CN117987211A - Radioactive decontamination foam-based eutectic solvent and preparation method and application thereof - Google Patents
Radioactive decontamination foam-based eutectic solvent and preparation method and application thereof Download PDFInfo
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- CN117987211A CN117987211A CN202410148804.XA CN202410148804A CN117987211A CN 117987211 A CN117987211 A CN 117987211A CN 202410148804 A CN202410148804 A CN 202410148804A CN 117987211 A CN117987211 A CN 117987211A
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- China
- Prior art keywords
- foam
- eutectic solvent
- hydrogen bond
- acid
- based eutectic
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- 239000006260 foam Substances 0.000 title claims abstract description 85
- 230000005496 eutectics Effects 0.000 title claims abstract description 69
- 239000002904 solvent Substances 0.000 title claims abstract description 69
- 238000005202 decontamination Methods 0.000 title claims abstract description 32
- 230000003588 decontaminative effect Effects 0.000 title claims abstract description 32
- 230000002285 radioactive effect Effects 0.000 title claims abstract description 31
- 238000002360 preparation method Methods 0.000 title abstract description 5
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 36
- 239000001257 hydrogen Substances 0.000 claims abstract description 36
- 125000000217 alkyl group Chemical group 0.000 claims abstract description 10
- 125000001424 substituent group Chemical group 0.000 claims abstract description 9
- 125000003118 aryl group Chemical group 0.000 claims abstract description 5
- 125000000753 cycloalkyl group Chemical group 0.000 claims abstract description 5
- 230000007935 neutral effect Effects 0.000 claims abstract description 5
- 150000007513 acids Chemical group 0.000 claims abstract description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical group [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 3
- 150000001875 compounds Chemical class 0.000 claims abstract description 3
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 3
- 239000001301 oxygen Substances 0.000 claims abstract description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 24
- 238000002156 mixing Methods 0.000 claims description 21
- 239000003945 anionic surfactant Substances 0.000 claims description 16
- 229910001220 stainless steel Inorganic materials 0.000 claims description 16
- 239000010935 stainless steel Substances 0.000 claims description 16
- 239000000370 acceptor Substances 0.000 claims description 15
- 239000004480 active ingredient Substances 0.000 claims description 7
- 239000002253 acid Substances 0.000 claims description 6
- GHVNFZFCNZKVNT-UHFFFAOYSA-N decanoic acid Chemical compound CCCCCCCCCC(O)=O GHVNFZFCNZKVNT-UHFFFAOYSA-N 0.000 claims description 6
- 239000000463 material Substances 0.000 claims description 6
- 238000000034 method Methods 0.000 claims description 6
- 239000004094 surface-active agent Substances 0.000 claims description 6
- 229920000742 Cotton Polymers 0.000 claims description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 4
- 229910052782 aluminium Inorganic materials 0.000 claims description 4
- 239000002280 amphoteric surfactant Substances 0.000 claims description 4
- 239000003093 cationic surfactant Substances 0.000 claims description 4
- 239000002736 nonionic surfactant Substances 0.000 claims description 4
- 239000002861 polymer material Substances 0.000 claims description 4
- 239000012209 synthetic fiber Substances 0.000 claims description 4
- 229920002994 synthetic fiber Polymers 0.000 claims description 4
- 150000001408 amides Chemical class 0.000 claims description 3
- SRSXLGNVWSONIS-UHFFFAOYSA-N benzenesulfonic acid Chemical compound OS(=O)(=O)C1=CC=CC=C1 SRSXLGNVWSONIS-UHFFFAOYSA-N 0.000 claims description 3
- RVAUVEOTZNLMQL-UHFFFAOYSA-N cyclohexanesulfinic acid Chemical compound OS(=O)C1CCCCC1 RVAUVEOTZNLMQL-UHFFFAOYSA-N 0.000 claims description 3
- 239000002023 wood Substances 0.000 claims description 3
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 claims description 2
- 229910052695 Americium Inorganic materials 0.000 claims description 2
- LSNNMFCWUKXFEE-UHFFFAOYSA-M Bisulfite Chemical compound OS([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-M 0.000 claims description 2
