CN102631843A - Preparation method of ionic liquid supported liquid membrane for separating CO2 in gas - Google Patents
Preparation method of ionic liquid supported liquid membrane for separating CO2 in gas Download PDFInfo
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- CN102631843A CN102631843A CN2011100377485A CN201110037748A CN102631843A CN 102631843 A CN102631843 A CN 102631843A CN 2011100377485 A CN2011100377485 A CN 2011100377485A CN 201110037748 A CN201110037748 A CN 201110037748A CN 102631843 A CN102631843 A CN 102631843A
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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
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
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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
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2
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Abstract
The invention relates to a preparation method of an ionic liquid supported liquid membrane for separating CO2 in a gas. According to the method, an ionic liquid is supported in a porous membrane, the mass of the supported ionic liquid is 10% to 70 % of the total mass of the ionic liquid supported liquid membrane, and the ionic liquid supported liquid membrane can be used for separating CO2 in the gas. Compared with the prior art, the membrane is prepared by a physical impregnation method, the operation is simple, and the requirement of equipment is not high. The ionic liquid is supported in a polymer or inorganic porous membrane material by the impregnation method to prepare the ionic liquid supported liquid membrane for separating the CO2 in the gas, so that higher CO2 permeation flux and greater gas separation factor can be obtained, and the service life of the supported liquid membrane can be prolonged. The ionic liquid supported liquid membrane provided by the invention has very broad application prospects in fields of trap of CO2 in a thermal power plant flue gas and an industrial exhaust gas, and separation of CO2 in closed spaces such as a spacecraft and a submarine.
Description
Technical field
The present invention relates to ionic liquid, relate in particular to a kind of preparation method of ionic liquid supporting liquid sheet and at CO
2Application on gas separates.
Background technology
CO
2With other gas such as N
2, CH
4Deng separation have important commercial Application meaning, CO
2With N
2Separation be CO in the power plant flue gas
2The key problem in technology that captures is to reducing CO
2Discharging directly effectively; The new natural gas of gathering contains the CO of 6-14% usually
2Deng sour gas, they not only influence the quality of commodity gas, and when temperature is low, combine to form acid solution with moisture, and etching apparatus, pipeline are to CO
2, CH
4Separate the utilization ratio that improves natural gas extremely important.Separation of C O in the industry
2With chemical absorption method is main; There is the absorption efficiency height in the conventional absorbent that uses at present but the energy consumption height of regenerating simultaneously (like MEA, DEA); Low but the characteristics of absorption efficiency low (like MDEA) simultaneously of the energy consumption of perhaps regenerating, and corrosivity such as conventional organic solvents such as hydramine are strong, volatile.Therefore, the researcher attempts to find the CO in a kind of effective captured gas of material of more clean and effective
2Deng pernicious gas.
Ionic liquid at room temperature is as a kind of emerging " green solvent ", in recent years discover CO
2Solubility in ionic liquid is more much bigger than other gas.Ionic liquid have very high heat endurance and also vapour pressure very little, it not only can be reduced environmental pollution as the gas separating medium, and be easy to recycle.In addition, through suitable selection cation, anion and different substituting groups, can significantly change ion liquid physicochemical properties, the ionic liquid that obtains corresponding to actual needs.Ionic liquid at room temperature is substituted conventional organic solvents be used for CO
2Separation be present CO
2The research focus of trapping technique.
Yet ion liquid viscosity is bigger under the general condition, as if the CO in the ionic liquid separating mixed gas that directly uses liquid flow
2, be difficult to obtain bigger gas transfer speed.For increasing gas and ion liquid contact-making surface to promote mass transfer; Application number is that 200510073345.0 application for a patent for invention utilizes infusion process ionic liquid to be coated on the porosu solids such as silica gel to make adsorbent, be used for adsorbing the sour gas of flue gas and motor-vehicle tail-gas.But adsorb saturated after, must deviate from could continue use behind the gas through Regeneration Treatment, cause operating process to be difficult to carry out continuously.
Membrane separation technique has series of advantages such as separative efficiency height, good impurity removing effect, power consumption be low, simple to operate and receives extensive concern.Supported liquid membrane is a kind of typical promotion transport membranes, have select separative efficiency high, see through that the component flux is big, film liquid consumption is few, extraction and strip and in same process, accomplish, be easy to realize advantages such as pilot scale and fund input are few.But at present also not with the CO of application of membrane separation technology in separating mixed gas
2Report.
Summary of the invention
The object of the invention is exactly for the defective that overcomes above-mentioned prior art existence a kind of requirement of satisfying separation process to high selectivity and high permeating flux to be provided; Can simplify die-manufacturing method, reduce the preparation method who can be used for the ionic liquid supporting liquid sheet of CO2 in the divided gas flow of scale molding cost.
