in the conversion of weapons-grade plutonium to MOX fuel.
Известен способ переработки металлического сплава плутония в смешанное оксидное уран-плутониевое (МОКС)-топливо /Porodnov P. Т., Qsipenko A.G., Skiba O. V. et al. A pyrochemical procedure for the conversion of military origin metallic plutonium into MOX fuel. // Proceeding of international conference on evaluation of emerging nuclear fuel cycle systems. Global 95, September 11-14, 1995, Versailles, France, p. 1346-1351/, включающий операции растворения компонентов сплава в расплаве смеси хлоридов щелочных металлов и уранила при барботаже расплава хлором; осаждения смешанных оксидов электролизом расплава и отделения солей от гранулята смешанных оксидов урана и плутония. A known method of processing a metal alloy of plutonium into a mixed oxide of uranium-plutonium (MOX) fuel / Porodnov P. T., Qsipenko A.G., Skiba O. V. et al. A pyrochemical procedure for the conversion of military origin metallic plutonium into MOX fuel. // Proceeding of international conference on evaluation of emerging nuclear fuel cycle systems. Global 95, September 11-14, 1995, Versailles, France, p. 1346-1351 /, including the operation of dissolving the components of the alloy in the melt of a mixture of alkali metal chlorides and uranyl while sparging the melt with chlorine; deposition of mixed oxides by melt electrolysis and separation of salts from the granulate of mixed oxides of uranium and plutonium.
Недостатком этого способа является то, что при его осуществлении скорость растворения сплава очень низка, что приводит к усиленному износу оборудования. The disadvantage of this method is that during its implementation, the dissolution rate of the alloy is very low, which leads to increased wear of the equipment.
Задачей настоящего изобретения является увеличение скорости растворения сплава. The objective of the present invention is to increase the dissolution rate of the alloy.
Она достигается тем, что по способу переработки металлического сплава плутония в МОКС топливо, включающему растворение компонентов топлива, осаждение электролизом и отделение солей от гранулята, растворение ведут при перемешивании расплава со скоростью от 0,8 до 10 см/с. При этом скорость растворения сплава увеличивается. It is achieved by the fact that according to the method of processing a plutonium metal alloy into MOX fuel, including the dissolution of fuel components, precipitation by electrolysis and separation of salts from granulate, the dissolution is carried out with stirring of the melt at a speed of from 0.8 to 10 cm / s. In this case, the dissolution rate of the alloy increases.
При растворении сплава в расплаве смеси хлоридов щелочных металлов и уранила при барботаже расплава хлором происходят следующие реакции:
3UO2Cl2+2Pu(тв.)=3UO2(тв.)+2PuCl3 (1)
UO2(тв.)+2Cl2(газ)=UO2Cl2 (2)
UO2Cl2+2С(конструкционный)+Cl2(газ)=UCl4+2CO2(газ) (3)
Pu3++Cl2(газ)=PuCl4 (4)
3PuCl4+Ga(тв.)=3PuCl3+GaCl3 (5)
В результате реакции (1) сплав покрывается слоем диоксида урана и дальнейшая скорость растворения сплава определяется скоростью реакций (2) и (3), причем диоксид урана представляет собой компактный осадок.When the alloy is dissolved in a melt of a mixture of alkali metal chlorides and uranyl, the following reactions occur during bubbling of the melt with chlorine:
3UO 2 Cl 2 + 2Pu (tv) = 3UO 2 (tv) + 2PuCl 3 (1)
UO 2 (tv) + 2Cl 2 (gas) = UO 2 Cl 2 (2)
UO 2 Cl 2 + 2C (structural) + Cl 2 (gas) = UCl 4 + 2CO 2 (gas) (3)
Pu 3+ + Cl 2 (gas) = PuCl 4 (4)
3PuCl 4 + Ga (solid) = 3PuCl 3 + GaCl 3 (5)
As a result of reaction (1), the alloy is covered with a layer of uranium dioxide and the further dissolution rate of the alloy is determined by the rate of reactions (2) and (3), and uranium dioxide is a compact precipitate.