- 229910052685 Curium Inorganic materials 0.000 claims description 2
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical group COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 claims description 2
- 229910052781 Neptunium Inorganic materials 0.000 claims description 2
- 229910019142 PO4 Inorganic materials 0.000 claims description 2
- ABLZXFCXXLZCGV-UHFFFAOYSA-N Phosphorous acid Chemical compound OP(O)=O ABLZXFCXXLZCGV-UHFFFAOYSA-N 0.000 claims description 2
- 229910052778 Plutonium Inorganic materials 0.000 claims description 2
- 229910052776 Thorium Inorganic materials 0.000 claims description 2
- 229910052770 Uranium Inorganic materials 0.000 claims description 2
- LXQXZNRPTYVCNG-UHFFFAOYSA-N americium atom Chemical compound [Am] LXQXZNRPTYVCNG-UHFFFAOYSA-N 0.000 claims description 2
- ZLMKQJQJURXYLC-UHFFFAOYSA-N bis(2-ethylhexoxy)-oxophosphanium Chemical compound CCCCC(CC)CO[P+](=O)OCC(CC)CCCC ZLMKQJQJURXYLC-UHFFFAOYSA-N 0.000 claims description 2
- 229910052792 caesium Inorganic materials 0.000 claims description 2
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 claims description 2
- 150000001735 carboxylic acids Chemical class 0.000 claims description 2
- 150000002576 ketones Chemical class 0.000 claims description 2
- 229910052747 lanthanoid Inorganic materials 0.000 claims description 2
- 150000002602 lanthanoids Chemical class 0.000 claims description 2
- 239000003446 ligand Substances 0.000 claims description 2
- LFNLGNPSGWYGGD-UHFFFAOYSA-N neptunium atom Chemical compound [Np] LFNLGNPSGWYGGD-UHFFFAOYSA-N 0.000 claims description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 2
- 239000010452 phosphate Substances 0.000 claims description 2
- 150000003003 phosphines Chemical class 0.000 claims description 2
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 claims description 2
- 229910052712 strontium Inorganic materials 0.000 claims description 2
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 2
- BUUPQKDIAURBJP-UHFFFAOYSA-N sulfinic acid Chemical compound OS=O BUUPQKDIAURBJP-UHFFFAOYSA-N 0.000 claims description 2
- 229910052713 technetium Inorganic materials 0.000 claims description 2
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 claims description 2
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 claims description 2
- ZMBHCYHQLYEYDV-UHFFFAOYSA-N trioctylphosphine oxide Chemical compound CCCCCCCCP(=O)(CCCCCCCC)CCCCCCCC ZMBHCYHQLYEYDV-UHFFFAOYSA-N 0.000 claims description 2
- 150000002170 ethers Chemical class 0.000 claims 1
- 239000007921 spray Substances 0.000 claims 1
- DNYWZCXLKNTFFI-UHFFFAOYSA-N uranium Chemical compound [U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U][U] DNYWZCXLKNTFFI-UHFFFAOYSA-N 0.000 claims 1
- 239000003599 detergent Substances 0.000 description 26
- 239000002689 soil Substances 0.000 description 19
- BYKRNSHANADUFY-UHFFFAOYSA-M sodium octanoate Chemical compound [Na+].CCCCCCCC([O-])=O BYKRNSHANADUFY-UHFFFAOYSA-M 0.000 description 14
- 230000000052 comparative effect Effects 0.000 description 10
- 238000001816 cooling Methods 0.000 description 8
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 6
- SEGLCEQVOFDUPX-UHFFFAOYSA-N di-(2-ethylhexyl)phosphoric acid Chemical compound CCCCC(CC)COP(O)(=O)OCC(CC)CCCC SEGLCEQVOFDUPX-UHFFFAOYSA-N 0.000 description 5
- -1 hydrogen ions Chemical class 0.000 description 5
- 238000009390 chemical decontamination Methods 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 238000005507 spraying Methods 0.000 description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 150000001413 amino acids Chemical class 0.000 description 2
- 125000004429 atom Chemical group 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 239000004744 fabric Substances 0.000 description 2
- 125000000740 n-pentyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 2
- 239000002915 spent fuel radioactive waste Substances 0.000 description 2
- QQZOPKMRPOGIEB-UHFFFAOYSA-N 2-Oxohexane Chemical compound CCCCC(C)=O QQZOPKMRPOGIEB-UHFFFAOYSA-N 0.000 description 1
- JJJOZVFVARQUJV-UHFFFAOYSA-N 2-ethylhexylphosphonic acid Chemical compound CCCCC(CC)CP(O)(O)=O JJJOZVFVARQUJV-UHFFFAOYSA-N 0.000 description 1
- HZIUHEQKVCPTAJ-UHFFFAOYSA-N 3-(2-ethylhexoxyphosphonoyloxymethyl)heptane Chemical compound CCCCC(CC)COP(=O)OCC(CC)CCCC HZIUHEQKVCPTAJ-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000003749 cleanliness Effects 0.000 description 1
