CN103451455A - Uranium (U) and plutonium (Pu) separation technology in Purex process - Google Patents

Uranium (U) and plutonium (Pu) separation technology in Purex process Download PDF

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CN103451455A
CN103451455A CN2012101668726A CN201210166872A CN103451455A CN 103451455 A CN103451455 A CN 103451455A CN 2012101668726 A CN2012101668726 A CN 2012101668726A CN 201210166872 A CN201210166872 A CN 201210166872A CN 103451455 A CN103451455 A CN 103451455A
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plutonium
uranium
flow process
purex
separation technology
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CN103451455B (en
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肖松涛
刘协春
罗方祥
杨贺
兰天
孟照凯
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China Institute of Atomic of Energy
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China Institute of Atomic of Energy
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Abstract

The invention belongs to the technical field of nuclear fuel postprocessing, and discloses a uranium (U) and plutonium (Pu) separation technology in a Purex process. According to the uranium and plutonium separation technology, Pu (IV) in 1BF material flow is reduced to Pu (III) in 1B tank by use of reducing agent 1BX and supplement extractant 1BS to enable plutonium to get into an aqueous phase and uranium to be retained in an organic phase, and uranium and plutonium separation is realized. The reducing agent 1BX which is used comprises 0.1-0.2 mol/L of formaldoxime, 0.35-0.5 mol/L of NO<3-> and 0.35-0.5 mol/L of H<+>; the flow ratio of 1BF:1BX is 1-4, and the flow ratio of 1BF:1BS is 4-6. The uranium and plutonium separation technology has the characteristics that the plutonium recovery rate is high, and the purification coefficients of removal of plutonium from uranium and removal of uranium from plutonium are large.

Description

Uranium, plutonium separating technology in the Purex flow process
Technical field
The invention belongs to the nuclear fuel reprocessing technical field, be specifically related to uranium in the Purex flow process, plutonium separating technology.
Background technology
The separation of uranium, plutonium is the important process in the Purex flow process, its main task is to wash uranium-bearing after technique is removed technetium and the organic phase feed liquid of plutonium through codecontamination cycle purification and technetium, with reductive agent, Pu (IV) is reverted to the extremely difficult Pu (III) be extracted, make plutonium enter water and uranium is retained in organic phase, realize the separation of uranium plutonium.Because organic chemical reagent has, speed of response is fast, selectivity good, do not introduce the characteristics such as salinity, destructible, at uranium, plutonium, in separating application, has carried out a large amount of research.N wherein, N-dimethyl hydroxylamine, N, N-ethyl-hydroxyethyl azanol, hydroxyurea, acetohydroximic acid etc. all can be used as reductive agent in separating, and obtain good effect at uranium, plutonium.But in the Purex flow process, material is generally nitric acid system, HNO 3the HNO that radiolysis produces 2can affect U/Pu separation factor, Pu df and Pu yield in U/Pu separation factor and Pu purification cycle in the codecontamination partitioning cycle, so need to add holding reductant with removing nitrous acid while in technique, using above-mentioned reductive agent.N 2h 4, CH 3n 2h 3, (CH 3) 2n 2h 2deng being all the holding reductant with applications well prospect, N wherein 2h 4in industry, be used widely.But due to N 2h 4with HNO 2the hydrazoic acid that reaction produces may set off an explosion, so N 2h 4use be restricted, thereby limited the process modification of Purex flow process.
Abroad ethylidenehydroxylamine is studied, but its fast restore Pu (IV), and can remove nitrous acid simultaneously, no longer need extra holding reductant, but by its applied research, also manifest some problems, as Pu produced to interphase impurity during from the organic phase back extraction to water.
At the 32nd the 1st phase of volume " nuclear and radiochemistry " of the 44th the 2nd phase of volume " nuclear and radiochemistry " in 2010 disclosed " reduction kinetics of formoxime and Pu (IV) " and 2010 disclosed " formoxime and HNO 2dynamics of oxidation-reduction " in formoxime and Pu (IV) and HNO are disclosed respectively 2the reaction kinetics basic research, some processing condition have been obtained, but its disclosed processing condition also are not suitable for the actually operating technique that uranium, plutonium separate, do not provide its processing condition of practical application in uranium, plutonium separating technology in the Purex flow process in document.
Summary of the invention
(1) goal of the invention
According to problems of the prior art, the present invention proposes uranium in the Purex flow process, plutonium separating technology, this technology utilization formoxime is as reductive agent, and the plutonium rate of recovery is high, go in plutonium and plutonium to go the df of uranium large in uranium.
  
