CN116173550A - Simplified system and method for separating and purifying uranium in irradiated nuclear fuel solution - Google Patents

Simplified system and method for separating and purifying uranium in irradiated nuclear fuel solution Download PDF

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CN116173550A
CN116173550A CN202211639704.4A CN202211639704A CN116173550A CN 116173550 A CN116173550 A CN 116173550A CN 202211639704 A CN202211639704 A CN 202211639704A CN 116173550 A CN116173550 A CN 116173550A
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uranium
plutonium
extraction
feed liquid
extractor
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杨素亮
郝轩
周今
柳倩
杨琪
朱礼洋
杨志红
田国新
兰友世
杨雅婷
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China Institute of Atomic of Energy
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China Institute of Atomic of Energy
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D11/00—Solvent extraction
    • B01D11/04—Solvent extraction of solutions which are liquid
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D11/00—Solvent extraction
    • 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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  • Extraction Or Liquid Replacement (AREA)
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Abstract

The invention discloses a simplified system and a method for separating and purifying uranium in an irradiated nuclear fuel solution, which are characterized in that the common extraction of uranium and plutonium is realized in a 1A extractor, a 1B+ extractor adopts feed liquid 1B+X with dual functions of reduction and complexation to wash uranium plutonium common extraction feed liquid 1AP extracted by the 1A extractor, 1B+S is adopted to carry out the supplementary extraction, a uranium-containing extract 1B+U obtained by the 1B+ extractor is reversely extracted by dilute nitric acid in a 1C extractor to obtain a water-phase uranium solution, the chemical yield of uranium is more than 99.9%, and a uranium product solution is obtained after uranium tail treatment; the method of the invention enhances the decontamination of other radionuclides in uranium-containing liquid flow by the co-decontamination separation cycle; the separation and purification of uranium in the nuclear fuel solution can be realized only by means of the co-decontamination separation cycle, so that a specific uranium purification cycle is omitted, and the process flow and the operation cost of the irradiation nuclear fuel aftertreatment are greatly simplified; by adding a 1BXX or 1B3X extractor, the uranium product solution can be further purified without affecting the separation and purification of other product elements.

Description

Simplified system and method for separating and purifying uranium in irradiated nuclear fuel solution
Technical Field
The invention belongs to the technical field of nuclear chemical industry and nuclear fuel circulation, and particularly relates to a simplified system and a method for separating and purifying uranium in a solvent extraction circulation reactor irradiation nuclear fuel solution.
Background
The nuclear fuel post-treatment is an essential step for realizing closed fuel circulation, and has very important influence on nuclear power economy and comprehensive utilization of nuclear energy. Nuclear fuel reprocessing is the extraction and purification of newly generated fissionable materials, and the recovery of virgin fissionable materials as well as unconverted conversion materials. In the prior art, an aqueous tributyl phosphate extraction process for separating uranium from plutonium by using the valence state change of the plutonium by taking an inert solvent such as hydrogenated kerosene, n-dodecane, hydrogenated tetrapropylene and the like as a diluent and tributyl phosphate (TBP) as an extractant is a feasible, economical and reliable nuclear fuel post-treatment process.
The main process products of the nuclear fuel post-treatment plant are uranium products and plutonium products. The process of extracting metal ions from an aqueous solution into an organic phase and back-extracting the metal ions into an aqueous phase under varying conditions is called an extraction cycle, which includes washing, stripping, and the like, and sometimes involves the adjustment of the valence of the metal ions. Referring to FIG. 1, the 1A, 1B and 1C extractors of a typical PUREX two-cycle scheme are co-decontamination separation cycles (or first cycle); the 2A and 2B extractors are plutonium purification cycles, the 2D and 2E are uranium purification cycles, and the plutonium purification cycle and the uranium purification cycle jointly form a second cycle. After the 1B extraction equipment, a plutonium barrier extraction equipment (1 BXX) is additionally arranged in part of post-treatment factories, a small amount of plutonium in 1BU is further reversely extracted to a water phase and then returned to the 1B equipment, so that on one hand, the chemical yield of the plutonium is ensured, and on the other hand, the decontamination of the plutonium and neptunium in the organic phase feed liquid is increased, and the pressure of uranium purification circulation on the decontamination of the plutonium and neptunium is reduced.
