CN115501867A - Immobilization method of functionalized amine ionic liquid for adsorbing radioactive iodine - Google Patents
Immobilization method of functionalized amine ionic liquid for adsorbing radioactive iodine Download PDFInfo
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- 239000002608 ionic liquid Substances 0.000 title claims abstract description 106
- 150000001412 amines Chemical class 0.000 title claims abstract description 85
- 230000002285 radioactive effect Effects 0.000 title claims abstract description 33
- 238000000034 method Methods 0.000 title claims abstract description 31
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 title claims abstract description 30
- 229910052740 iodine Inorganic materials 0.000 title claims abstract description 30
- 239000011630 iodine Substances 0.000 title claims abstract description 30
- 239000011148 porous material Substances 0.000 claims abstract description 47
- 238000001179 sorption measurement Methods 0.000 claims abstract description 42
- 239000000463 material Substances 0.000 claims abstract description 31
- -1 amine compound Chemical class 0.000 claims abstract description 28
- INQOMBQAUSQDDS-UHFFFAOYSA-N iodomethane Chemical compound IC INQOMBQAUSQDDS-UHFFFAOYSA-N 0.000 claims abstract description 19
- 238000005956 quaternization reaction Methods 0.000 claims abstract description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical class [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 48
- IMNIMPAHZVJRPE-UHFFFAOYSA-N triethylenediamine Chemical compound C1CN2CCN1CC2 IMNIMPAHZVJRPE-UHFFFAOYSA-N 0.000 claims description 42
- 238000001035 drying Methods 0.000 claims description 32
- VKYKSIONXSXAKP-UHFFFAOYSA-N hexamethylenetetramine Chemical compound C1N(C2)CN3CN1CN2C3 VKYKSIONXSXAKP-UHFFFAOYSA-N 0.000 claims description 20
- 238000002390 rotary evaporation Methods 0.000 claims description 16
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 15
- 239000000203 mixture Substances 0.000 claims description 15
- 238000005303 weighing Methods 0.000 claims description 15
- 239000002808 molecular sieve Substances 0.000 claims description 12
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 12
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 10
- 235000010299 hexamethylene tetramine Nutrition 0.000 claims description 10
- 239000004312 hexamethylene tetramine Substances 0.000 claims description 10
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 9
- 239000008367 deionised water Substances 0.000 claims description 7
- 229910021641 deionized water Inorganic materials 0.000 claims description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 7
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 6
- NAQMVNRVTILPCV-UHFFFAOYSA-N hexane-1,6-diamine Chemical compound NCCCCCCN NAQMVNRVTILPCV-UHFFFAOYSA-N 0.000 claims description 6
- 238000011068 loading method Methods 0.000 claims description 6
- 238000002360 preparation method Methods 0.000 claims description 6
- 239000000376 reactant Substances 0.000 claims description 6
- 239000000741 silica gel Substances 0.000 claims description 6
- 229910002027 silica gel Inorganic materials 0.000 claims description 6
- 239000006184 cosolvent Substances 0.000 claims description 5
- 238000000746 purification Methods 0.000 claims description 4
- LCFNGTOKBVGQNC-UHFFFAOYSA-N 1-azabicyclo[2.2.2]octan-4-ylmethanamine Chemical compound C1CN2CCC1(CN)CC2 LCFNGTOKBVGQNC-UHFFFAOYSA-N 0.000 claims description 3
- CEMKLAOKVLRABO-UHFFFAOYSA-N 1-azabicyclo[2.2.2]octane-4-carbonitrile Chemical compound C1CN2CCC1(C#N)CC2 CEMKLAOKVLRABO-UHFFFAOYSA-N 0.000 claims description 3
- KWYHDKDOAIKMQN-UHFFFAOYSA-N N,N,N',N'-tetramethylethylenediamine Chemical compound CN(C)CCN(C)C KWYHDKDOAIKMQN-UHFFFAOYSA-N 0.000 claims description 3
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 3
- 125000002704 decyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 claims description 3
- 125000003438 dodecyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 claims description 3
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 claims description 3
- 125000003187 heptyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 3
- 125000004051 hexyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 claims description 3
- 239000013335 mesoporous material Substances 0.000 claims description 3
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 claims description 3
- 239000012229 microporous material Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 125000001421 myristyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 3
- 125000002347 octyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 3
- 125000000913 palmityl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 3
- 125000001147 pentyl group Chemical group C(CCCC)* 0.000 claims description 3
