CN1375103A - Process for recycling ionic liquids - Google Patents

Process for recycling ionic liquids Download PDF

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Publication number
CN1375103A
CN1375103A CN00811751A CN00811751A CN1375103A CN 1375103 A CN1375103 A CN 1375103A CN 00811751 A CN00811751 A CN 00811751A CN 00811751 A CN00811751 A CN 00811751A CN 1375103 A CN1375103 A CN 1375103A
Authority
CN
China
Prior art keywords
ionic liquid
product
aforementioned
chloride
ethyl imidazol
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
CN00811751A
Other languages
Chinese (zh)
Inventor
A·J·简波斯
R·C·蒂得
肯尼斯·理查德·泽登
W·R·皮特勒
D·W·鲁尼
贾斯廷·E·哈特
T·韦尔顿
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sellafield Ltd
Original Assignee
British Nuclear Fuels PLC
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by British Nuclear Fuels PLC filed Critical British Nuclear Fuels PLC
Publication of CN1375103A publication Critical patent/CN1375103A/en
Pending legal-status Critical Current

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Classifications

    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21CNUCLEAR REACTORS
    • G21C19/00Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
    • G21C19/42Reprocessing of irradiated fuel
    • G21C19/44Reprocessing of irradiated fuel of irradiated solid fuel
    • G21C19/48Non-aqueous processes
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00Energy generation of nuclear origin
    • Y02E30/30Nuclear fission reactors
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02WCLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00Technologies for solid waste management
    • Y02W30/50Reuse, recycling or recovery technologies

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Extraction Or Liquid Replacement (AREA)
  • Removal Of Specific Substances (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Vaporization, Distillation, Condensation, Sublimation, And Cold Traps (AREA)

Abstract

A method for treating a spent ionic liquid composition includes heating the composition to form a partial decomposition product thereof. The product is separated from composition contaminants and the separated product is reacted with a reactant to regenerate the ionic liquid.