The radioactivity of uranium products is one of the most important technical indicators of nuclear fuel reprocessing plants, where the control requirements on the content of plutonium and neptunium contributing to alpha radiation are particularly stringent. According to the technical index requirement of the French UP3 nuclear fuel post-treatment plant, the alpha radioactive pollution of uranium in uranium products per gram is lower by 250Bq. The concentration of uranium in the final uranium product solution obtained by the extraction cycle is generally of the order of tens of grams per liter, with a uranium-plutonium ratio exceeding 1.0x10 according to the above-mentioned index requirements 9 The uranium neptunium ratio exceeds 1.0X10 7 The decontamination coefficient of the uranium product of the whole process to plutonium is up to 1.0x10 6 As above, the neptunium is also decontaminated to 1.0X10 4 The above. In a typical PUREX two-cycle process, uranium in a 1CU feed liquid from which plutonium, neptunium and split elements have been separated is purified again on the basis of a co-decontamination separation cycle to further remove the plutonium and neptunium, thereby obtaining a purer uranium product solution to meet the technical index requirements of the process. Under typical conditions, the decontamination coefficient of the co-decontaminating and separating recycled uranium product to plutonium is 10 4 On the order of magnitude, the decontamination coefficient for neptunium is 10 2 Magnitude, while the decontamination coefficient of uranium purification cycle for both plutonium and neptunium is at or near 10 2 Magnitude. In a typical PUREX two-cycle process, a 2D extraction apparatus is used to extract uranium from a 2DF feed obtained by seasoning (evaporation concentration, acid adjustment and valence adjustment) of a 1CU feed and to wash the impurity elements therein, and a 2E extraction apparatus is used as a stripping tank for uranium to transfer uranium to an aqueous phase with dilute nitric acid at a higher temperature. To further enhance the decontamination of plutonium and neptunium in uranium products, there is a lack of combustionThe post-treatment plant also requires the addition of three cycles of uranium. Overall, the uranium purification process is extremely complex even with the PUREX two-cycle process.
Disclosure of Invention
Aiming at the technical problems existing in the prior art, the invention aims to provide a system and a method for simplifying the process of post-treatment of spent fuel PUREX, reducing the running cost of a post-treatment plant and effectively separating and purifying uranium from nitric acid solution of irradiated nuclear fuel.
In order to achieve the above purpose, the invention adopts the following technical scheme: a simplified system for separating and purifying uranium in irradiated nuclear fuel solution consists of a single-cycle co-extraction unit, a uranium-plutonium separation unit and a uranium back-extraction unit.
Further, the uranium-plutonium separation unit is a 1b+ extraction system; the 1B+ extraction system may be composed of only a single 1B+ extractor, may also include 1B and 1BXX extractors, or may be composed of 1B, 1BXX and 1B3X extractors together.
The invention also provides a method for simplifying separation and purification of uranium in the irradiated nuclear fuel solution, which comprises the steps of carrying out complex reduction back extraction and impurity washing on plutonium in an organic phase 1AP feed liquid of a co-extraction unit by using 1B+X feed liquid with double functions of reduction and complexation in 1B+ extraction equipment, and carrying out supplementary extraction on uranium in an aqueous phase by using an organic solvent 1B+S to obtain a uranium-containing organic phase 1B+U and a plutonium-containing back extraction aqueous phase 1B+P, wherein the uranium-plutonium is separated; the plutonium-containing water phase 1B+P enters a plutonium purification cycle after being regulated; and carrying out uranium stripping in the uranium-containing organic phase 1B+U-stripping unit 1C extractor to obtain a high-purity aqueous uranium solution.