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 3
- 230000003100 immobilizing effect Effects 0.000 claims description 2
- 125000000524 functional group Chemical group 0.000 abstract description 3
- 239000007787 solid Substances 0.000 abstract description 3
- 239000007790 solid phase Substances 0.000 abstract description 3
- 239000012071 phase Substances 0.000 abstract description 2
- 239000000047 product Substances 0.000 description 8
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical class C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 5
- 238000005576 amination reaction Methods 0.000 description 4
- NLKNQRATVPKPDG-UHFFFAOYSA-M potassium iodide Chemical compound [K+].[I-] NLKNQRATVPKPDG-UHFFFAOYSA-M 0.000 description 4
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- 238000001704 evaporation Methods 0.000 description 3
- 238000002474 experimental method Methods 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000007655 standard test method Methods 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- 239000003463 adsorbent Substances 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 239000002657 fibrous material Substances 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 125000004433 nitrogen atom Chemical group N* 0.000 description 2
- 239000012264 purified product Substances 0.000 description 2
- 239000012629 purifying agent Substances 0.000 description 2
- 239000002901 radioactive waste Substances 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- PNDPGZBMCMUPRI-HVTJNCQCSA-N 10043-66-0 Chemical compound [131I][131I] PNDPGZBMCMUPRI-HVTJNCQCSA-N 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- 239000000443 aerosol Substances 0.000 description 1
- 238000004887 air purification Methods 0.000 description 1
- 150000001449 anionic compounds Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 231100001261 hazardous Toxicity 0.000 description 1
- 229910001412 inorganic anion Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052756 noble gas Inorganic materials 0.000 description 1
- 150000002835 noble gases Chemical class 0.000 description 1
- 231100000956 nontoxicity Toxicity 0.000 description 1
- 150000002891 organic anions Chemical class 0.000 description 1
- 150000002892 organic cations Chemical class 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000002910 solid waste Substances 0.000 description 1
- 238000000967 suction filtration Methods 0.000 description 1
- 238000009423 ventilation Methods 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/30—Processes for preparing, regenerating, or reactivating
- B01J20/32—Impregnating or coating ; Solid sorbent compositions obtained from processes involving impregnating or coating
- B01J20/3231—Impregnating or coating ; Solid sorbent compositions obtained from processes involving impregnating or coating characterised by the coating or impregnating layer
- B01J20/3242—Layers with a functional group, e.g. an affinity material, a ligand, a reactant or a complexing group
- B01J20/3244—Non-macromolecular compounds
- B01J20/3246—Non-macromolecular compounds having a well defined chemical structure
- B01J20/3248—Non-macromolecular compounds having a well defined chemical structure the functional group or the linking, spacer or anchoring group as a whole comprising at least one type of heteroatom selected from a nitrogen, oxygen or sulfur, these atoms not being part of the carrier as such
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/02—Treating gases
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- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The invention relates to an immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine. The invention can immobilize the functionalized amine ionic liquid prepared by performing quaternization reaction on an amine compound and a halogenated alkyl compound with methyl iodide adsorption function on an inorganic porous material through an adsorption or medium immobilization method, thereby transferring the functional group of the functionalized amine ionic liquid to a solid carrier, and ensuring that the prepared functionalized amine ionic liquid-supported inorganic porous adsorption material has the properties of the functionalized amine ionic liquid and the inorganic porous material carrier. Moreover, the functionalized amine ionic liquid prepared by the method provided by the invention is loaded with the inorganic porous adsorption material, and the macroscopic phase of the adsorption material is a solid phase, so that the adsorption material is convenient to recover.
Description
Technical Field
The invention belongs to the technical field of nuclear air purification, and particularly relates to an immobilization method of a functional amine ionic liquid for adsorbing radioactive iodine.
