CN1203489C - Method for back-extracting and separating radioactive element from organic phase by using water soluble oxaamide - Google Patents
Method for back-extracting and separating radioactive element from organic phase by using water soluble oxaamide Download PDFInfo
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- CN1203489C CN1203489C CNB031463940A CN03146394A CN1203489C CN 1203489 C CN1203489 C CN 1203489C CN B031463940 A CNB031463940 A CN B031463940A CN 03146394 A CN03146394 A CN 03146394A CN 1203489 C CN1203489 C CN 1203489C
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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
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Abstract
The present invention relates to a method for back extracting and separating radioactive elements from an organic phase by using water soluble oxa-amide, which belongs to the fields of nuclear fuel reprocessing, high activity liquid waste separation, applied chemistry, etc. The method uses an alkyl-3-oxa-valeramide water solution of which the length of a substituting alkyl carbon chain is smaller than the length of 3 carbon elements as a back extracting agent, transuranic elements and lanthanide elements are back extracted through multilevel cross current or are back extracted through continuous countercurrent in organic phases of tributyl phosphate and trialkylphosphine oxide, and actinide elements and the lanthanide elements are extracted from the tributyl phosphate and the trialkylphosphine oxide. The method has the advantages of simple back extraction flow, little secondary waste, etc.
Description
Technical field
The present invention relates to particularly use the oxa-acid amides of substituted alkyl carbochain less than 3 carbon with the water-soluble oxa-acid amides method that back extraction separates radioelement from organic phase.Belong to the nuclear fuel aftertreatment, high activity liquid waste separates, fields such as applied chemistry.
Background technology
The spentnuclear fuel that nuclear power station produces has produced high activity liquid waste (HLLW) through aftertreatment, and the processing of high activity liquid waste is one of key issue that influences at present nuclear energy uses with disposing, and also is the major issue that influences environment for human survival.
It is plutonium reduction recovery (PUREX) flow process of extractant that the aftertreatment of spentnuclear fuel is generally adopted at present with tributyl phosphate (TBP).This flow process comprises three circulations: the codecontamination of uranium plutonium, uranium purifying, plutonium purifying.Promptly earlier from the spentnuclear fuel lysate, extract uranium, plutonium simultaneously, from load organic phases, carry out the uranium plutonium and separate, carry out uranium, plutonium purifying then respectively.The experience of this flow process existing decades of industry operation, but the improvement of basic procedure is being carried out has always proposed some technically and more rational economically flow process.
For the processing of HLLW, except that the glass solidification deep stratum is stored, mainly contain at present separation-transmuting (Partitioning-Transmutation, P-T) with separate-reorganize and outfit (Partitioning-Conditioning, P-C) two kinds of methods.Research of Separation Technique to actinide among the HLLW is the focus of this area research, has proposed multiple separation process, and wherein trialkyl phosphine (TRPO) flow process of China's research is considered to two in the world one of flow process of application prospect most.In the TRPO flow process, at first with 30% trialkyl oxidation see-kerosene extracts actinide, uses 5.5mol/LHNO then respectively from high activity liquid waste
3, 0.6mol/L oxalic acid and 5%Na
2CO
3Solution carries out back extraction, obtains americium+rare earth, neptunium+plutonium and three logistics of uranium.From separation-transmuting viewpoint, each logistics separately is favourable, but flow process is comparatively complicated, and required progression is more; From separating-reorganize and outfit viewpoint, transuranic element is separated together, be cured, can make process simplification like this, be easy to industrial realization.
Uranium, plutonium that collection is gone in the TBP organic phase strip out with reductive agents such as ferrous sulfamate, uranouss, the transuranic element and the lanthanide series that are extracted in the TRPO organic phase strip out with nitric acid, oxalic acid, and there is the bad decomposition of back extraction thing in above-mentioned back washing agent, produces shortcomings such as the secondary refuse is many.
Summary of the invention
It is simpler to the purpose of this invention is to provide a kind of back extraction flow process, the method that the back extraction that the secondary refuse is few separates radioelement.Amide substance has stronger complexing to many metallic ions, has been used for some metallic ion and radioactive nuclide are extracted.But all be it to be dissolved in the organic solvent use up to now, as extractant.The report that uses as back washing agent of water breakthrough dissolubility amide substance not as yet.The present invention utilizes the water-soluble character of short acid amides of the strong complexing of amide substance and substituting group carbochain, with water-soluble amide as the back washing agent in nuclear fuel aftertreatment and the HLLW treatment scheme.