Description

Recycling ion liquid method
The field of the invention
The present invention relates to handle useless ion liquid method.The ionic liquid of hereinafter mentioning is the ionic liquid that was used in the reprocessing nuclear fuel, but it should be understood that the present invention can be used in all ionic liquid technical fields, is included in nuclear industry application in addition.
Background of the present invention
The ionic liquid that does not contain molecular solvent is at first open in a series of US patents (24446331,2446339,2446350) by Hurley and Wier.In general, ionic liquid is a salt, the potpourri of salt, or produce the potpourri of the component of one or more salt, it melts under the temperature that is lower than room temperature or a little higher than room temperature.(term used herein " salt " is meant the material of being made up of kation and anionic species fully).This class I liquid I is known as " ionic liquid ", though this term sometimes is used in reference to the salt that melts under higher temperature.In this manual, term " ionic liquid " is meant the salt that melts under 100 ℃ temperature at the most.
Pendent patent application PCT/GB99/00246 discloses the method for reprocessing spent nuclear fuel, and it comprises that the ingredient with spent fuel or spent fuel is dissolved in the ionic liquid, and other component in fissile material and the radioactive fuel is separated basically.The ion liquid subsequent treatment that is obtained is also disclosed, by solvent extraction or electrochemical treatment to reclaim dissolved uranium or plutonium.
Except easy fissioner, useless ionic liquid also contains the fission product that dissolves with uranium.People have paid bigger effort and have developed a kind of in the cheap approach of expense of removing these pollutants after mixture separation goes out uranium with the form that is fit to convert it into the stabilize waste form.
Can realize removing of pollutant by any or combination in many different approaches.Selected fission product such as plutonium can be by applying proper voltage with the electrochemical means extracting.The shortcoming of this method is that electrolysis is expensive process, especially when carrying out on industrial scale.
Fission product can come to extract from ionic liquid in addition or further by adding organic solvent.The interpolation of organic substance causes the precipitation of fission product compound.Sediment can filter out from ionic liquid and be converted to oxide through calcining before consolidation step.Ionic liquid after the cleaning can be recovered then and be applied in the electrorefining.
Burning is another alternative plan of removing pollutant, and wherein useless ionic liquid is heated to and surpasses 200 ℃ temperature.The shortcoming of this process can be measured from the angle of economy; The burning of imidazole salts causes the generation of carbon dioxide, water and oxides of nitrogen potpourri (NOx).This means that ionic liquid can not recycle and in fact catching hell.
Because a factor of maximum cost is the cost of essential raw material in the industry, helping by recycling any method that at utmost reduces these costs obviously is the alternative plan that has more temptation.
Narration of the present invention
According to the invention provides the method for handling the useless ionic liquid compositions that comprises ionic liquid and pollutant, this method comprises that the described ionic liquid of heating is to form its partially decomposed product, with this product and described separated from contaminants, allow the reaction of separated products and reaction reagent then with this ionic liquid of regenerating.
When the 1-methyl-when 3-ethyl imidazol(e) chloride under reduced pressure heated, the decomposition of ion liquid section ground obtained 1-methylimidazole, 1-ethyl imidazol(e), methyl chloride and chloric ethane.In initial experiment, this pyrolysis product was at room temperature placed 2 days and was reacted again and obtains 1,3-methylimidazole chloride, 1,3-diethyl imidazolium chloride and 1-methyl-muriatic potpourri of 3-ethyl imidazol(e).These results are wonderful, are considered to destroy recycling ion liquid any current potential because thermal decomposition is former.Yet,, be used to clean ion liquid thermal decomposition and it seems it is attractive economically selection scheme now for these experiments.
Preferably, make decomposition product with at least a other decomposition product and separated from contaminants.Separation can realize by the volatilization in heating process.In one embodiment of the invention, partially decomposed product separates with at least a other decomposition product by distillation.
Preferably, ionic liquid is at 200-300 ℃ or more preferably be heated under 2mmHg or lower low pressure under 220 ℃-250 ℃ the temperature.
Of the present invention being described in detail
Useless ionic liquid for example 1-methyl-3-ethyl imidazol(e) chloride is polluted by fission product, also may be polluted by organic radiolytic product, and need handle, in order that to be suitable for converting it into the form recovery fission product of stabilize waste form.
In the method according to the invention, heating under reduced pressure under the temperature of ionic liquid in 200 ℃ of-300 ℃ of scopes.In preferred embodiments, 1-methyl-3-ethyl imidazol(e) had been lower than under the pressure of 2mmHg under 220-250 ℃ temperature heating 2-3 hour.The only decomposition of part takes place in these conditions permit ionic liquids, therefore allows to reclaim the useful constituent compound as much as possible in the ionic liquid.It should be understood that imidazole salts that condition that part decomposes replaces for difference all is different with different mixtures for them.
Ion liquid pyrolysis causes the generation of volatility pyrolysis product.For 1-methyl-3-ethyl imidazol(e) chloride, these products are 1-methylimidazoles, 1-ethyl imidazol(e), methyl chloride and chloric ethane.Chloric ethane resolves into hydrogen chloride and ethene then.
Volatile products are collected in the cold-trap, and the follow-up distillation of potpourri can be isolated each component.The volatile component of tool is hydrogen chloride and ethene.Hydrogen chloride can use the oxyhydroxide scrubber to wash from system, and ethene can be bottled or be burnt as accessory substance.
The 1-methylimidazole can separate by distilling with the 1-ethyl imidazol(e), so that specific ionic liquid 1-methyl-3-ethyl imidazol(e) chloride obtains regeneration.It should be understood that at 1-methyl-3-ethyl imidazol(e) chloride, 1,3-methylimidazole chloride and 1, the technology that the potpourri of 3-diethyl imidazolium chloride is operated is not need detachment process.
Specific if desired ionic liquid 1-methyl-3-ethyl imidazol(e) chloride, isolated 1-methylimidazole and chloric ethane reaction, thus make initial ionic liquid 1-methyl-3-ethyl imidazol(e) chloride regeneration.Because by decomposing, some chloric ethanes have lost, add fresh chloric ethane with this ionic liquid of holomorphosis.1-ethyl imidazol(e) and methyl chloride react and make ionic liquid 1-methyl-3-ethyl imidazol(e) chloride regeneration.
In a preferred embodiment of the invention, the fission product residue changes into stable waste formation through calcining.In another embodiment, fission product residue and acid reaction and being converted to can be made the discarded suitable form of handling.