Background
With the rapid development of the nuclear energy industry in China, the amount of radioactive waste generated and accumulated is more and more, and the effective control and treatment of the radioactive waste also become the key of the sustainable development of the nuclear energy. During normal operation of a nuclear reactor, a variety of gaseous fission products are released, including radioactive iodine, aerosols, noble gases, etc., (ii) isotopes of radioactive iodine 131 I、 129 I) The radioactive contaminants, which are considered to be the most hazardous, must be disposed of.
For the removal of radioactive iodine, in the current ventilation system of the nuclear power station, an iodine adsorber uses an iodine removal adsorption material obtained by dipping activated carbon by triethylene diamine (TEDA) and potassium iodide (KI) to adsorb the radioactive iodine. However, TEDA has the problems of low ignition point and volatility, and is easy to sublimate into gas at room temperature, which causes the adsorption performance of the iodine adsorber to be rapidly deteriorated and the effective service life to be reduced when the iodine adsorber is operated at a slightly high temperature, thereby causing the operation cost of nuclear facilities and the increase of the amount of solid waste. In addition, the TEDA loading of the activated carbon can cause the ignition point of the activated carbon to be reduced, and the use risk of the iodine adsorber is increased.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide an immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine, which is characterized in that the functionalized amine ionic liquid prepared by carrying out quaternary amination reaction on an amine compound and a halogenated alkyl compound with methyl iodide adsorption function is immobilized on an inorganic porous material by an adsorption or medium immobilization method,
in order to achieve the above purpose, the technical scheme adopted by the invention is as follows: an immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine, comprising the following steps:
s1, weighing a functionalized amine ionic liquid and a functionalized amine ionic liquid solvent according to a set proportion, and dissolving the functionalized amine ionic liquid in the functionalized amine ionic liquid solvent to obtain an impregnant solution; the functionalized amine ionic liquid is prepared by taking an amine compound with a methyl iodide adsorption function and a halogenated alkyl compound as reactants through a quaternization reaction;
s2, weighing an inorganic porous material according to a set proportion, and uniformly mixing the impregnant solution and the inorganic porous material to obtain a mixture of the impregnant solution and the inorganic porous material;
and S3, drying the mixture of the impregnant solution and the inorganic porous material under a set drying condition to obtain the functionalized amine ionic liquid loaded inorganic porous adsorption material.
Further, the inorganic porous material is selected from one of activated carbon, activated carbon fiber, molecular sieve and silica gel.
Further, when the inorganic porous material is selected from one of activated carbon, molecular sieve and silica gel, after the impregnant solution and the inorganic porous material are uniformly mixed, the method also comprises the step of rotary evaporation:
and (3) transferring the mixture of the impregnant solution and the inorganic porous material into a rotary evaporator for rotary evaporation, loading the functionalized amine ionic liquid on the inorganic porous material, and drying the obtained rotary evaporated sample under the drying condition set in the step S3 to obtain the functionalized amine ionic liquid loaded inorganic porous adsorption material.
Further, the temperature of the rotary evaporation step is 10-200 ℃, and the time of the rotary evaporation step is 5-72 h.
Further, the preparation method of the functionalized amine ionic liquid comprises the following steps: and carrying out quaternization reaction on the reactant dissolved by the cosolvent to obtain an initial product, and then carrying out purification and drying steps on the initial product to obtain the functionalized amine ionic liquid.
Further, the amine compound having a methyl iodide adsorption function is one selected from triethylene diamine, hexamethylenetetramine, 4-aminomethyl quinuclidine, 4-cyanoquinuclidine, N-dimethyl-p-phenylenediamine, tetramethylethylenediamine and hexamethylenediamine;
the halogenated alkyl compound is selected from one of halogenated methyl, halogenated ethyl, halogenated propyl, halogenated butyl, halogenated pentyl, halogenated hexyl, halogenated heptyl, halogenated octyl, halogenated decyl, halogenated dodecyl, halogenated tetradecyl and halogenated hexadecyl compounds.
Further, the functionalized amine ionic liquid solvent is selected from one of deionized water, ethanol, methanol and glycol.