- 238000010668 complexation reaction Methods 0.000 description 1
- 239000008139 complexing agent Substances 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000010494 dissociation reaction Methods 0.000 description 1
- 230000005593 dissociations Effects 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000374 eutectic mixture Substances 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000009392 mechanical decontamination Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003758 nuclear fuel Substances 0.000 description 1
- 239000013110 organic ligand Substances 0.000 description 1
- 230000033116 oxidation-reduction process Effects 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 238000003904 radioactive pollution Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 239000002265 redox agent Substances 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000001360 synchronised effect Effects 0.000 description 1
- RMZAYIKUYWXQPB-UHFFFAOYSA-N trioctylphosphane Chemical compound CCCCCCCCP(CCCCCCCC)CCCCCCCC RMZAYIKUYWXQPB-UHFFFAOYSA-N 0.000 description 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
-
- 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
- G21F9/04—Treating liquids
- G21F9/06—Processing
- G21F9/12—Processing by absorption; by adsorption; by ion-exchange
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D1/00—Detergent compositions based essentially on surface-active compounds; Use of these compounds as a detergent
- C11D1/02—Anionic compounds
- C11D1/04—Carboxylic acids or salts thereof
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D17/00—Detergent materials or soaps characterised by their shape or physical properties
- C11D17/0008—Detergent materials or soaps characterised by their shape or physical properties aqueous liquid non soap compositions
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/20—Organic compounds containing oxygen
- C11D3/2072—Aldehydes-ketones
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/20—Organic compounds containing oxygen
- C11D3/2075—Carboxylic acids-salts thereof
- C11D3/2079—Monocarboxylic acids-salts thereof
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/26—Organic compounds containing nitrogen
- C11D3/32—Amides; Substituted amides
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/34—Organic compounds containing sulfur
- C11D3/3409—Alkyl -, alkenyl -, cycloalkyl - or terpene sulfates or sulfonates
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/34—Organic compounds containing sulfur
- C11D3/3418—Toluene -, xylene -, cumene -, benzene - or naphthalene sulfonates or sulfates
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/36—Organic compounds containing phosphorus
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/16—Organic compounds
- C11D3/36—Organic compounds containing phosphorus
- C11D3/362—Phosphates or phosphites
-
- C—CHEMISTRY; METALLURGY
- C11—ANIMAL OR VEGETABLE OILS, FATS, FATTY SUBSTANCES OR WAXES; FATTY ACIDS THEREFROM; DETERGENTS; CANDLES
- C11D—DETERGENT COMPOSITIONS; USE OF SINGLE SUBSTANCES AS DETERGENTS; SOAP OR SOAP-MAKING; RESIN SOAPS; RECOVERY OF GLYCEROL
- C11D3/00—Other compounding ingredients of detergent compositions covered in group C11D1/00
- C11D3/43—Solvents
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Wood Science & Technology (AREA)
- Life Sciences & Earth Sciences (AREA)
- Health & Medical Sciences (AREA)
- Emergency Medicine (AREA)
- Physics & Mathematics (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Detergent Compositions (AREA)
Abstract
The invention provides a radioactive decontamination foam-based eutectic solvent, a preparation method and application thereof, wherein the eutectic solvent comprises a hydrogen bond donor and a hydrogen bond acceptor; the hydrogen bond donor is an acidic compound with a specific substituent, the hydrogen bond acceptor is an oxygen coordination neutral compound with a specific substituent, and the specific substituent is a symmetrical or asymmetrical straight-chain alkyl, branched-chain alkyl, cycloalkyl or aryl with 1-16C atoms. The foam-based eutectic solvent of the invention can realize high-efficiency decontamination of various radionuclides under a broad-spectrum condition.
