CN112226635A - Uranyl ion separation method based on carboxyl functional ionic liquid - Google Patents
Uranyl ion separation method based on carboxyl functional ionic liquid Download PDFInfo
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- 238000000926 separation method Methods 0.000 title claims abstract description 51
- 239000002608 ionic liquid Substances 0.000 title claims abstract description 36
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 title claims abstract description 35
- WYICGPHECJFCBA-UHFFFAOYSA-N dioxouranium(2+) Chemical compound O=[U+2]=O WYICGPHECJFCBA-UHFFFAOYSA-N 0.000 title claims description 7
- 238000000605 extraction Methods 0.000 claims abstract description 87
- -1 uranyl ions Chemical class 0.000 claims abstract description 28
- 238000000034 method Methods 0.000 claims abstract description 25
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000007864 aqueous solution Substances 0.000 claims abstract description 18
- 229910052698 phosphorus Inorganic materials 0.000 claims abstract description 18
- 239000011574 phosphorus Substances 0.000 claims abstract description 18
- 239000000243 solution Substances 0.000 claims description 26
- SGZRFMMIONYDQU-UHFFFAOYSA-N n,n-bis(2-methylpropyl)-2-[octyl(phenyl)phosphoryl]acetamide Chemical compound CCCCCCCCP(=O)(CC(=O)N(CC(C)C)CC(C)C)C1=CC=CC=C1 SGZRFMMIONYDQU-UHFFFAOYSA-N 0.000 claims description 22
- ZXMGHDIOOHOAAE-UHFFFAOYSA-N 1,1,1-trifluoro-n-(trifluoromethylsulfonyl)methanesulfonamide Chemical compound FC(F)(F)S(=O)(=O)NS(=O)(=O)C(F)(F)F ZXMGHDIOOHOAAE-UHFFFAOYSA-N 0.000 claims description 19
- 239000000463 material Substances 0.000 claims description 9
- 238000004458 analytical method Methods 0.000 claims description 8
- 229910052757 nitrogen Inorganic materials 0.000 claims description 6
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 claims description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- 239000008346 aqueous phase Substances 0.000 claims description 4
- QUXFOKCUIZCKGS-UHFFFAOYSA-N bis(2,4,4-trimethylpentyl)phosphinic acid Chemical compound CC(C)(C)CC(C)CP(O)(=O)CC(C)CC(C)(C)C QUXFOKCUIZCKGS-UHFFFAOYSA-N 0.000 claims description 4
- 238000002354 inductively-coupled plasma atomic emission spectroscopy Methods 0.000 claims description 4
- 230000010355 oscillation Effects 0.000 claims description 4
- 238000002474 experimental method Methods 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 3
- KQFVVXPBOWQBIL-UHFFFAOYSA-N 2-(3-ethylimidazol-1-ium-1-yl)acetate Chemical compound CCN1C=C[N+](CC([O-])=O)=C1 KQFVVXPBOWQBIL-UHFFFAOYSA-N 0.000 claims description 2
- ZATMQQFXKCSCSO-UHFFFAOYSA-N 2-(3-methylimidazol-3-ium-1-yl)acetate Chemical compound C[N+]=1C=CN(CC([O-])=O)C=1 ZATMQQFXKCSCSO-UHFFFAOYSA-N 0.000 claims description 2
- VJAMETCERVCPLT-UHFFFAOYSA-N CC(C([O-])=O)[N+]1=CN(C)C=C1 Chemical compound CC(C([O-])=O)[N+]1=CN(C)C=C1 VJAMETCERVCPLT-UHFFFAOYSA-N 0.000 claims description 2
- ZRKPPMNYQAOPIN-UHFFFAOYSA-N CCC(C([O-])=O)[N+]1=CN(C)C=C1 Chemical compound CCC(C([O-])=O)[N+]1=CN(C)C=C1 ZRKPPMNYQAOPIN-UHFFFAOYSA-N 0.000 claims description 2
- JZHZHERKWYDLOH-UHFFFAOYSA-N CCCCN1C=C[N+](CC([O-])=O)=C1 Chemical compound CCCCN1C=C[N+](CC([O-])=O)=C1 JZHZHERKWYDLOH-UHFFFAOYSA-N 0.000 claims description 2
- 239000003570 air Substances 0.000 claims description 2
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 239000000919 ceramic Substances 0.000 claims description 2
- 238000007865 diluting Methods 0.000 claims description 2
- 229910052734 helium Inorganic materials 0.000 claims description 2
- 239000001307 helium Substances 0.000 claims description 2
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 claims description 2
- 230000001788 irregular Effects 0.000 claims description 2
- 229910052751 metal Inorganic materials 0.000 claims description 2
- 239000002184 metal Substances 0.000 claims description 2
- 229910052754 neon Inorganic materials 0.000 claims description 2
- GKAOGPIIYCISHV-UHFFFAOYSA-N neon atom Chemical compound [Ne] GKAOGPIIYCISHV-UHFFFAOYSA-N 0.000 claims description 2
- 239000004033 plastic Substances 0.000 claims description 2