Further, the inorganic porous material is selected from one of a microporous material, a mesoporous material or a macroporous material.
Further, the mass ratio of the functionalized amine ionic liquid to the inorganic porous material is 0.005-30: 100, respectively; the mass ratio of the functionalized amine ionic liquid solvent to the inorganic porous material is 0-100: 100.
further, the set drying conditions include: drying under vacuum condition, wherein the drying temperature is 5-200 ℃; the drying time is 8-72 h.
The invention has the following beneficial effects: by adopting the immobilization method of the functionalized amine ionic liquid for adsorbing radioactive iodine, provided by the invention, the functionalized amine ionic liquid prepared by carrying out quaternary amination reaction on an amine compound and a haloalkyl compound with a methyl iodide adsorption function can be immobilized on an inorganic porous material by an adsorption or medium immobilization method, so that a functional group of the functionalized amine ionic liquid is transferred to a solid carrier, and the prepared functionalized amine ionic liquid-supported inorganic porous adsorption material has the properties of the functionalized amine ionic liquid and the inorganic porous material carrier. Moreover, the functionalized amine ionic liquid prepared by the method provided by the invention is loaded with the inorganic porous adsorption material, and the macroscopic phase of the adsorption material is a solid phase, so that the adsorption material is convenient to recover.
Drawings
Fig. 1 is a schematic flow chart of a method for immobilizing a functionalized amine ionic liquid for adsorbing radioactive iodine according to an embodiment of the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention are further clearly and completely described below with reference to the accompanying drawings and examples, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, rather than all embodiments, and all other embodiments obtained by a person of ordinary skill in the art without any creative work based on the examples of the present invention belong to the protection scope of the present invention.
Ionic Liquids (Ionic Liquids) are composed of organic cations and polyatomic organic or inorganic anions, are in a liquid state at or near room temperature, are also called room-temperature molten salts, and have the advantages of stable physicochemical properties, difficult volatilization, adjustable structure, no toxicity, difficult combustion and explosion and the like.
In order to solve the problem that the nuclear-grade activated carbon impregnant TEDA is volatile, the inventor introduces an 'ionic liquid' concept into the preparation field of iodine-removing adsorbing materials based on a plurality of benefits of the ionic liquid: amine compounds with methyl iodide adsorption function are modified into functional amine ionic liquid through quaternization reaction, the volatility of the amine compounds is reduced on the premise of keeping the excellent iodine removal performance of the functional amine compounds, and the amine compounds are used for replacing an active iodine adsorption material impregnant TEDA. However, when the functionalized amine ionic liquid is used alone, radioactive iodine is not easy to enter the viscous functionalized amine ionic liquid to be adsorbed, and only the outer layer functionalized amine ionic liquid is utilized, so that the problems of large using amount, low utilization rate and the like of the functionalized amine ionic liquid are caused, and the single use of the functionalized amine ionic liquid in the field of iodine removal adsorption is not suggested. Therefore, the embodiment of the invention provides an immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine, which is characterized in that the functionalized amine ionic liquid is immobilized on an inorganic porous material through an adsorption or medium immobilization method, so that a functional group of the functionalized amine ionic liquid is transferred to a solid carrier, the functionalized amine ionic liquid has the properties of the functionalized amine ionic liquid and the inorganic porous material carrier, and is in a solid phase in a macroscopic view, so that the functionalized amine ionic liquid is convenient to recover.
As shown in fig. 1, in the immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to this embodiment, under a specific condition, the functionalized amine ionic liquid is supported on an inorganic porous material according to a specific ratio by an immobilization technique, and is dried to prepare a novel low-volatility iodine removal adsorbent, i.e., a functionalized amine ionic liquid-supported inorganic porous adsorbent; the method comprises the following steps:
s1, weighing a functionalized amine ionic liquid and a functionalized amine ionic liquid solvent according to a set proportion, and dissolving the functionalized amine ionic liquid in the functionalized amine ionic liquid solvent to obtain an impregnant solution;
the functionalized amine ionic liquid is prepared by taking an amine compound and a halogenated alkyl compound with methyl iodide adsorption functions as reactants through a quaternization reaction: and performing quaternization reaction on the reactant dissolved by the cosolvent to obtain an initial product, and performing purification and drying on the initial product to obtain the functionalized amine ionic liquid.