Description
Technical Field
The invention belongs to the technical fields of nuclear facility retirement, nuclear waste treatment and disposal, and relates to a radioactive decontamination foam-based eutectic solvent, a preparation method and application thereof.
Background
Nuclear energy is a strategic energy source with continuous stability, cleanliness and high energy density, and the development of the nuclear energy source has important significance for energy safety guarantee. However, nuclear fuel and spent fuel formed after use are radioactive, and leakage can cause great harm to the natural environment. In order to ensure ecological health development and safe utilization of nuclear energy, it is necessary to perform effective decontamination treatment on radioactive contaminated equipment during retirement of nuclear facilities. In recent years, a large number of nuclear reactors in various countries of the world enter retirement, resulting in a large increase in the demand for radioactive decontamination work in the nuclear power industry.
Radioactive decontamination mainly comprises methods of mechanical decontamination, chemical decontamination, physical decontamination and the like. The chemical decontamination is to remove the radionuclide on the surface by utilizing the actions of dissolution, oxidation reduction, complexation, passivation, surface infiltration and the like of chemical reagents, has various irreplaceable advantages, and is widely applied in decontamination industry. Chemical decontamination products consist essentially of a carrier and a decontamination active ingredient. Wherein, the carrier can contain or carry the decontamination active ingredient, support and assist decontamination. Common carriers mainly comprise foam, film body and the like, and various commercial products are available at present. The detergent active ingredients are combined with radionuclides through chemical action, are usually prepared by mixing complexing agents, redox agents and the like, and are the key content of the research and development of various detergents currently. Because the radiation dose of spent fuel is extremely high and the nuclides with long-term radioactivity are numerous, the high requirements on decontamination active ingredients are put forward in the aspects of decontamination efficiency, decontamination nuclide types and the like. The development of novel highly effective and broad spectrum detergent actives is a key tool to the decommissioning of nuclear facilities.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a radioactive decontamination foam-based eutectic solvent, and a preparation method and application thereof. The foam-based eutectic solvent of the invention can realize high-efficiency decontamination of various radionuclides under a broad-spectrum condition.
To achieve the purpose, the invention adopts the following technical scheme:
In one aspect, the present invention provides a radioactive detersive foam-based eutectic solvent comprising a eutectic solvent and a foam carrier, the eutectic solvent comprising a hydrogen bond donor and a hydrogen bond acceptor; the hydrogen bond donor is an acidic compound having a specific substituent, and the hydrogen bond acceptor is an oxygen coordination neutral compound having a specific substituent, and the specific substituent is a symmetrical or asymmetrical linear alkyl, branched alkyl, cycloalkyl or aryl group having 1 to 16 (e.g., 1,2, 4, 6, 8, 10, 12, 14 or 16) C atoms.
The eutectic solvent of the present invention is a two-component or three-component eutectic mixture of a combination of hydrogen bond acceptors and hydrogen bond donors. Because the hydrogen bond donor/hydrogen bond acceptor molecules are selected and combined in a very rich way, the combination of a plurality of nuclides is hopefully realized through the targeted design of the eutectic solvent, and the efficient decontamination of radioactive pollution nuclear facilities is further promoted.
Preferably, the hydrogen bond donor is selected from any one or a combination of at least two of phosphonic acid, dithiophosphinic acid, organic carboxylic acid, organic sulfonic acid or organic sulfinic acid.
In the present invention, the hydrogen bond donor has the following structural formula:
r may be a symmetrical or asymmetrical straight chain alkyl, branched alkyl, cycloalkyl or aryl group having 1 to 16C atoms.
Preferably, the hydrogen bond donor is selected from any one or a combination of at least two of bis (2-ethylhexyl) phosphonic acid, bis (2, 4-trimethylpentyl) dithiophosphinic acid, n-decanoic acid, phenylsulfonic acid or cyclohexylsulfinic acid.