- 239000010453 quartz Substances 0.000 claims description 2
- 239000005060 rubber Substances 0.000 claims description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910001220 stainless steel Inorganic materials 0.000 claims description 2
- 239000010935 stainless steel Substances 0.000 claims description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims 2
- 229910002092 carbon dioxide Inorganic materials 0.000 claims 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims 1
- 239000001569 carbon dioxide Substances 0.000 claims 1
- 229910052760 oxygen Inorganic materials 0.000 claims 1
- 239000001301 oxygen Substances 0.000 claims 1
- 125000005289 uranyl group Chemical group 0.000 claims 1
- 229910052770 Uranium Inorganic materials 0.000 abstract description 7
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 abstract description 7
- 239000002915 spent fuel radioactive waste Substances 0.000 abstract description 5
- 238000004064 recycling Methods 0.000 abstract description 4
- 239000002253 acid Substances 0.000 abstract description 3
- 238000011156 evaluation Methods 0.000 description 5
- 239000003758 nuclear fuel Substances 0.000 description 4
- 238000011161 development Methods 0.000 description 3
- 230000005855 radiation Effects 0.000 description 3
- 239000003085 diluting agent Substances 0.000 description 2
- 238000010790 dilution Methods 0.000 description 2
- 239000012895 dilution Substances 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 229910052778 Plutonium Inorganic materials 0.000 description 1
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 1
- 206010041662 Splinter Diseases 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- UBAZGMLMVVQSCD-UHFFFAOYSA-N carbon dioxide;molecular oxygen Chemical compound O=O.O=C=O UBAZGMLMVVQSCD-UHFFFAOYSA-N 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 239000003350 kerosene Substances 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000002901 radioactive waste Substances 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B60/00—Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
- C22B60/02—Obtaining thorium, uranium, or other actinides
- C22B60/0204—Obtaining thorium, uranium, or other actinides obtaining uranium
- C22B60/0217—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes
- C22B60/0252—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries
- C22B60/026—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries liquid-liquid extraction with or without dissolution in organic solvents
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/20—Treatment or purification of solutions, e.g. obtained by leaching
- C22B3/26—Treatment or purification of solutions, e.g. obtained by leaching by liquid-liquid extraction using organic compounds
- C22B3/37—Treatment or purification of solutions, e.g. obtained by leaching by liquid-liquid extraction using organic compounds containing boron, silicon, selenium or tellurium
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
- C22B7/006—Wet processes
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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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/20—Recycling
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- Environmental & Geological Engineering (AREA)
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Abstract
The invention provides a method for separating uranyl ions based on carboxyl functional ionic liquid, which combines a phosphorus-containing extractant with higher acid resistance and carboxyl functional ionic liquid with excellent stability, and can quickly separate UO in an aqueous solution through room-temperature extraction conditions2 2+And (5) separating. The invention realizes UO based on carboxyl functional ionic liquid2 2+Can be used for rapid separation and enrichment of UO with high concentration2 2+The method can be used for industrial extraction and separation and simultaneously can be used for UO in spent fuel aftertreatment2 2+The separation process is a rapid, convenient and efficient UO separation process2 2+The method has important significance for fully recycling and utilizing uranium.