Optionally, the amine compound with methyl iodide adsorption function is selected from one of triethylene diamine (TEDA), hexamethylenetetramine (HMTA), 4-aminomethyl quinuclidine, 4-cyanoquinuclidine, N-dimethyl-p-phenylenediamine, tetramethylethylenediamine and hexamethylenediamine; the halogenated alkyl compound is selected from one of halogenated methyl, halogenated ethyl, halogenated propyl, halogenated butyl, halogenated pentyl, halogenated hexyl, halogenated heptyl, halogenated octyl, halogenated decyl, halogenated dodecyl, halogenated tetradecyl and halogenated hexadecyl compounds; the cosolvent is selected from one of ethanol and glycol.
The set molar ratio of the amine compound with methyl iodide adsorption function to the halogenated alkyl compound is 1; the reaction temperature of the quaternization reaction is 60-300 ℃, and the reaction time is 5-30 h.
The purification step comprises: dissolving the initial product by using a cosolvent to obtain an initial product solution, adding a purifying agent into the initial product solution to obtain a mixture, and performing suction filtration on the mixture for 3 times to obtain a purified product; the purifying agent is selected from one of ethanol, ethyl acetate and acetone.
The drying step comprises: and drying the purified product for 8-72 h at 30-200 ℃ under a vacuum condition to obtain the functionalized amine ionic liquid.
Optionally, the functionalized amine ionic liquid solvent is selected from one of deionized water, ethanol, methanol and ethylene glycol.
Optionally, the functionalized amine ionic liquid is a monocationic ionic liquid, that is, in the quaternary amination reaction of an amine compound and a haloalkyl compound with a methyl iodide adsorption function, a nitrogen atom in the amine compound with a methyl iodide adsorption function is converted into an ammonium ion N through a coordination bond synthesized by the quaternary amination reaction + So that the methyl iodide is converted into ionic liquid, thereby achieving the effect of reducing the volatility of the amine compound with the methyl iodide adsorption function; and the other nitrogen atom is reserved, so that the obtained monocationic ionic liquid retains the function of removing radioactive methyl iodide.
S2, weighing an inorganic porous material according to a set proportion, and uniformly mixing the impregnant solution and the inorganic porous material to obtain a mixture of the impregnant solution and the inorganic porous material;
optionally, the inorganic porous material may be selected from a microporous material (pore size less than 2 nm), a mesoporous material (pore size of 2-50 nm), or a macroporous material (pore size greater than 50 nm).
Optionally, the inorganic porous material includes, but is not limited to, activated carbon fiber, molecular sieve, silica gel.
Optionally, the set ratio includes: the mass ratio of the functionalized amine ionic liquid to the inorganic porous material is 0.005-30: 100, respectively; the mass ratio of the functionalized amine ionic liquid solvent to the inorganic porous material is (0-100): 100.
and S3, drying the mixture of the impregnant solution and the inorganic porous material under a set drying condition to obtain the functionalized amine ionic liquid loaded inorganic porous adsorption material.
Optionally, the set drying conditions include: drying under vacuum condition, wherein the drying temperature is 5-200 ℃; the drying time is 8-72 h.
Optionally, when the inorganic porous material is selected from one of activated carbon, a molecular sieve and silica gel, after the impregnant solution and the inorganic porous material are uniformly mixed, the method further comprises a rotary evaporation step: and (3) transferring the mixture of the impregnant solution and the inorganic porous material into a rotary evaporator for rotary evaporation, evaporating the functionalized amine ionic liquid solvent, loading the functionalized amine ionic liquid on the inorganic porous material, and drying the obtained rotary evaporated sample under the drying condition set in the step S3 to obtain the functionalized amine ionic liquid loaded inorganic porous adsorption material.
Optionally, the temperature of the rotary evaporation step is 10-200 ℃.