При перемешивании расплава осадок диоксида урана удаляется в объем расплава в виде порошка с большой величиной площади поверхности и поверхность сплава не пассивируется. Таким образом, одновременно идут реакции (1) - (5), что увеличивает скорость растворения сплава. When the melt is mixed, the uranium dioxide precipitate is removed into the melt volume in the form of a powder with a large surface area and the alloy surface is not passivated. Thus, reactions (1) - (5) simultaneously occur, which increases the dissolution rate of the alloy.
При этом перемешивание необходимо вести со скоростью от 0,8 до 10 см/с. Это связано с тем, что при перемешивании расплава со скоростью до 0,8 см/с поверхность сплава зарастает осадком диоксида урана и скорость растворения сплава снижается. При скорости перемешивания более 10 см/с часть поверхности сплава оказывается не покрытой расплавом, что приводит к возгоранию сплава при непосредственном контакте с газообразным хлором и выбросу хлоридов плутония в ловушку возгонов. При этом возрастают потери плутония. In this case, mixing must be carried out at a speed of from 0.8 to 10 cm / s. This is due to the fact that when the melt is stirred at a speed of up to 0.8 cm / s, the surface of the alloy is overgrown with a precipitate of uranium dioxide and the dissolution rate of the alloy decreases. At a mixing speed of more than 10 cm / s, part of the surface of the alloy is not covered by the melt, which leads to the ignition of the alloy in direct contact with gaseous chlorine and the release of plutonium chlorides into the sublimation trap. At the same time, plutonium losses increase.
Таким образом, для увеличения скорости растворения сплава проводят перемешивание расплава со скоростью от 0,8 до 10 см/с. Thus, to increase the dissolution rate of the alloy, melt is mixed at a speed of 0.8 to 10 cm / s.
Изобретение иллюстрируется следующими примерами. The invention is illustrated by the following examples.
Провели 5 экспериментов по переработке плутоний-галлиевого сплава. Использовали хлоратор - электолизер /Skiba O.V., Savochkin. Yu, P., Porodnov P. T. et al. Technology of pyrochemical reprocessing and production of nuclear fuel// Proceedings of international conference on future nuclear systems: emerging fuel cycles and waste disposal options. Global 93, September 12-17, 1993, Seattle, USA, p.1344-1350/ с устройствами для подачи хлора, перемешивания расплава-загрузки сплава, электроосаждения, измерения температуры, потенциала катода, конденсации летучих хлоридов, отбора проб расплава. Масса загрузки солей в пирографитовый тигель составляла 90 кг. Плутониевый сплав (5,4 кг) загружали в хлоратор - электролизер после плавления солей и достижения рабочей температуры 720oC. Начальная концентрация урана в расплаве составляла 20%. Растворение сплава проводили барботажем хлора через расплав и с/без перемешивания расплава в устройстве перемешивания расплава-загрузки сплава. Солевые пробы передавали на радиометрический анализ по Pu.Conducted 5 experiments on the processing of plutonium-gallium alloy. Used a chlorinator - electrolyzer / Skiba OV, Savochkin. Yu, P., Porodnov PT et al. Technology of pyrochemical reprocessing and production of nuclear fuel // Proceedings of international conference on future nuclear systems: emerging fuel cycles and waste disposal options. Global 93, September 12-17, 1993, Seattle, USA, p.1344-1350 / with devices for supplying chlorine, mixing the melt-loading alloy, electrodeposition, measuring temperature, cathode potential, condensation of volatile chlorides, sampling melt. The mass of loading of salts into the pyrographite crucible was 90 kg. Plutonium alloy (5.4 kg) was loaded into a chlorinator-electrolyzer after melting the salts and reaching a working temperature of 720 o C. The initial concentration of uranium in the melt was 20%. The dissolution of the alloy was carried out by bubbling of chlorine through the melt and with / without stirring the melt in the device for mixing the melt-loading alloy. Salt samples were transferred for Pu radiometric analysis.
Параметры и результаты даны в таблице. Результаты, приведенные в таблице, показывают, что увеличение скорости растворения сплава происходит при использовании изобретения. Parameters and results are given in the table. The results shown in the table show that an increase in the dissolution rate of the alloy occurs when using the invention.