Description
Technical Field
The invention belongs to UO2 2+In particular to a uranyl ion separation method based on carboxyl functional ionic liquid.
Background
Nuclear energy has the advantages of not emitting pollutants into the atmosphere, not generating greenhouse gases, and the like, and is considered as clean and low-carbon energy. Advanced nuclear fuel cycle is a necessary path for sustainable development of nuclear energy, and the post-treatment of spent fuel is a key link in the advanced nuclear fuel cycle. Uranium is the most important nuclear fuel in nuclear energy utilization, and the recycling of uranium in the nuclear fuel cycle post-treatment is significant to the sustainable development of nuclear energy. The sustainable development of nuclear energy must solve two major problems: optimization of uranium resource utilization and minimization of nuclear waste. Currently, the practically used PUREX post-treatment process uses 30% tributyl phosphate (TBP) as an extractant and kerosene as a diluent to recover uranium and plutonium at the same time. Indeed, conventional UO2 2+In the separation method, the diluent has the problems of easy volatilization, easy combustion, poor radiation stability, low critical concentration of splinter elements in a system and the like.
Disclosure of Invention
In view of the above, the invention provides a uranyl ion separation method based on a carboxyl functional ionic liquid. The invention combines the phosphorus-containing extractant with higher acid resistance with the carboxyl functional ionic liquid with excellent stability to develop the rapid separation of UO in the enriched aqueous solution2 2+Can be used for UO in spent fuel aftertreatment2 2+Can be used in UO separation and enrichment process2 2+The method has important significance for fully recycling and utilizing uranium.
The invention specifically adopts the following technical scheme:
a uranyl ion separation method based on carboxyl functional ionic liquid is characterized by comprising the following steps:
a) preparing an extraction system: weighing a proper amount of phosphorus-containing extractant according to the requirement of a separation system, dissolving the phosphorus-containing extractant by using carboxyl functional ionic liquid, and preparing carboxyl functional ionic liquid solution of the phosphorus-containing extractant with specified concentration, namely the required extraction system;
b) an extraction separation process: will be concentratedDegree C0UO of2 2+Adding the aqueous solution and the carboxyl functional ionic liquid solution containing the phosphorus extractant into an extraction device according to a certain ratio, placing the extraction device into a constant-temperature oscillation device, and carrying out extraction separation experiments under different conditions according to requirements;
c) UO in solution2 2+And (3) concentration analysis: diluting an appropriate amount of aqueous phase solution before and after extraction separation, and performing ICP-OES analysis on the diluted solution to obtain UO in the aqueous phase solution after extraction separation2 2+Concentration C1；
d) Calculation of separation efficiency: using the formula E ═ C0-C1)/C0x 100% calculation of the extraction System with respect to UO2 2+The extraction efficiency of (2).
Further, in step a), the phosphorus-containing extractant may be selected from any one of the following materials: N-octylphenyl-N, N' -diisobutylaminocarboxylphosphine oxide (CMPO), 1, 8-bis-diphenylphosphinoyl-2, 7-octanedione (DPPODO), bis (2, 4, 4-trimethylpentyl) phosphinic acid (Cyanex272), tributyl phosphate (TBP), and the like.
Further, in step a), the carboxyl functional ionic liquid can be selected from any one of the following materials: 1-carboxymethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt ([ HOOCmim)][NTf2]) 1-carboxyethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxypropyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxymethyl-3-ethylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxymethyl-3-butylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxymethyl-3-pentylimidazolium bistrifluoromethylsulfonyl imide salt and the like.
Further, in the step a), the concentration of the phosphorus-containing extractant in the extraction system is 1mM to 1000 Mm.
Further, in step a), the shape of the extraction device can be any one or combination of more than one of the following shapes: tubular, spherical, ellipsoidal, conical, cubic, regular polyhedral, irregular polyhedral, and the like.