Optionally, the time of the rotary evaporation step is 5-72 h.
Example 1
The preparation method of the TEDA ionic liquid loaded activated carbon comprises the following steps:
s11, weighing 1.2g of TEDA ionic liquid by using a weighing balance, and dissolving the TEDA ionic liquid in 40g of deionized water to obtain an impregnant solution;
s12, weighing 40g of activated carbon, slowly pouring the impregnant solution into a container filled with the activated carbon, uniformly stirring, transferring the mixture of the impregnant solution and the activated carbon into a rotary evaporator, carrying out rotary evaporation for 10 hours at 90 ℃, evaporating most deionized water, and loading the TEDA ionic liquid on the activated carbon to obtain a sample subjected to rotary evaporation;
s13, standing and drying the rotary-steamed sample at 100 ℃ for 36h to obtain the TEDA ionic liquid loaded activated carbon material.
Referring to the requirements of standard radioactive iodine adsorption performance experiments of adsorption materials in the standard test method of ASTM D3803-1991 (2014) nuclear-grade activated carbon, the removal efficiency of the radioactive methyl iodide of the TEDA ionic liquid loaded activated carbon material obtained in example 1 reaches 99.97% under the conditions of 30 ℃, 40% relative humidity and 4.8m/min of material linear velocity of air flow passing through the material.
Example 2
The preparation method of the TEDA ionic liquid loaded activated carbon fiber comprises the following steps:
s21, weighing 4g of TEDA ionic liquid by using a weighing balance, and dissolving the TEDA ionic liquid in 100g of ethanol to obtain an impregnant solution;
s22, weighing 40g of activated carbon fibers, slowly pouring the impregnant solution into a container filled with the activated carbon fibers, standing for 48 hours at the temperature of 20 ℃, and fully diffusing the impregnant solution in the activated carbon fibers so as to uniformly mix the impregnant solution and the activated carbon fibers;
s23, standing and drying the mixture of the impregnant solution and the activated carbon fiber at 50 ℃ for 72 hours to obtain the TEDA ionic liquid loaded activated carbon fiber material.
Referring to the requirements of standard radioactive iodine adsorption performance experiments of adsorption materials in the standard test method of ASTM D3803-1991 (2014) nuclear-grade activated carbon, the removal efficiency of the TEDA ionic liquid loaded activated carbon fiber material obtained in example 2 on radioactive methyl iodine reaches 99.94% under the conditions of 30 ℃, 40% relative humidity and 4.8m/min of linear velocity of air flow passing through the material.
Example 3
The preparation method of the HMTA ionic liquid loaded molecular sieve comprises the following steps:
s11, weighing 12g of HMTA ionic liquid by using a weighing balance, and dissolving the HMTA ionic liquid in 150g of deionized water to obtain an impregnant solution;
s12, weighing 40g of molecular sieve, slowly pouring the impregnant solution into a container filled with the molecular sieve, uniformly stirring, transferring the mixture of the impregnant solution and the molecular sieve into a rotary evaporator, carrying out rotary evaporation for 20 hours at 70 ℃, evaporating most deionized water, and loading the HMTA ionic liquid on the molecular sieve to obtain a sample subjected to rotary evaporation;
s13, standing and drying the rotary evaporated sample at 130 ℃ for 24h to obtain the HMTA ionic liquid loaded activated carbon material.
Referring to the requirements of standard radioactive iodine adsorption performance experiments of adsorption materials in a standard test method of ASTM D3803-1991 (2014) nuclear grade activated carbon, the removal efficiency of radioactive methyl iodide of the HMTA ionic liquid loaded molecular sieve material obtained in example 3 reaches 98.99% under the conditions of 30 ℃, 40% relative humidity and 4.8m/min of gas flow passing material linear velocity.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is intended to include such modifications and variations.