Claims (23)

1. handle the method for the useless ionic liquid compositions that comprises ionic liquid and pollutant, this method comprises that the described ionic liquid of heating is to form its partially decomposed product, this product and described separated from contaminants are opened, allowed separated products and the described ionic liquid of reaction reagent reaction regeneration then.
2. according to the process of claim 1 wherein that product and at least a other decomposition product that described part is decomposed open with described separated from contaminants together.
3. according to the method for claim 2 or claim 3, the product that wherein said part is decomposed is separated by distillation and at least a other decomposition product.
4. according to any one method in the aforementioned claim, the product that wherein said part is decomposed reacts with at least a other decomposition product described ionic liquid is regenerated.
5. according to any one method in the aforementioned claim, wherein said separation is to realize by the volatilization in heating process.
6. according to any one method in the aforementioned claim, wherein said ionic liquid is 1-methyl-3-ethyl imidazol(e) chloride.
7. according to the method for claim 6, the product that wherein said part is decomposed is the 1-methylimidazole, 1-ethyl imidazol(e), the potpourri of methyl chloride and chloric ethane.
8. according to the method for claim 7, wherein 1-methylimidazole and chloric ethane react the 1-methyl of regenerating-3-ethyl imidazol(e) chloride.
9. according to the method for claim 5, the product that wherein said part is decomposed is the 1-ethyl imidazol(e).
10. according to the method for claim 9, wherein 1-ethyl imidazol(e) and methyl chloride react the 1-methyl of regenerating-3-ethyl imidazol(e) chloride.
11. according to any one method in the aforementioned claim, wherein said ionic liquid under reduced pressure is heated.
12. according to the method for claim 11, wherein said pressure is 2mmHg or lower.
13. according to any one method in the aforementioned claim, wherein said ionic liquid is heated to 200-300 ℃ temperature.
14. according to the method for claim 13, wherein said ionic liquid is heated to 220-250 ℃ temperature.
15. according to any one method among the claim 3-14, wherein the volatile products that obtain from described ion liquid volatilization are collected in the cold-trap.
16. according to any one method in the aforementioned claim, wherein hydrogen chloride is by heating that described ionic liquid produces and by using the oxyhydroxide scrubber from system it to be disposed.
17., wherein produce ethene by heating described ionic liquid according to any one method in the aforementioned claim.
18. according to the method for claim 17, wherein said ethene is bottled or is burnt as accessory substance.
19. reprocessing nuclear fuel and the technology of handling the waste salt that is polluted by fission product, this technology comprises the method for arbitrary aforementioned claim.
20., wherein described fission product is polluted residue and separates and before waste treatment, calcine according to the technology of claim 19.
21., wherein before waste treatment, make described fission product pollute residue and acid reaction according to the technology of claim 19.
22. the purposes of thermal decomposition in useless ion liquid processing, wherein decomposition product is used to ion liquid regeneration.
23. according to the purposes of claim 23, wherein said ionic liquid is used to the reprocessing of spent nuclear fuel.
CN00811751A 1999-08-19 2000-08-21 Process for recycling ionic liquids Pending CN1375103A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB9919606.5 1999-08-19
GB9919606A GB9919606D0 (en) 1999-08-19 1999-08-19 Process for recycling ionic liquids

Publications (1)

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CN1375103A true CN1375103A (en) 2002-10-16

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EP (1) EP1218890A2 (en)
JP (1) JP2003507185A (en)
CN (1) CN1375103A (en)
AU (1) AU7018700A (en)
GB (1) GB9919606D0 (en)
WO (1) WO2001015175A2 (en)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101925408A (en) * 2007-12-28 2010-12-22 雪佛龙美国公司 Process for ionic liquid catalyst regeneration
CN105597630B (en) * 2012-02-14 2018-02-23 雪佛龙美国公司 Used ionic-liquid catalyst is hydrolyzed for disposal
CN112680609A (en) * 2020-12-14 2021-04-20 中国人民解放军63653部队 Plutonium recovery ionic liquid extractant and method for extracting and separating plutonium from plutonium-containing waste liquid