Further, in step a), the material of the extraction device may be selected from any one of the following materials: stainless steel is made of metal, plastic or rubber, quartz, high borosilicate, ceramic and the like.
Further, in step b), UO in aqueous solution2 2+Is 0.5 to 1000 Mm;
further, in the step b), the temperature of the extraction environment is 15-100 ℃;
further, in step b), the atmosphere in the extraction environment may be selected from any one or more of the following mixed atmospheres: air, argon, helium, neon, nitrogen, oxygen, carbon dioxide, and the like.
Compared with the existing extraction separation system, the invention has the following advantages:
1) UO based on carboxyl functional ionic liquid in the invention2 2+The separation method realizes rapid separation and enrichment of the UO with higher concentration2 2+At low concentration of UO2 2+Compared with the traditional extraction method, the extraction equilibrium time of the system at 30 ℃ only needs 5min, and the extraction equilibrium can be reached only in 1min at the temperature of more than 80 ℃, so that the equilibrium time of extraction and separation is greatly shortened. Can realize higher concentration UO2 2+For higher concentrations of UO2 2+The extraction efficiency of the solution is high.
2) The carboxyl functional ionic liquid of the phosphorus-containing extractant can realize UO in one step2 2+Separation and enrichment of (1), i.e. separation of UO by extraction of the system2 2+Then, the volume of radioactive waste is effectively reduced, and UO is optimized2 2+The separation and enrichment process of (1).
3) UO based on carboxyl functional ionic liquid in the invention2 2+The separation method provides a UO enriched by extraction separation with low vapor pressure, low flammability, high radiation stability and high critical concentration of lobe elements2 2+The method has the advantages of simple process, convenient and efficient operation and the like.
UO based on carboxyl functional ionic liquid provided by the invention2 2+Separation ofThe method can quickly realize the UO with higher concentration by the carboxyl functional ionic liquid containing the phosphorus extractant2 2+The extraction separation of (2). The invention can be used for UO2 2+The method can be used for industrial extraction and separation and simultaneously can be used for UO in spent fuel aftertreatment2 2+The separation process of (1). The solution is used for separating UO in the enriched aqueous solution by preparing carboxyl functional ionic liquid solution of phosphorus-containing extractant with proper concentration2 2+。
Because of strong interaction between anions and cations, compared with the traditional volatile and flammable traditional organic solvent, the ionic liquid has excellent unique properties, such as low vapor pressure, low flammability, high radiation stability, high critical concentration of lobe elements and the like, which just makes up the defects of the traditional organic solvent. The invention combines the phosphorus-containing extractant with higher acid resistance with the carboxyl functional ionic liquid with excellent stability, and can quickly extract UO in the aqueous solution under the condition of room temperature extraction2 2+And (5) separating. The invention can be used for UO2 2+The method can be used for industrial extraction and separation and simultaneously can be used for UO in spent fuel aftertreatment2 2+The separation process is a rapid, convenient and efficient UO separation process2 2+The method has important significance for fully recycling and utilizing uranium.
Drawings
FIG. 1 shows CMPO/[ HOOCmim ]][NTf2]Rapid separation and enrichment of higher concentration UO2 2+Is described.
FIG. 2 shows CMPO/[ HOOCmim ] in example 1][NTf2]And (4) evaluating the extraction kinetics of the extraction system.
FIG. 3 shows CMPO/[ HOOCmim ] in example 2][NTf2]And (4) evaluating the extraction capability of the system.
FIG. 4 is a graph showing the evaluation of the extraction capacities of the different extraction systems of example 4.
Detailed Description
The process of the present invention is illustrated below by means of specific examples, but the present invention is not limited thereto.
The experimental methods described in the following examples are all conventional methods unless otherwise specified; the reagents and materials are commercially available, unless otherwise specified.