The object of the invention can be realized through following technical scheme: a kind ofly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; It is characterized in that; This method is a supported ion liquid in perforated membrane, and the quality of supported ion liquid accounts for the 10%-70% of ionic liquid supporting liquid sheet gross mass, and this ionic liquid supporting liquid sheet can be used for the CO in the divided gas flow
2
Described method is specifically: perforated membrane is placed in the vacuum drying chamber vacuum drying 1-10 hour; To remove air residual in the porous fenestra, perforated membrane is taken out from vacuum drying chamber, at its surface sprinkling ionic liquid; Ionic liquid is covered perforated membrane fully; Then it is stored in 20~60 ℃ the vacuum drying chamber and left standstill 1~24 hour, wipe the ionic liquid of film remained on surface again with filter paper gently away, promptly make ionic liquid supporting liquid sheet.
Described ionic liquid is a kind of cation and a kind of anion or several cation and several kinds of anion formations, the mixture that at room temperature is in a liquid state.
Described cation is imidazoles cation, phosphine cationoid, pyridines cation, guanidine cationoid or ammonium salt cation, and described anion is BF
4 -, PF
6 -, Tf
2N
-, CF
3SO
3 -, amino acid group or contain the ion of similar amino acid structure.
The material of described perforated membrane is macromolecule or inorganic porous membrane material; Described high-molecular porous membrane material is Kynoar (PVDF), polyether sulfone (PES), polytetrafluoroethylene (PTFE), polysulfones (PS) or polyacrylonitrile (PAN), and described inorganic porous membrane material is Woelm Alumina or molecular sieve.
The face shaping of described perforated membrane is flat or tubular type.
Described gas comprises the arbitrary gas in carbon dioxide and nitrogen, methane, carbon monoxide, hydrogen sulfide, hydrogen, the oxygen.
Compared with prior art, the present invention utilizes the big and difficult characteristic of volatilizing of ionic liquid viscosity, ionic liquid is coated on makes ionic liquid supporting liquid sheet in the porous material, is used for the CO of divided gas flow
2, under the prerequisite that obtains gas high permeating flux and high selectivity, improve the stability of film.Compare with existing polymeric membrane, the development ionic liquid supporting liquid sheet has the advantage of following two aspects: through reasonably combined and cation, anion combined ionic liquid, can satisfy the requirement of separation process to high selectivity and high permeating flux 1.; 2. can simplify die-manufacturing method, reduce scale molding cost.
The present invention adopts physics dipping legal system film, and is simple to operate, not high to equipment requirements.In macromolecule or inorganic porous membrane material, make ionic liquid supporting liquid sheet with ionic liquid loaded through infusion process, be used for the CO of divided gas flow
2, can obtain higher CO
2Permeation flux and bigger gas separation factor, and can prolong service life of supported liquid membrane.Ionic liquid supporting liquid sheet of the present invention is CO in thermal power plant's flue gas, industrial discharge gas
2Enclosure space CO such as capture and spaceship, submarine
2Separation field has very wide application prospect.
The specific embodiment
Further specify the present invention through the specific embodiment and instance below, but the present invention is not limited to following embodiment, before and after not breaking away from, under the scope of said aim, changes and implement to be included in the technical scope of the present invention.
Embodiment 1:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-ethyl-3-methylimidazole two (the fluoroform sulphonyl is inferior) amine ionic liquid [Emim] Tf
2N guarantees that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ CH
4Gas, separation factor are 8~20, CO
2Permeability 1~10GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 2:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-butyl-3-methylimidazole two (the fluoroform sulphonyl is inferior) amine ionic liquid [Bmim] Tf
2N guarantees that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ CH
4Gas, separation factor are 8~15, CO
2Permeability 1~12GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 3:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-butyl-3-methyl imidazolium tetrafluoroborate ionic liquid [Bmim] BF
4, guarantee that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ CH
4Gas, separation factor are 8~17, CO
2Permeability 1~10GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 4:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-butyl-3-methylimidazole hexafluorophosphate ionic liquid [Bmim] PF
6, guarantee that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ CH
4Gas, separation factor are 8~18, CO
2Permeability 1~9GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 5:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-ethyl-3-methylimidazole two (the fluoroform sulphonyl is inferior) amine ionic liquid [Emim] Tf
2N guarantees that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ N
2Gas, separation factor are 10~40, CO
2Permeability 1~10GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 6:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-butyl-3-methylimidazole two (the fluoroform sulphonyl is inferior) amine ionic liquid [Bmim] Tf
2N guarantees that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ N
2Gas, separation factor are 10~35, CO
2Permeability 1~13GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 7:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-butyl-3-methyl imidazolium tetrafluoroborate ionic liquid [Bmim] BF
4, guarantee that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ N
2Gas, separation factor are 10~45, CO
2Permeability 1~10GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 8:
In the time of 40 ℃, Kynoar (PVDF) was placed in the vacuum drying chamber vacuum drying 4 hours, to remove air residual in the fenestra.Perforated membrane is taken out from vacuum drying chamber, with dropper at film surface sprinkling 1-butyl-3-methylimidazole hexafluorophosphate ionic liquid [Bmim] PF
6, guarantee that ionic liquid covers perforated membrane fully, it is stored in 40 ℃ the vacuum drying chamber left standstill 12 hours.Wipe the ionic liquid of film remained on surface gently away with filter paper, promptly make ionic liquid supporting liquid sheet.Then ionic liquid supporting liquid sheet is put into membrane cisterna, be used for separation of C O
2/ N
2Gas, separation factor are 10~40, CO
2Permeability 1~9GPU, continued operation more than 24 hours membrane separating property remain unchanged.