The inventive method selects for use the substituted alkyl carbon chain lengths to make back washing agent less than the alkyl-3-oxa-pentanamide aqueous solution of 3 carbon, from the organic phase of the tributyl phosphate that extracted actinide and lanthanide series and trialkyl phosphine, strip/or continuous flow upstream reextraction transuranic element and lanthanide series through multistage cross flow.Uranium is then still stayed organic phase, thereby realizes separating of uranium and transuranic element and lanthanide series.Uranium can continue to use through subsequent treatment, and transuranic element is with after lanthanide series separates, or glass solidification or become the short-half-life nucleic through transmuting, and radioactive long-term hazards is reduced to minimum.
As back washing agent, have following characteristics with water-soluble oxa-acid amides:
1, contain in the water-soluble oxa-amide molecule and transuranic element and the very strong coordinating group of lanthanide series complexing power, can make transuranic element and lanthanide series fully from organic extractant back extraction come out, stripping efficiency is near 100%.
2, water-soluble oxa-acid amides can be dissolved in the aqueous solution fully, and the dissolving in organic phase is less than 1%, and back washing agent in use loses very little.
3, water-soluble oxa-acid amides is made up of C, H, O, N element, and the back extraction product decomposes easily, and does not produce the secondary solid refuse.
4, water-soluble oxa-acid amides synthetic method is simple, with low cost, is convenient to industrial-scale production.
5, water-soluble oxa-acid amides can be from neutral phosphor (phosphine) acid extraction agent, acid phosphorus (phosphine) acid extraction agent and amide-type extractant back extraction transuranic element and lanthanide series, and the uranium of not stripping.
Description of drawings
Fig. 1 is a cross-flow reextraction process flow diagram.Material liquid is introduced from the first order, and each level all adds fresh back washing agent S, and the back extraction organic phase of each grade gained continues to contact back extraction once more with fresh back washing agent in the one-level of back, till radioactive element content meets the requirements in the organic phase after the back extraction that obtains.
Fig. 2 gets process flow diagram for countercurrent reextraction.Load organic phases adds from the left side, and back washing agent adds from the right side, and two phase countercurrent flow flows.
Embodiment
Selected water-soluble oxa-acid amides has two kinds: monoamides and bisamide, and its molecular formula is as follows:
(I) monoamides
R wherein, R ' can be methyl, ethyl or propyl group.
(II) bisamide
R wherein
1, R
2, R
3, R
4Can be respectively methyl, ethyl or propyl group.
Fig. 1,2 is process chart of the present invention.1,2,3,4,5 are the section of stripping among the figure, and each section is an one-level.O
1Be the organic phase after the load (containing extractants such as TBP or TRPO); S is back washing agent (a water-soluble oxa-acid amides); P is the water that contains actinide; O
2Be the organic phase after stripping.
The organic phase O that contains actinide (uranium and transuranic element) and lanthanide series
1Enter the 1st grade of cross-flow reextraction flow process, contact with fresh back washing agent S step by step, S is with O
1In most of transuranic element and lanthanide series be stripped into water and become P, organic phase has become the organic phase O that only contains uranium
2, through 3-5 level cross-flow back extraction, the transuranic element of approaching＞99% and lanthanide series enter water P.Perhaps, the organic phase O that contains actinide (uranium and transuranic element) and lanthanide series
1Enter countercurrent reextraction and get the 1st grade of flow process, with the back washing agent S counter current contacting that adds from final stage, S is with O
1In most of transuranic element and lanthanide series be stripped into water and become P, organic phase has become the organic phase O that only contains uranium
2, through the back extraction of 3-5 stage countercurrent, the transuranic element of approaching＞99% and lanthanide series enter water P.
Carry out cross-flow reextraction test by reextraction flow process shown in Figure 1, concrete parameter is as follows:
O
1: the organic phase of uranium-bearing, transuranic element and lanthanide series (30%v/v TRPO-kerosin)
S: contain the water-soluble N of 0.5mol/L, N-dialkyl group-3-oxa--penta monoamides solution, acidity is 0.1-0.8mol/L HNO
3
P, P
1, P
2, P
3, P
4, P
5: the strip aqueous product stream that contains transuranic element and lanthanide series.