Example 1, CMPO/[ HOOCmim][NTf2]Evaluation of extraction kinetics of the System
a) Preparing an extraction system: weighing appropriate amount of CMPO according to the requirement of the separation system, dissolving with carboxyl functional ionic liquid, and preparing into 20mM CMPO/[ HOOCmim][NTf2]A solution;
b) an extraction separation process: seven 0.4mL aliquots of CMPO/[ HOOCmim ] were removed][NTf2]The solution is respectively placed in seven extraction devices, and 0.4mL of solution with the concentration of 2Mm (C) is added in sequence0) UO of2 2+An aqueous solution. Then placing the extraction device in a constant temperature oscillator, and respectively oscillating and extracting for 1min, 5min, 15min, 30min, 60min, 120min and 240min at 30 ℃;
c) UO in solution2 2+And (3) concentration analysis: respectively taking out the solution under different oscillation extraction time for dilution, and carrying out ICP-OES analysis on the diluted solution to obtain UO in the aqueous solution after extraction and separation under different oscillation extraction time2 2+Concentration (C)1)；
d) Calculation of separation efficiency: using the formula E ═ C0-C1)/C0x 100% calculating the extraction efficiency of the extraction system;
the extraction time is 1min, 5min, 15min, 30min, 60min, 120min, and 240min, and the extraction time is CMPO/[ HOOCmim][NTf2]The extraction efficiency of the extraction system is 57.57%, 99.78%, 99.96%, 99.989%, 99.98%, 99.993% and 99.997% respectively.
Example 2, 20mM CMPO/[ HOOCmim][NTf2]Evaluation of the extraction Capacity of the System
a) Preparing an extraction system: according to the requirements of the separation systemWeighing appropriate amount of CMPO, dissolving with carboxyl functional ionic liquid, and making into 20mM CMPO/[ HOOCmim ]][NTf2]A solution;
b) an extraction separation process: five portions of 0.4mL MPO/[ HOOCmim ] were removed][NTf2]The solution is respectively placed in five extraction devices, and 0.4mL of UO with concentration of 2mM, 5mM, 10mM, 30mM and 50mM is respectively and correspondingly added2 2+An aqueous solution. Then placing the extraction device in a constant temperature oscillator, and respectively oscillating and extracting for 240min at the temperature of 30 ℃;
c) UO in solution2 2+And (3) concentration analysis: respectively taking out the solutions in different extraction devices for dilution, and carrying out ICP-OES analysis on the diluted solutions to obtain UO in the aqueous solutions extracted and separated in the different extraction devices2 2+Concentration;
d) calculation of separation efficiency: by measuring UO in aqueous solution before and after extraction separation2 2+Concentration, using the formula E ═ C0-C1)/C0x 100% calculating the extraction efficiency of the extraction system, where C0For extracting UO from aqueous solution before separation2 2+Concentration, C1For extracting UO from separated aqueous solution2 2+Concentration;
when the extraction time is 240min, 20mM CMPO/[ HOOCmim ] is present in the different extraction apparatus of this embodiment][NTf2]The extraction system is used for respectively treating 2mM, 5mM, 10mM, 30mM and 50mM UO2 2+The extraction efficiencies of the aqueous solution were 99.997%, 99.975%, 94.15%, 76.45%, and 66.88%, respectively.
Example 3, 50mM CMPO/[ HOOCmim][NTf2]Evaluation of the extraction Capacity of the System
In accordance with the method of example 2, 50mM CMPO/[ HOOCmim ] can be obtained by adjusting the CMPO concentration in step a) from 20mM to 50mM without changing other conditions][NTf2]The extraction capacity of the system. The extraction time was 240min, 50mM CMPO/[ HOOCmim ]][NTf2]The extraction system is used for respectively treating 2mM, 5mM, 10mM, 30mM and 50mM UO2 2+The extraction efficiencies of the aqueous solutions were 99.87%, 99.995%, 100.00%, 89.78%, and 79.31%, respectively.
Example 4 evaluation of the extraction Capacity of the 100mM CMPO/[ HOOCmim ] [ NTf2] System
In accordance with the method of example 2, the concentration of CMPO in step a) was adjusted from 20mM to 100mM, and other conditions were not changed to obtain 100mM CMPO/[ HOOCmim ]][NTf2]The extraction capacity of the system. When the extraction time is 240min, 100mM CMPO/[ HOOCmim ]][NTf2]The extraction system is used for respectively treating 2mM, 5mM, 10mM, 30mM and 50mM UO2 2+The extraction efficiencies of the aqueous solution were 99.91%, 99.98%, 99.97%, 99.94%, and 91.00%, respectively.