Claims (10)
1. A method for immobilizing functionalized amine ionic liquid for adsorbing radioactive iodine is characterized by comprising the following steps:
s1, weighing a functionalized amine ionic liquid and a functionalized amine ionic liquid solvent according to a set proportion, and dissolving the functionalized amine ionic liquid in the functionalized amine ionic liquid solvent to obtain an impregnant solution; the functionalized amine ionic liquid is prepared by taking an amine compound with a methyl iodide adsorption function and a halogenated alkyl compound as reactants through a quaternization reaction;
s2, weighing an inorganic porous material according to a set proportion, and uniformly mixing the impregnant solution and the inorganic porous material to obtain a mixture of the impregnant solution and the inorganic porous material;
and S3, drying the mixture of the impregnant solution and the inorganic porous material under a set drying condition to obtain the functionalized amine ionic liquid loaded inorganic porous adsorption material.
2. The immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 1, wherein the inorganic porous material is selected from one of activated carbon, activated carbon fiber, molecular sieve and silica gel.
3. The immobilization method of the functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 2, wherein when the inorganic porous material is selected from one of activated carbon, molecular sieve and silica gel, after the impregnant solution is uniformly mixed with the inorganic porous material, the immobilization method further comprises a rotary evaporation step:
and (3) transferring the mixture of the impregnant solution and the inorganic porous material into a rotary evaporator for rotary evaporation, loading the functionalized amine ionic liquid on the inorganic porous material, and drying the obtained rotary evaporated sample under the drying condition set in the step S3 to obtain the functionalized amine ionic liquid loaded inorganic porous adsorption material.
4. The immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 3, wherein the rotary evaporation temperature is 10-200 ℃ and the rotary evaporation time is 5-72 h.
5. The immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 1, wherein the preparation method of the functionalized amine ionic liquid comprises: and carrying out quaternization reaction on the reactant dissolved by the cosolvent to obtain an initial product, and then carrying out purification and drying steps on the initial product to obtain the functionalized amine ionic liquid.
6. The immobilization method of a functionalized amine ionic liquid for absorbing radioactive iodine according to claim 1, wherein the amine compound having a methyl iodide adsorption function is one selected from triethylene diamine, hexamethylenetetramine, 4-aminomethyl quinuclidine, 4-cyanoquinuclidine, N-dimethyl-p-phenylenediamine, tetramethylethylenediamine and hexamethylenediamine;
the halogenated alkyl compound is selected from one of halogenated methyl, halogenated ethyl, halogenated propyl, halogenated butyl, halogenated pentyl, halogenated hexyl, halogenated heptyl, halogenated octyl, halogenated decyl, halogenated dodecyl, halogenated tetradecyl and halogenated hexadecyl compounds.
7. The immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 1, wherein the functionalized amine ionic liquid solvent is one selected from deionized water, ethanol, methanol and ethylene glycol.
8. The immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 1, wherein the inorganic porous material is selected from one of a microporous material, a mesoporous material and a macroporous material.
9. The immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to claim 1, wherein the set ratio comprises: the mass ratio of the functionalized amine ionic liquid to the inorganic porous material is (0.005-30): 100; the mass ratio of the functionalized amine ionic liquid solvent to the inorganic porous material is 0-100: 100.
10. the immobilization method of a functionalized amine ionic liquid for adsorbing radioactive iodine according to any one of claims 1 to 9, wherein the set drying conditions comprise: drying under vacuum condition, wherein the drying temperature is 5-200 ℃; the drying time is 8-72 h.
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| CN110681356A (en) * | 2019-10-15 | 2020-01-14 | 符瞰 | Preparation method of novel radioactive waste gas adsorption material and iodine adsorption application thereof |
| CN111389370A (en) * | 2020-03-20 | 2020-07-10 | 中国辐射防护研究院 | Preparation method of nuclear-grade activated carbon loaded with ionic liquid |
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| CN110681356A (en) * | 2019-10-15 | 2020-01-14 | 符瞰 | Preparation method of novel radioactive waste gas adsorption material and iodine adsorption application thereof |
| CN111389370A (en) * | 2020-03-20 | 2020-07-10 | 中国辐射防护研究院 | Preparation method of nuclear-grade activated carbon loaded with ionic liquid |
| CN114432736A (en) * | 2022-01-06 | 2022-05-06 | 辽宁大学 | Application of hydroxyl functional ionic liquid in iodine extraction |
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