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Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| RU2000121276/06A RU2183867C2 (en) | 2000-08-09 | 2000-08-09 | Method for recovering metal alloy of plutonium to produce composite uranium-plutonium oxide fuel |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| RU2000121276/06A RU2183867C2 (en) | 2000-08-09 | 2000-08-09 | Method for recovering metal alloy of plutonium to produce composite uranium-plutonium oxide fuel |
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| Publication Number | Publication Date |
|---|---|
| RU2183867C2 true RU2183867C2 (en) | 2002-06-20 |
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| RU2000121276/06A RU2183867C2 (en) | 2000-08-09 | 2000-08-09 | Method for recovering metal alloy of plutonium to produce composite uranium-plutonium oxide fuel |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2004079097A1 (en) * | 2003-03-07 | 2004-09-16 | Valery Fedorovich Mityakin | Coating (variants), method for producing said coating and a mixer for producing a coating mixture |
| RU2238600C2 (en) * | 2002-08-19 | 2004-10-20 | Государственное унитарное предприятие "Всероссийский научно-исследовательский институт химической технологии" | Method for nonaqueous dissolution of uranium and uranium-containing materials |
| RU2450373C2 (en) * | 2008-07-10 | 2012-05-10 | Сергей Павлович Распопин | Method of nuclear fuel synthesis for power fast neutron reactors with reactor core from molten salt |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB1349982A (en) * | 1971-01-18 | 1974-04-10 | Atomic Energy Authority Uk | Preparation of solutions of mixed uranium and plutonium nitrates |
| DE3837572A1 (en) * | 1987-11-05 | 1989-05-18 | Us Energy | METHOD FOR ELECTROFFINATING AND DEVICE FOR RECOVERING URANE AND MIXING OF URANIUM AND PLUTONIUM FROM CONSUMED FUELS |
| RU2079909C1 (en) * | 1994-09-27 | 1997-05-20 | Научно-исследовательский и конструкторский институт энерготехники | Method of nuclear fuel pyrochemical regeneration |
| RU2131477C1 (en) * | 1998-03-16 | 1999-06-10 | Сибирский химический комбинат | Method of processing armament plutonium |
| US5932930A (en) * | 1994-06-28 | 1999-08-03 | General Electric Company | Method for fabricating mixed oxide fuel |
-
2000
- 2000-08-09 RU RU2000121276/06A patent/RU2183867C2/en not_active IP Right Cessation
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB1349982A (en) * | 1971-01-18 | 1974-04-10 | Atomic Energy Authority Uk | Preparation of solutions of mixed uranium and plutonium nitrates |
| DE3837572A1 (en) * | 1987-11-05 | 1989-05-18 | Us Energy | METHOD FOR ELECTROFFINATING AND DEVICE FOR RECOVERING URANE AND MIXING OF URANIUM AND PLUTONIUM FROM CONSUMED FUELS |
| US5932930A (en) * | 1994-06-28 | 1999-08-03 | General Electric Company | Method for fabricating mixed oxide fuel |
| RU2079909C1 (en) * | 1994-09-27 | 1997-05-20 | Научно-исследовательский и конструкторский институт энерготехники | Method of nuclear fuel pyrochemical regeneration |
| RU2131477C1 (en) * | 1998-03-16 | 1999-06-10 | Сибирский химический комбинат | Method of processing armament plutonium |
Non-Patent Citations (1)
| Title |
|---|
| RORODNOV P.T. etc. A pycochemical procedure for the conversion of military metallic plutonium into MOX fuel. Proceedings of international conference on evaluation of emerging nuclear fuel cycle systemc. Global 95. Versailles, France, September 11-14, 1995, р.1346-1351. * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| RU2238600C2 (en) * | 2002-08-19 | 2004-10-20 | Государственное унитарное предприятие "Всероссийский научно-исследовательский институт химической технологии" | Method for nonaqueous dissolution of uranium and uranium-containing materials |
| WO2004079097A1 (en) * | 2003-03-07 | 2004-09-16 | Valery Fedorovich Mityakin | Coating (variants), method for producing said coating and a mixer for producing a coating mixture |
| RU2450373C2 (en) * | 2008-07-10 | 2012-05-10 | Сергей Павлович Распопин | Method of nuclear fuel synthesis for power fast neutron reactors with reactor core from molten salt |
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Effective date: 20110810 |