Claims (9)
1. A uranyl ion separation method based on carboxyl functional ionic liquid is characterized by comprising the following steps:
a) preparing an extraction system: weighing a phosphorus-containing extractant, dissolving the phosphorus-containing extractant by using a carboxyl functional ionic liquid, and preparing a carboxyl functional ionic liquid solution of the phosphorus-containing extractant with a specified concentration, namely the required extraction system;
b) an extraction separation process: the UO with the concentration of C02 2+Adding the aqueous solution and the carboxyl functional ionic liquid solution containing the phosphorus extractant into an extraction device, placing the extraction device in a constant-temperature oscillation device, and carrying out extraction separation experiments under different conditions according to requirements;
c) UO in solution2 2+And (3) concentration analysis: diluting an appropriate amount of aqueous phase solution before and after extraction separation, and performing ICP-OES analysis on the diluted solution to obtain UO in the aqueous phase solution after extraction separation22+Concentration C1；
d) Calculation of separation efficiency: using the formula E ═ C0-C1)/C0x 100% calculation of the extraction System with respect to UO2 2+The extraction efficiency of (2);
2. the method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 1, wherein in the step a), the phosphorus-containing extractant is selected from any one of the following materials: N-octylphenyl-N, N' -diisobutylaminocarboxylphosphine oxide (CMPO), 1, 8-bis-diphenylphosphinoyl-2, 7-octanedione (DPPODO), bis (2, 4, 4-trimethylpentyl) phosphinic acid (Cyanex272) or tributyl phosphate (TBP).
3. The method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 1, wherein in the step a), the carboxyl functional ionic liquid is selected from any one of the following materials: 1-carboxymethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt ([ HOOCmim)][NTf2]) 1-carboxyethyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxypropyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt, 1-carboxymethyl-3-ethylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxymethyl-3-propylimidazolium bistrifluoromethylsulfonyl imide salt and the like, 1-carboxymethyl-3-butylimidazolium bistrifluoromethylsulfonyl imide salt and the like, or 1-carboxymethyl-3-pentylimidazolium bistrifluoromethylsulfonyl imide salt.
4. The method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 1, wherein in the step a), the concentration of the phosphorus-containing extractant in the extraction system is 1mM to 1000 Mm.
5. The method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 1, wherein in the step a), the shape of the extraction device can be any one or more of the following combinations: tubular, spherical, ellipsoidal, conical, cubic, regular polyhedral or irregular polyhedral.
6. The method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 5, wherein in the step a), the material of the extraction device is selected from any one of the following materials: stainless steel all metal, plastic or rubber, quartz, borosilicate, or ceramic.
7. The method for uranyl ion separation based on carboxyl functional ionic liquid according to claim 1, wherein the method comprisesCharacterized in that in step b), UO is present in the aqueous solution2 2+ at a concentration of 0.5 to 1000 Mm;
8. the method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 1, wherein in the step b), the extraction environment temperature is 15-100 ℃;
9. the method for separating uranyl ions based on a carboxyl functional ionic liquid according to claim 1, wherein in the step b), the atmosphere in the extraction environment can be selected from any one or more of the following atmospheres: air, argon, helium, neon, nitrogen, oxygen, or carbon dioxide.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
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| CN202011083076.7A CN112226635B (en) | 2020-10-12 | 2020-10-12 | Uranyl ion separation method based on carboxyl functional ionic liquid |
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| CN101638722A (en) * | 2009-08-21 | 2010-02-03 | 北京大学 | Method for extracting and separating uranyl ions from aqueous phase |
| CN103045869A (en) * | 2012-12-27 | 2013-04-17 | 北京大学 | Method for enriching uranium and thorium from water phase by using cloud point extraction technology |
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