(2) technical scheme
In order to solve existing problem in prior art, the present invention is achieved by the following technical solutions:
Uranium, plutonium separating technology in the Purex flow process, this technique is to utilize reductive agent 1BX and supplementary extraction agent 1BS that the Pu in the 1BF feed liquid (IV) is reduced into to Pu (III), makes plutonium enter water and uranium is retained in organic phase, realizes the separation of uranium plutonium, key is, reductive agent used is formoxime.But this reductive agent fast restore Pu (IV), and can quick and HNO 2holding reductant during reaction can separate as the uranium plutonium simultaneously, without additional other reduction balustrade.
Described reductive agent 1BX consists of: the formoxime of 0.1 ~ 0.2mol/L, the NO of 0.35 ~ 0.5mol/L 3 -and the H of 0.35 ~ 0.5mol/L +; The stream ratio that the stream ratio of 1BF:1BX is 1 ~ 4,1BF:1BS is 4 ~ 6.
  
(3) beneficial effect
Uranium, plutonium separating technology in Purex flow process provided by the invention, practical application in uranium, plutonium separating technology first, the beneficial effect had is: (1) adopts formoxime as reductive agent, and this reductive agent complex ability and reducing power are strong, and stablizes and be difficult for acidolysis under acid system; (2) without additional holding reductant, saved cost.Due to formoxime fast restore Pu (IV), and can quick and HNO 2holding reductant during reaction can separate as the uranium plutonium simultaneously, without additional other reduction balustrade; (3) do not produce interphase impurity; (4) adopting the stream ratio that the stream ratio of 1BF:1BX is 1 ~ 4,1BF:1BS is 4 ~ 6, and the plutonium yield is greater than under 99.9% prerequisite, removes the plutonium separation factor in uranium>5*10 3, in plutonium, go the separation factor of uranium to be greater than 10 4.
Embodiment
Below in conjunction with embodiment, the present invention is further elaborated.
embodiment 1
Utilize reductive agent 1BX and supplementary extraction agent 1BS that the Pu in the 1BF feed liquid (IV) is reduced into to Pu (III), make plutonium enter water and uranium is retained in organic phase, realize the separation of uranium, plutonium, but this reductive agent fast restore Pu (IV), and can be fast and HNO 2holding reductant during reaction can separate as the uranium plutonium simultaneously, without additional other reduction balustrade.The processing condition of this technique and technological effect are as table 1:
Technique used and technological effect in table 1 embodiment 1
embodiment 2
The method used with embodiment 1 is identical, and different is processing condition, and processing condition used and corresponding result are as table 2:
Technique used and technological effect in table 2 embodiment 2
embodiment 3
The method used with embodiment 1 is identical, and different is processing condition, and processing condition used and corresponding result are as table 3:
Technique used and technological effect in table 3 embodiment 3
Figure 2012101668726100002DEST_PATH_IMAGE003

Claims (4)

1.Purex uranium, plutonium separating technology in flow process, this technique is in the 1B groove, to utilize reductive agent 1BX and supplementary extraction agent 1BS that the Pu in the 1BF feed liquid (IV) is reduced into to Pu (III), make plutonium enter water and uranium is retained in organic phase, realize the separation of uranium, plutonium, it is characterized in that, reductive agent 1BX used consists of: the formoxime of 0.1 ~ 0.2mol/L, the NO of 0.35 ~ 0.5mol/L 3 -and the H of 0.35 ~ 0.5mol/L +.
2. uranium, plutonium separating technology in Purex flow process according to claim 1, is characterized in that, the stream ratio that the stream ratio of described 1BF:1BX is 1 ~ 4,1BF:1BS is 4 ~ 6.
3. uranium, plutonium separating technology in Purex flow process according to claim 1, is characterized in that, extraction progression >=3 grade are mended in back extraction progression >=8 grade in described 1B groove.
4. uranium, plutonium separating technology in Purex flow process according to claim 1, is characterized in that, it is 21 ~ 42.5 ℃ that the temperature that described uranium, plutonium separate is controlled.
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Cited By (11)