Further, the feed liquid 1B+X with double functions of reduction and complexation is nitric acid solution of one or more of glutarimide dioxime, succinimidyl dioxime, hydroxyurea, glyoxime acid and methyl glyoxime acid and hydroxylamine nitrate; the solution can also be nitric acid solution of other feed liquid with double functions of reduction and complexation and hydroxylamine nitrate.
Further, the feed liquid 1B+X with double functions of reduction and complexation is nitric acid solution of one or more of glutarimide dioxime, succinimidyl dioxime, hydroxyurea, glyoxime acid and methyl glyoxime acid and hydrazine nitrate; the solution can also be nitric acid solution of other feed liquid with double functions of reduction and complexation and hydrazine nitrate.
Further, adding the nitric acid solution 1AF, TBP-kerosene solution 1AX and nitric acid solution 1AS of spent fuel into a 1A extractor for extraction to obtain uranium-plutonium co-extracted organic phase feed liquid 1AP.
Further, the flow ratio of each feed liquid in the 1B+ extraction equipment is in the range of 1AP:1B+S:1B+X=1.0:0.05-0.5:0.05-0.5.
Further, in the 1B extraction equipment, reducing the plutonium in the +4 valence state in the 1AP feed liquid of the co-extraction unit to +3 valence state by using 1BX feed liquid with a reduction effect, thereby back-extracting the plutonium to the water phase, and carrying out supplementary extraction on uranium in the back-extracted water phase by using 1BS to obtain uranium-containing extracted organic phase 1BU and plutonium-containing water phase 1BP separated from uranium and plutonium; the plutonium-containing water phase 1BP enters a plutonium purification cycle after being regulated; washing and supplementing impurities in uranium-containing organic phase in the extraction liquid 1BU, feed liquid 1BXXX with double functions of reduction and complexation and organic solvent 1BXXS in a 1BXX extractor to obtain an extraction liquid organic phase 1BXXU; and carrying out uranium back extraction on the extract liquid 1BXXU in a back extraction unit 1C extractor to obtain a high-purity aqueous uranium solution.
Further, in the 1B extraction equipment, reducing the plutonium in the +4 valence state in the organic phase 1AP feed liquid of the co-extraction unit to +3 valence state by using 1BX feed liquid with a reduction effect, thereby stripping the plutonium to an aqueous phase, and carrying out supplementary extraction on uranium in the stripped aqueous phase by using 1BS to obtain uranium-containing organic phase 1BU and plutonium-containing aqueous phase 1BP separated by uranium and plutonium; the plutonium-containing water phase 1BP enters a plutonium purification cycle after being regulated; in 1BXX extraction equipment, washing and purifying uranium-containing organic phase 1BU by feed liquid 1BXXX with double functions of reduction and complexation, and carrying out supplementary extraction by organic solvent 1BXXS to obtain extracted organic phase feed liquid 1BXXU; adding the extracted organic phase feed liquid 1BXXU into a 1B3X extractor, washing again by using a water phase detergent 1B3XX, and performing supplementary extraction by using an organic solvent 1B3XS to obtain an extracted organic phase feed liquid 1B3XU; and adding the extract liquid 1B3XU into a 1C extractor for back extraction to obtain a high-purity aqueous phase uranium solution of a uranium product solution with very low content of neptunium.