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US6991718B2 (en) 2001-11-21 2006-01-31 Sachem, Inc. Electrochemical process for producing ionic liquids
AU2003263890A1 (en) 2002-08-16 2004-03-03 Sachem, Inc. Lewis acid ionic liquids
US8247117B2 (en) * 2004-12-27 2012-08-21 National Institute Of Advanced Industrial Science And Technology Ionic liquid
JP4652359B2 (en) * 2007-03-09 2011-03-16 日本合成化学工業株式会社 Decomposition treatment method of ionic liquid
JP4753141B2 (en) * 2007-08-01 2011-08-24 独立行政法人 日本原子力研究開発機構 Method for dissolving and separating uranium using ionic liquid, and method for recovering uranium using the same
KR100974890B1 (en) 2008-04-18 2010-08-11 인하대학교 산학협력단 A recycling process of ionic liquids using microwave irradiation
JP4843106B2 (en) * 2011-01-24 2011-12-21 独立行政法人日本原子力研究開発機構 Uranium recovery method using ionic liquid
JP5734004B2 (en) * 2011-02-07 2015-06-10 三菱重工業株式会社 Method and apparatus for treating plutonium-containing waste liquid
WO2013098056A1 (en) 2011-12-28 2013-07-04 Lanxess Deutschland Gmbh Purification of optionally hydrogenated nitrile rubber
WO2014184803A2 (en) 2013-04-19 2014-11-20 Reliance Industries Limited A process for regenerating ionic compound
JP2020094979A (en) 2018-12-14 2020-06-18 日立Geニュークリア・エナジー株式会社 Organic iodine collection apparatus and organic iodine collection method
JP7470491B2 (en) 2019-02-25 2024-04-18 日立Geニュークリア・エナジー株式会社 Organic iodine remover
JP7281393B2 (en) 2019-12-18 2023-05-25 日立Geニュークリア・エナジー株式会社 Organic iodine remover and organic iodine remover
JP7373454B2 (en) 2020-04-10 2023-11-02 日立Geニュークリア・エナジー株式会社 Organic iodine collection device
US11578278B2 (en) 2020-08-01 2023-02-14 Honeywell International Inc. Renewable transportation fuel process with thermal oxidation system
US11780795B2 (en) 2020-08-04 2023-10-10 Honeywell International Inc. Cumene-phenol complex with thermal oxidation system
US11578020B2 (en) 2020-08-04 2023-02-14 Honeywell International Inc. Naphtha complex with thermal oxidation system
US12017984B2 (en) 2020-08-04 2024-06-25 Honeywell International Inc. Propane/butane dehydrogenation complex with thermal oxidation system
US11492306B2 (en) * 2020-09-30 2022-11-08 Honeywell International Inc. Alkylation process with thermal oxidation system
JP2024025247A (en) 2022-08-10 2024-02-26 日立Geニュークリア・エナジー株式会社 filter vent device

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GB9719551D0 (en) * 1997-09-16 1997-11-19 British Nuclear Fuels Plc Treatment of molten salt reprocessing wastes
GB9802852D0 (en) * 1998-02-11 1998-04-08 British Nuclear Fuels Plc Nuclear fuel reprocessing

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101925408A (en) * 2007-12-28 2010-12-22 雪佛龙美国公司 Process for ionic liquid catalyst regeneration
CN105597630B (en) * 2012-02-14 2018-02-23 雪佛龙美国公司 Used ionic-liquid catalyst is hydrolyzed for disposal
CN112680609A (en) * 2020-12-14 2021-04-20 中国人民解放军63653部队 Plutonium recovery ionic liquid extractant and method for extracting and separating plutonium from plutonium-containing waste liquid

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Publication number Publication date
GB9919606D0 (en) 1999-10-20
WO2001015175A2 (en) 2001-03-01
JP2003507185A (en) 2003-02-25
WO2001015175A3 (en) 2002-02-21
EP1218890A2 (en) 2002-07-03
AU7018700A (en) 2001-03-19

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