Preferably, the hydrogen bond acceptor is selected from any one or a combination of at least two of ketone, amide clamp ether, neutral phosphines or phosphate ligands.
In the present invention, the hydrogen bond acceptor has the following structural formula:
r may be a symmetrical or asymmetrical straight chain alkyl, branched alkyl, cycloalkyl or aryl group having 1 to 16C atoms.
Preferably, the hydrogen bond acceptor is selected from any one or a combination of at least two of tetra-N-octyl diamide clip ether, methyl butyl ketone, N-dibutyl-hexadecyl monoamide, trioctylphosphine oxide or tributyl phosphate.
Preferably, the molar ratio of the hydrogen bond donor to the hydrogen bond acceptor may be in the range of 1:10 to 10:1, for example 1:10, 1:9, 1:8, 1:7, 1:6, 1:5, 1:4, 1:3, 1:2, 1:1, 2:1, 3:1, 4:1, 5:1, 6:1, 7:1, 8:1, 9:1 or 10:1.
Preferably, the foam carrier is formed by mixing a surfactant with water.
In the present invention, the surfactant may be an anionic surfactant, a cationic surfactant, an amphoteric surfactant, or a nonionic surfactant.
Preferably, the volume ratio of surfactant to water may be 1:10-10:1, for example 1:10, 1:9, 1:8, 1:7, 1:6, 1:5, 1:4, 1:3, 1:2, 1:1, 2:1, 3:1, 4:1, 5:1, 6:1, 7:1, 8:1, 9:1 or 10:1.
Preferably, the volume ratio of eutectic solvent to foam carrier is 1:10-10:1, e.g., 1:10, 1:9, 1:8, 1:7, 1:6, 1:5, 1:4, 1:3, 1:2, 1:1, 2:1, 3:1, 4:1, 5:1, 6:1, 7:1, 8:1, 9:1, or 10:1.
In another aspect, the present invention provides a method for preparing the radioactive decontamination foam-based eutectic solvent as described above, the method comprising the steps of:
(1) Mixing a hydrogen bond donor and a hydrogen bond acceptor to obtain a eutectic solvent which is used as a radioactive decontamination active ingredient;
(2) And mixing the eutectic solvent with a foam carrier to obtain the radioactive decontamination foam-based eutectic solvent.
In another aspect, the present invention provides the use of a radiodecontaminating foam-based eutectic solvent as described above as a radionuclide decontaminant.
Preferably, the application is spraying the radioactive decontamination foam-based eutectic solvent on the radioactive contamination surface, and wiping the surface after standing, so that efficient decontamination of various radionuclides under a broad spectrum of conditions can be realized.
Preferably, the rest time may be 1-60 minutes, for example 1 minute, 5 minutes, 10 minutes, 15 minutes, 20 minutes, 25 minutes, 30 minutes, 35 minutes, 40 minutes, 45 minutes, 50 minutes, 55 minutes or 60 minutes.
Preferably, the material of the contaminated surface can be stainless steel, aluminum, wood or high polymer material.
Preferably, the acidity of the contaminated surface may be any acidity in the range of pH 14-pH 1 (e.g., pH14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, or 1) and 0.1-14mol/L (e.g., 0.1mol/L, 0.5mol/L, 1mol/L, 3mol/L, 5mol/L, 8mol/L, 10mol/L, 12mol/L, or 14 mol/L) H +.
Preferably, the wiping material used for the wiping surface can be paper, cotton or synthetic fiber.
Preferably, the radionuclide is a radionuclide of valency I-VII.
Preferably, the radionuclide is one or a combination of at least two of cesium (Cs (I)), strontium (Sr (II)), americium (Am (III)), curium (Cm (III)), lanthanide (Ln (III)), thorium (Th (IV)), plutonium (Pu (IV)), neptunium (Np (V)), uranium (U (VI)) or technetium (Tc (VII)).