The technical scheme of the invention has the beneficial effects that the system and the method for simplifying the separation and purification of uranium in the irradiated nuclear fuel solution are adopted, and the system comprises a co-extraction unit, a uranium-plutonium separation unit and a uranium back-extraction unit; the method comprises the steps of (1) enabling feed liquid with dual functions of reduction and complexation to act on an extract 1AP extracted by a 1A extractor to obtain uranium and plutonium separated extracts 1B+U and 1B+P, separating by a 1B+ extractor system to obtain extract 1B+U, and back extracting in a 1C extractor to obtain aqueous phase uranium solution with low plutonium and neptunium content; the chemical recovery rate of uranium in the whole process is more than 99.9% after the 1BS is used for supplementary extraction. The system and the method of the invention realize the separation and purification of uranium in the irradiated nuclear fuel solution and the preliminary separation of plutonium and neptunium through only one extraction cycle; the enhanced co-decontamination separation single circulation system of the invention is adopted to recycle the decontamination of plutonium and neptunium in uranium-containing liquid stream, including 1B organic phase liquid stream 1 BU; the separation and purification of uranium in the nuclear fuel solution are realized through single circulation only by virtue of the co-decontamination separation circulation, so that the process flow of the irradiation nuclear fuel aftertreatment is greatly simplified, and the uranium separation and purification cost is reduced; by adding a 1BXX or 1B3X extractor and prolonging a single circulation system, the uranium solution can be further purified without affecting the separation and purification of other elements in the plutonium line.
Drawings
FIG. 1 is a schematic diagram of a typical prior art PUREX two-cycle flow scheme;
FIG. 2 is a schematic diagram of a simplified separation and purification of uranium in irradiated nuclear fuel solution according to a first embodiment of the present invention;
fig. 3 is a schematic diagram of uranium in a simplified separation and purification irradiated nuclear fuel solution according to a second embodiment of the present invention.
Detailed Description
The present invention will be described in detail with reference to the accompanying drawings and examples.
Example 1
The embodiment of the invention provides a system for simplifying separation and purification of uranium in irradiated nuclear fuel solution, which consists of a single-cycle co-extraction unit, a uranium-plutonium separation unit and a uranium back-extraction unit.
Preferably, the co-extraction unit is a 1A extraction apparatus; the back extraction unit is 1C extraction equipment.
Preferably, the uranium-plutonium separation unit is a single 1b+ extraction device, a combination of 1B and 1BXX extraction devices or a combination of 1B, 1BXX, 1B3X extraction devices.
Referring to fig. 2, the embodiment of the invention also provides a method for simplifying separation and purification of uranium in the irradiated nuclear fuel solution, in a 1b+ extraction device, using feed liquid 1b+x with dual functions of reduction and complexation, back-extracting and washing an organic phase 1AP feed liquid obtained by the back-extracting 1A extraction device, and carrying out supplementary extraction of uranium by an organic solvent 1b+s to obtain uranium-plutonium separated organic phase 1b+u feed liquid and aqueous phase 1b+p feed liquid; the water phase 1B+P feed liquid enters plutonium purification circulation after being regulated; and transferring uranium to a water phase by back extraction of a back extractant 1CX in 1C extraction equipment by using the organic phase 1B+U feed liquid to obtain a high-purity water phase uranium product solution.
Preferably, the feed liquid 1B+X with dual functions of reduction and complexation is nitric acid solution of one or more of glutarimide dioxime, succinimidyl dioxime, hydroxyurea, glyoxime acid and methyl hydroxamic acid and hydroxylamine nitrate; or other feed liquid with double functions of reduction and complexation and nitric acid solution of hydroxylamine.
Preferably, the feed liquid 1B+X with dual functions of reduction and complexation is nitric acid solution of one or more of glutarimide dioxime, succinimidyl dioxime, hydroxyurea, glyoxime acid and methyl glyoxime acid and hydrazine nitrate; or other feed liquid with double functions of reduction and complexation and nitric acid solution with hydrazine.
Preferably, the nitric acid solution 1AF, TBP-kerosene solution 1AX and nitric acid solution 1AS of spent fuel are added into a 1A extractor to be extracted to obtain uranium and plutonium extraction organic phase feed liquid 1AP.
Preferably, the 1AX is 30% TBP-kerosene (v/v, volume percent), and the 1AS is 3.0mol/L nitric acid solution; the 1CX is 0.01mol/L nitric acid solution.