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CN103820656A (en) * 2014-01-28 2014-05-28 中国原子能科学研究院 Uranium and plutonium separation technology in Purex process
CN104004928A (en) * 2014-05-30 2014-08-27 中国原子能科学研究院 Plutonium purification and concentration method
CN105734310A (en) * 2016-03-02 2016-07-06 中国原子能科学研究院 Plutonium purification and concentration method utilizing dioxime imide as reduction and reextraction agent
CN105779794A (en) * 2016-04-15 2016-07-20 中国原子能科学研究院 Uranium and plutonium separating technology with hydroxyamino acetic acid serving as reverse extracting reagent
CN105913887A (en) * 2016-04-14 2016-08-31 中国原子能科学研究院 Plutonium purification cycle process using formaldoxime as back extraction reagent
CN106893878A (en) * 2017-03-02 2017-06-27 中国原子能科学研究院 A kind of method that plutonium is reclaimed in the spentnuclear fuel from radioactivity
CN107130121A (en) * 2017-05-09 2017-09-05 中国原子能科学研究院 Neptunium, the uranium purification process of plutonium are removed simultaneously in a kind of nuclear fuel Purex post processings flow
CN108369828A (en) * 2015-10-21 2018-08-03 原子能和替代能源委员会 Application of the aldoxime containing at least five carbon atoms in plutonium reduction reextraction extract operation as anti-nitrous agent
CN108461166A (en) * 2018-02-23 2018-08-28 张国强 A kind of novel uranium plutonium mixed oxide fuel equipment
CN110831681A (en) * 2017-06-29 2020-02-21 原子能和替代能源委员会 Carboxamide for separating uranium (VI) and plutonium (IV) without reducing plutonium (IV)
CN111474234A (en) * 2020-03-13 2020-07-31 中国原子能科学研究院 Method for analyzing content of trace plutonium in large amount of uranium in nuclear fuel post-processing flow

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Cited By (15)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103820656A (en) * 2014-01-28 2014-05-28 中国原子能科学研究院 Uranium and plutonium separation technology in Purex process
CN104004928A (en) * 2014-05-30 2014-08-27 中国原子能科学研究院 Plutonium purification and concentration method
CN108369828A (en) * 2015-10-21 2018-08-03 原子能和替代能源委员会 Application of the aldoxime containing at least five carbon atoms in plutonium reduction reextraction extract operation as anti-nitrous agent
CN105734310A (en) * 2016-03-02 2016-07-06 中国原子能科学研究院 Plutonium purification and concentration method utilizing dioxime imide as reduction and reextraction agent
CN105734310B (en) * 2016-03-02 2018-03-09 中国原子能科学研究院 A kind of plutonium using dioxime Asia acid amides as reduction reextraction agent purifies method for concentration
CN105913887B (en) * 2016-04-14 2018-01-19 中国原子能科学研究院 It is a kind of to use formaldoxime to be stripped the plutonium purification cycle technique of reagent
CN105913887A (en) * 2016-04-14 2016-08-31 中国原子能科学研究院 Plutonium purification cycle process using formaldoxime as back extraction reagent
CN105779794A (en) * 2016-04-15 2016-07-20 中国原子能科学研究院 Uranium and plutonium separating technology with hydroxyamino acetic acid serving as reverse extracting reagent
CN106893878A (en) * 2017-03-02 2017-06-27 中国原子能科学研究院 A kind of method that plutonium is reclaimed in the spentnuclear fuel from radioactivity
CN106893878B (en) * 2017-03-02 2018-11-30 中国原子能科学研究院 A method of recycling plutonium from radioactivity spentnuclear fuel
CN107130121A (en) * 2017-05-09 2017-09-05 中国原子能科学研究院 Neptunium, the uranium purification process of plutonium are removed simultaneously in a kind of nuclear fuel Purex post processings flow
CN110831681A (en) * 2017-06-29 2020-02-21 原子能和替代能源委员会 Carboxamide for separating uranium (VI) and plutonium (IV) without reducing plutonium (IV)
CN108461166A (en) * 2018-02-23 2018-08-28 张国强 A kind of novel uranium plutonium mixed oxide fuel equipment
CN108461166B (en) * 2018-02-23 2019-05-07 柳州增程材料科技有限公司 A kind of equipment of uranium plutonium mixed oxide fuel
CN111474234A (en) * 2020-03-13 2020-07-31 中国原子能科学研究院 Method for analyzing content of trace plutonium in large amount of uranium in nuclear fuel post-processing flow

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