Compared with the prior art, the invention has the following beneficial effects:
The foam-based eutectic solvent is used as a detergent, promotes dissociation of hydrogen ions of acidic compounds through hydrogen bonding, and can realize efficient decontamination of radionuclides in all acidity ranges. The eutectic solvent as an active ingredient of the detergent is composed of two or more organic ligands, so that synchronous decontamination of various radionuclides under a broad spectrum of conditions can be achieved.
Detailed Description
The technical scheme of the invention is further described by the following specific embodiments. It will be apparent to those skilled in the art that the examples are merely to aid in understanding the invention and are not to be construed as a specific limitation thereof.
The experimental methods described in the following examples are all conventional methods unless otherwise specified; the reagents and materials, unless otherwise specified, are commercially available.
Example 1:
The molar ratio was set to 1:1 with di (2-ethylhexyl) phosphoric acid, and preparing the tetra-n-octyl diamide clamp ether-di (2-ethylhexyl) phosphoric acid eutectic solvent by a heating-cooling method. The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:1 to prepare the foam-based eutectic solvent type radioactive detergent 1. Detergent 1 was sprayed on a stainless steel surface contaminated with Cs (I) at pH 3 and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 95%.
Example 2:
The molar ratio was set to 1:1 with di (2-ethylhexyl) phosphonic acid, and preparing the tetra-n-octyl diamide clamp ether-di (2-ethylhexyl) phosphonic acid eutectic solvent by a heating-cooling method. The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:1 to prepare the foam-based eutectic solvent type radioactive detergent 2. Detergent 2 was sprayed on a stainless steel surface contaminated with Sr (II) at pH 1 and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 98%.
Example 3:
The molar ratio was set to 1:5, mixing methyl butyl ketone and di (2, 4-trimethyl amyl) dithiophosphinic acid, and preparing the methyl butyl ketone-di (2, 4-trimethyl amyl) dithiophosphinic acid eutectic solvent by a dissolution-evaporation method. Mixing the isooctylamine hydrochloride serving as a cationic surfactant with water according to the following formula 1:5 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:5, and preparing the foam-based eutectic solvent type radioactive detergent 3. Detergent 3 was sprayed on an aluminum material surface having a pH of 14 and contaminated with Am (III), and allowed to stand for 1 minute. The surface was then wiped with cotton cloth and the surface soil release rate tested reached 99%.
Example 4:
The molar ratio was set to 1:10, N-dibutyl-hexadecyl monoamide is mixed with N-capric acid, and the N, N-dibutyl-hexadecyl monoamide-N-capric acid eutectic solvent is prepared by an ultrasonic method. The amphoteric surfactant amino acid is mixed with water according to a ratio of 1:10 by volume, to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:10 by volume ratio to prepare the foam-based eutectic solvent type radioactive detergent 4. Detergent 4 was sprayed on the woody surface at pH 5 and contaminated with Cm (III) and allowed to stand for 30 minutes. And then the surface is wiped by adopting synthetic fiber, and the decontamination rate of the tested surface reaches 99 percent.
Example 5:
The molar ratio was set to 5:1 with phenylsulfonic acid, and preparing the trioctylphosphine oxide-phenylsulfonic acid eutectic solvent by a heating-cooling method. Mixing the nonionic surfactant glycerol and water according to a ratio of 5:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to a ratio of 5:1, and preparing the foam-based eutectic solvent type radioactive detergent 5. Spraying the detergent 5 on the surface of the high polymer material which is 1mol/LH + and is polluted by Ln (III), and standing for 60 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 99%.
Example 6:
The molar ratio was set to 10:1 is mixed with the cyclohexylsulfinic acid, and the tributyl phosphate-cyclohexylsulfinic acid eutectic solvent is prepared by a heating-cooling method. The anionic surfactant sodium octoate is mixed with water according to a ratio of 10:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and a foam carrier according to a ratio of 10:1, and preparing the foam-based eutectic solvent type radioactive detergent 6. Detergent 6 was sprayed on a stainless steel surface contaminated with Th (IV) at 5mol/L H + and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 100%.
Example 7:
The molar ratio was set to 1:1 with di (2-ethylhexyl) phosphoric acid, and preparing the tetra-n-octyl diamide clamp ether-di (2-ethylhexyl) phosphoric acid eutectic solvent by a heating-cooling method. The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:1, and preparing the foam-based eutectic solvent type radioactive detergent 7. Detergent 7 was sprayed onto a stainless steel surface contaminated with Pu (IV) at 14mol/L H + and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 100%.