Preferably, the organic solvent 1b+s is 30% tbp-kerosene.
Preferably, the back extraction temperature in the 1C extraction equipment is 50+/-5 ℃.
Preferably, the feed flow ratio in the 1b+ extraction device is 1ap:1b+s:1b+x=1.0:0.1:0.05.
Example two
Referring to fig. 3, the system and method according to the first embodiment of the present invention are adopted to simplify the separation and purification of uranium in the irradiated nuclear fuel solution, and the nitric acid solution 1AF, TBP-kerosene solution 1AX and nitric acid solution 1AS of spent fuel are added into a 1A extractor; adding the extract 1AP extracted by the 1A extractor, the feed liquid 1BX with reduction effect and the organic solvent 1BS into 1B extraction equipment for extraction to obtain organic phase 1BU feed liquid and aqueous phase 1BP feed liquid separated from uranium and plutonium; the water phase 1BP feed liquid enters plutonium purification circulation after being regulated; washing the 1BU feed liquid by feed liquid 1BXXX with double functions of reduction and complexation in 1BXX extraction equipment, and carrying out complementary extraction by an organic solvent 1BXXS to obtain an extracted organic phase 1BXXU feed liquid; and adding the extracted organic phase feed liquid 1BXXU and the stripping agent 1CX into a 1C extractor for back extraction to obtain a high-purity aqueous phase uranium product solution.
Preferably, 1AF contains 410g/L uranium, 4.0g/L plutonium and 0.5g/L neptunium, the nitric acid concentration is 3.0mol/L,1AX is 30% TBP-hydrogenated kerosene, 1AS is 1.0mol/L nitric acid, and the ratio of each material flow to 1AF:1AX:1AS is 1.0:4.75:0.75.
Preferably, 1BS is 30% TBP-hydrogenated kerosene, 1BX is 0.2mol/L hydroxylamine nitrate-0.15 mol/L hydrazine-1.5 mol/L nitric acid solution, and the flow ratio 1AP:1BX:1BS is 10.0:1.0:1.5.
Preferably, 1BXXS is 30% TBP-hydrogenated kerosene, 1BXXX is 0.4mol/L glutarimide dioxime-0.3 mol/L hydroxylamine nitrate-0.7 mol/L nitric acid, and the flow ratio is 1BU to 1BXXX to 1BXXS is 1.0:0.1.0.12.
Preferably, the 1CX is 0.01mol/L nitric acid, the flow ratio 1BXXU to 1CX is 1.0:1.25, and the stripping temperature is 55+ -5 ℃.
The recovery rate of uranium after separation and purification by the method is more than 99.9%, the activity of plutonium contained in each gram of uranium in uranium product solution is 37.0+/-3.0 Bq, and the activity of neptunium contained in uranium product solution is 67.0+/-4.0 Bq. Wherein the total amount of alpha nuclides contained in each gram of uranium except uranium is about 104.0Bq.
It will be apparent to those skilled in the art that various modifications and variations can be made to the present invention without departing from the spirit or scope of the invention. Thus, it is intended that the present invention also include such modifications and alterations insofar as they come within the scope of the appended claims or the equivalents thereof.

Claims (7)

1. A simplified system for separating and purifying uranium in irradiated nuclear fuel solution is characterized in that: consists of a single-cycle co-extraction unit, a uranium-plutonium separation unit and a uranium back-extraction unit.
2. The simplified system for separating and purifying uranium in irradiated nuclear fuel solution according to claim 1, wherein: the uranium-plutonium separation unit is a 1B+ extraction system; the 1B+ extraction system is one of single 1B+ extraction equipment, 1B and 1BXX combined extraction equipment or 1B, 1BXX and 1B3X combined extraction equipment.