O
2: the organic phase of a uranium-bearing
Back extraction progression: 5 grades; Stream ratio: organic phase/water=1: 1
Back-extraction time; 30 minutes; Reextraction temperature: 25 ℃
The back extraction ratio of transuranic element and lanthanide series is greater than 99%, and the back extraction ratio of uranium is less than 0.1%.
Carry out cross-flow reextraction test by Fig. 1 flow process, wherein:
S: contain the water-soluble N of 0.1mol/L, N, N ', N '-tetraalkyl-3-oxa--glutaramide solution, acidity is 1.5--2.0mol/LHNO
3
All the other parameters are with embodiment 1.Strip through 5 grades of cross-flows, can the reaching more than 99% of the stripping rate of transuranic element and lanthanide series, the stripping rate of uranium is less than 0.1%.
Carry out cross-flow reextraction test by Fig. 1 flow process, wherein:
O
1: the organic phase of uranium-bearing and plutonium (30%TBP-kerosin)
All the other parameters are stripped through 5 grades of cross-flows with embodiment 1, and the back extraction ratio of plutonium is greater than 99.9%, and the back extraction ratio of uranium is less than 0.1%.
Carry out cross-flow reextraction test by flow process shown in Figure 1, wherein:
O
1: the organic phase of uranium-bearing and plutonium (30%TBP-kerosin), all the other parameters are with embodiment 2.Strip through 5 grades of cross-flows, the back extraction ratio of plutonium is greater than 99.9%, and the back extraction ratio of uranium is less than 0.1%.
Claims (3)
1, the water-soluble oxa-acid amides of a kind of usefulness separates the method for radioelement from the organic phase back extraction, it is characterized in that: make back washing agent less than the alkyl-3-oxa-pentanamide aqueous solution of 3 carbon with the substituted alkyl carbon chain lengths, from the organic phase of the tributyl phosphate that extracted actinide and lanthanide series and trialkyl phosphine, strip/or continuous flow upstream reextraction transuranic element and lanthanide series through multistage cross flow.
The method of 2, separating radioelement from the organic phase back extraction according to the water-soluble oxa-acid amides of the said a kind of usefulness of claim 1, it is characterized in that said substituted alkyl carbon chain lengths is N less than the alkyl-3-oxa-pentanamide aqueous solution of 3 carbon, N-dialkyl group-3-oxa--penta monoamides solution.
The method of 3, separating radioelement from the organic phase back extraction according to the water-soluble oxa-acid amides of the said a kind of usefulness of claim 1, it is characterized in that said substituted alkyl carbon chain lengths is N less than the alkyl-3-oxa-pentanamide aqueous solution of 3 carbon, N, N ', N '-tetraalkyl-3-oxa--glutaramide solution.
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| Application Number | Priority Date | Filing Date | Title |
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| CNB031463940A CN1203489C (en) | 2003-07-11 | 2003-07-11 | Method for back-extracting and separating radioactive element from organic phase by using water soluble oxaamide |
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| CNB031463940A CN1203489C (en) | 2003-07-11 | 2003-07-11 | Method for back-extracting and separating radioactive element from organic phase by using water soluble oxaamide |
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| CN1203489C true CN1203489C (en) | 2005-05-25 |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| FR3039696B1 (en) * | 2015-07-29 | 2017-07-28 | Commissariat Energie Atomique | ONE-CYCLE TREATMENT METHOD, FREE OF PLUTONIUM REDUCTIVE EXTRACTION OPERATION, OF A NITRIC AQUEOUS SOLUTION OF DISSOLUTION OF US NUCLEAR FUEL |
| FR3042903B1 (en) * | 2015-10-21 | 2017-12-08 | Commissariat Energie Atomique | USE OF HYDROXYIMINOALCANOIC ACIDS AS ANTI-NITROUS AGENTS IN PLUTONIUM-REDUCTIVE DESEXTRACTION OPERATIONS |
| FR3068257B1 (en) * | 2017-06-29 | 2022-01-14 | Commissariat Energie Atomique | CARBAMIDES FOR THE SEPARATION OF URANIUM(VI) AND PLUTONIUM(IV) WITHOUT PLUTONIUM(IV) REDUCTION |
| CN111863298B (en) * | 2020-06-10 | 2022-08-05 | 中国原子能科学研究院 | Deep purification method of PUREX process polluted solvent |
| CN111650142A (en) * | 2020-07-09 | 2020-09-11 | 中国原子能科学研究院 | Method for analyzing concentration of nitrous acid in uranium-containing organic phase |
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