Example 8:
The molar ratio was set to 1:1 with di (2-ethylhexyl) phosphoric acid, and preparing the tetra-n-octyl diamide clamp ether-di (2-ethylhexyl) phosphoric acid eutectic solvent by a heating-cooling method. The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:1, and preparing the foam-based eutectic solvent type radioactive detergent 8. Detergent 8 was sprayed on a stainless steel surface contaminated with Np (V) at pH 1 and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 77%.
Example 9:
The molar ratio was set to 1:1 with di (2-ethylhexyl) phosphoric acid, and preparing the tetra-n-octyl diamide clamp ether-di (2-ethylhexyl) phosphoric acid eutectic solvent by a heating-cooling method. The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:1, and preparing the foam-based eutectic solvent type radioactive detergent 9. Detergent 9 was sprayed on the stainless steel surface contaminated with U (VI) at pH 1 and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 100%.
Example 10:
The molar ratio was set to 1:1 with di (2-ethylhexyl) phosphoric acid, and preparing the tetra-n-octyl diamide clamp ether-di (2-ethylhexyl) phosphoric acid eutectic solvent by a heating-cooling method. The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume ratio to form a foam carrier. Mixing the eutectic solvent and the foam carrier according to the following ratio of 1:1, and preparing the foam-based eutectic solvent type radioactive detergent 10. The detergent 10 was sprayed on a stainless steel surface having a pH of 1 and contaminated with Tc (VII), and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 97%.
Comparative example 1:
the anionic surfactant sodium octoate was mixed with water according to 1:1 by volume, and forming foam. The foam was sprayed onto a stainless steel surface at pH 3 and contaminated with Cs (I) and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 7%.
Comparative example 2:
The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume, and forming foam. The foam was sprayed onto a stainless steel surface having a pH of 1 and being contaminated with Sr (II), and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 12%.
Comparative example 3:
mixing the isooctylamine hydrochloride serving as a cationic surfactant with water according to the following formula 1:5 by volume, and forming foam. The foam was sprayed onto an aluminum surface of pH 14 and contaminated with Am (III) and allowed to stand for 1 minute. The surface was then rubbed with cotton cloth and the surface soil release rate was tested to 23%.
Comparative example 4:
The amphoteric surfactant amino acid is mixed with water according to a ratio of 1:10 by volume, and forming a foam. Foam was sprayed on the wood surface at pH 5 and contaminated with Cm (III) and allowed to stand for 30 minutes. The surface was then wiped with synthetic fibers and the surface was tested for soil release up to 24%.
Comparative example 5:
mixing the nonionic surfactant glycerol and water according to a ratio of 5:1 by volume, and forming foam. Spraying the foam on the surface of the high polymer material which is 1mol/L H + and polluted by Ln (III), and standing for 60 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 20%.
Comparative example 6:
The anionic surfactant sodium octoate is mixed with water according to a ratio of 10:1 by volume, and forming foam. The foam was sprayed on a stainless steel surface contaminated with Th (IV) at 5mol/L H + and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 32%.
Comparative example 7:
The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume, and forming foam. The foam was sprayed onto a stainless steel surface of 14mol/L H + and contaminated with Pu (IV) and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 33%.
Comparative example 8:
The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume, and forming foam. Foam was sprayed on a stainless steel surface having a pH of 1 and contaminated with Np (V) and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface was tested for a soil release rate of 11%.
Comparative example 9:
The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume, and forming foam. The foam was sprayed onto a stainless steel surface having a pH of 1 and contaminated with U (VI) and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 22%.
Comparative example 10:
The anionic surfactant sodium octoate was mixed with water according to 1:1 by volume, and forming foam. The foam was sprayed onto a stainless steel surface having a pH of 1 and contaminated with Tc (VII) and allowed to stand for 10 minutes. The surface was then wiped with paper and the surface soil release rate tested reached 23%.