3. The simplified method for separating and purifying uranium in irradiated nuclear fuel solution according to claim 1, wherein: in a 1B+ extraction device of a uranium-plutonium separation unit, carrying out complex reduction back extraction and impurity washing on plutonium in an organic phase 1AP feed liquid of the co-extraction unit by using 1B+X feed liquid with double functions of reduction and complexation, and carrying out supplementary extraction on uranium in an aqueous phase by using an organic solvent 1B+S to obtain uranium-containing organic phase 1B+U and plutonium-containing back extraction aqueous phase 1B+P separated by uranium-plutonium; the plutonium-containing water phase 1B+P enters a plutonium purification cycle after being regulated; and carrying out uranium stripping in the uranium-containing organic phase 1B+U-stripping unit 1C extractor to obtain a high-purity aqueous uranium solution.
4. The method for separating and purifying uranium in irradiated nuclear fuel solution by using a system according to claim 1, wherein the method is characterized by comprising the following steps: in 1B extraction equipment of a uranium-plutonium separation unit, reducing plutonium in a +4 valence state in an organic phase 1AP feed liquid of the co-extraction unit to a +3 valence state by using 1BX feed liquid with a reduction effect, thereby stripping the plutonium to an aqueous phase, and carrying out supplementary extraction on uranium in a stripping aqueous phase by using 1BS to obtain uranium-containing extracted organic phase 1BU and plutonium-containing aqueous phase 1BP separated by uranium-plutonium; the plutonium-containing aqueous phase liquid 1BP enters a plutonium purification cycle after being regulated; the extract 1BU, the feed liquid 1BXXX with double functions of reduction and complexation and the organic solvent 1BXXS are subjected to washing and complementary extraction of impurities in uranium-containing organic phase in a 1BXX extractor to obtain an extracted organic phase 1BXXU; and carrying out uranium back extraction on the extract liquid 1BXXU in a back extraction unit 1C extractor to obtain a high-purity aqueous uranium solution.
5. The method for separating and purifying uranium in irradiated nuclear fuel solution by using a system according to claim 1, wherein the method is characterized by comprising the following steps: in 1B extraction equipment of a uranium-plutonium separation unit, reducing plutonium in a +4 valence state in an organic phase 1AP feed liquid of the co-extraction unit to a +3 valence state by using 1BX feed liquid with a reduction effect, thereby stripping the plutonium to an aqueous phase, and carrying out supplementary extraction on uranium in a stripping aqueous phase by using 1BS to obtain uranium-containing organic phase 1BU and plutonium-containing aqueous phase 1BP separated by uranium-plutonium; the plutonium-containing water phase 1BP enters a plutonium purification cycle after being regulated; the uranium-containing organic phase 1BU feed liquid is subjected to washing purification by feed liquid 1BXXX with double functions of reduction and complexation in 1BXX extraction equipment, and is subjected to supplementary extraction by an organic solvent 1BXXS to obtain extracted organic phase feed liquid 1BXXU; adding the extracted organic phase feed liquid 1BXXU into a 1B3X extractor, washing again by using a water phase detergent 1B3XX, and performing supplementary extraction by using an organic solvent 1B3XS to obtain an extracted organic phase feed liquid 1B3XU; and adding the extract liquid 1B3XU into a 1C extractor for back extraction to obtain the aqueous uranium solution with low neptunium content.
6. The method for separating and purifying uranium in irradiated nuclear fuel solution according to any one of claims 3 to 5, wherein: the feed liquid 1B+X and 1BXXX with double functions of reduction and complexation are mixed nitric acid solution of hydrazine nitrate and one or more of glutarimide dioxime, succinimidyl dioxime, glyoxime acid, methyl hydroxamic acid and hydroxyurea.
7. The method for separating and purifying uranium in irradiated nuclear fuel solution according to any one of claims 3 to 5, wherein: the 1B3XX is aqueous phase feed liquid or nitric acid solution of sodium nitrite with double functions of reduction and complexation.
CN202211639704.4A 2022-12-20 2022-12-20 Simplified system and method for separating and purifying uranium in irradiated nuclear fuel solution Pending CN116173550A (en)

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