Table 1 comparison of detergent and foam stain removal effect
The applicant states that the present invention is illustrated by the above examples as well as the method of preparing and using the same, but the invention is not limited to, i.e. it is not meant that the invention must be practiced in dependence upon the above examples. It should be apparent to those skilled in the art that any modification of the present invention, equivalent substitution of raw materials for the product of the present invention, addition of auxiliary components, selection of specific modes, etc., falls within the scope of the present invention and the scope of disclosure.
Claims (10)
1. A radioactive decontamination foam-based eutectic solvent, wherein the radioactive decontamination foam-based eutectic solvent comprises a eutectic solvent and a foam carrier, the eutectic solvent comprising a hydrogen bond donor and a hydrogen bond acceptor; the hydrogen bond donor is an acidic compound with a specific substituent, the hydrogen bond acceptor is an oxygen coordination neutral compound with a specific substituent, and the specific substituent is a symmetrical or asymmetrical straight-chain alkyl, branched-chain alkyl, cycloalkyl or aryl with 1-16C atoms.
2. The radiodecontaminating foam-based eutectic solvent of claim 1, wherein the hydrogen bond donor is selected from any one or a combination of at least two of phosphonic acid, dithiophosphinic acid, organic carboxylic acid, organic sulfonic acid, or organic sulfinic acid.
3. The radiodecontaminating foam-based eutectic solvent of claim 1 or 2, wherein the hydrogen bond donor is selected from any one or a combination of at least two of bis (2-ethylhexyl) phosphonic acid, bis (2, 4-trimethylpentyl) dithiophosphinic acid, n-decanoic acid, phenylsulfonic acid, or cyclohexylsulfinic acid.
4. A radiodecontamination foam-based eutectic solvent according to any one of claims 1-3, wherein the hydrogen bond acceptors are selected from any one or a combination of at least two of ketones, amides, amide clamp ethers, neutral phosphines or phosphate ligands;
preferably, the hydrogen bond acceptor is selected from any one or a combination of at least two of tetra-N-octyl diamide clip ether, methyl butyl ketone, N-dibutyl-hexadecyl monoamide, trioctylphosphine oxide or tributyl phosphate.
5. The radiodecontaminating foam-based eutectic solvent of any of claims 1-4, wherein the molar ratio of hydrogen bond donor to hydrogen bond acceptor can be in the range of 1:10-10:1.
6. The radiodecontamination foam-based eutectic solvent of any one of claims 1-5, wherein the foam carrier is formed from a surfactant mixed with water;
Preferably, the surfactant may be an anionic surfactant, a cationic surfactant, an amphoteric surfactant or a nonionic surfactant;
preferably, the volume ratio of the surfactant to water may be in the range 1:10 to 10:1.
7. The radiodecontaminating foam-based eutectic solvent of any of claims 1-6, wherein the volume ratio of the eutectic solvent to foam carrier is 1:10-10:1.
8. The method of preparing a radioactively decontaminating foam-based eutectic solvent according to any of claims 1-7, comprising the steps of:
(1) Mixing a hydrogen bond donor and a hydrogen bond acceptor to obtain a eutectic solvent which is used as a radioactive decontamination active ingredient;
(2) And mixing the eutectic solvent with a foam carrier to obtain the radioactive decontamination foam-based eutectic solvent.
9. Use of the radiodecontaminating foam-based eutectic solvent according to any of claims 1-7 as a radionuclide decontaminant.
10. The use according to claim 9, wherein the use is to spray the radioactive decontamination foam-based eutectic solvent onto the radioactive contaminated surface, and to wipe the surface after standing;
preferably, the rest time may be 1 to 60 minutes;
preferably, the material of the polluted surface can be stainless steel, aluminum, wood or high polymer material;
Preferably, the acidity of the contaminated surface may be any acidity in the range of pH 14-pH 1 and 0.1-14mol/L H +;
Preferably, the material of the wiper used for wiping the surface can be paper, cotton or synthetic fiber;
preferably, the radionuclide is a radionuclide of valency I-VII;
preferably, the radionuclide is one or a combination of at least two of cesium, strontium, americium, curium, lanthanide, thorium, plutonium, neptunium, uranium or technetium.
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