Embodiment 9:
A kind ofly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; This method is that polyether sulfone (PES) perforated membrane was placed in the vacuum drying chamber vacuum drying 10 hours; To remove air residual in the porous fenestra, perforated membrane is taken out from vacuum drying chamber, at its surface sprinkling ionic liquid; Ionic liquid is covered perforated membrane fully, and this ionic liquid is by pyridines cation and CF
3SO
3 -The mixture that at room temperature is in a liquid state that constitutes; Then it is stored in 20 ℃ the vacuum drying chamber and left standstill 24 hours; Wipe the ionic liquid of film remained on surface more gently away with filter paper; Make the quality of supported ion liquid account for 10% of ionic liquid supporting liquid sheet gross mass, promptly make ionic liquid supporting liquid sheet, this ionic liquid supporting liquid sheet can be used for the CO in the divided gas flow
2Gas comprises the arbitrary gas in carbon dioxide and nitrogen, methane, carbon monoxide, hydrogen sulfide, hydrogen, the oxygen.
Embodiment 10:
A kind ofly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; This method is that tubular type Woelm Alumina perforated membrane was placed in the vacuum drying chamber vacuum drying 1 hour, to remove air residual in the porous fenestra, perforated membrane is taken out from vacuum drying chamber; At its surface sprinkling ionic liquid; Ionic liquid is covered perforated membrane fully, and this ionic liquid is the mixture that at room temperature is in a liquid state that is made up of guanidine cationoid and glycine root, it is stored in 60 ℃ the vacuum drying chamber left standstill 1 hour then; Wipe the ionic liquid of film remained on surface more gently away with filter paper; Make the quality of supported ion liquid account for 70% of ionic liquid supporting liquid sheet gross mass, promptly make ionic liquid supporting liquid sheet, this ionic liquid supporting liquid sheet can be used for the CO in the divided gas flow
2Gas comprises the arbitrary gas in carbon dioxide and nitrogen, methane, carbon monoxide, hydrogen sulfide, hydrogen, the oxygen.
Embodiment 11:
A kind ofly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; This method is that flat polytetrafluoroethylene (PTFE) perforated membrane was placed in the vacuum drying chamber vacuum drying 6 hours, to remove air residual in the porous fenestra, perforated membrane is taken out from vacuum drying chamber; At its surface sprinkling ionic liquid; Ionic liquid is covered perforated membrane fully, and this ionic liquid is the mixture that at room temperature is in a liquid state that is made up of ammonium salt cation and alanine root, it is stored in 40 ℃ the vacuum drying chamber left standstill 10 hours then; Wipe the ionic liquid of film remained on surface more gently away with filter paper; Make the quality of supported ion liquid account for 40% of ionic liquid supporting liquid sheet gross mass, promptly make ionic liquid supporting liquid sheet, this ionic liquid supporting liquid sheet can be used for the CO in the divided gas flow
2Gas comprises the arbitrary gas in carbon dioxide and nitrogen, methane, carbon monoxide, hydrogen sulfide, hydrogen, the oxygen.
Claims (7)
1. one kind can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; It is characterized in that; This method is a supported ion liquid in perforated membrane, and the quality of supported ion liquid accounts for the 10%-70% of ionic liquid supporting liquid sheet gross mass, and this ionic liquid supporting liquid sheet can be used for the CO in the divided gas flow
2
2. according to claim 1ly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; It is characterized in that, described method specifically: perforated membrane is placed in the vacuum drying chamber vacuum drying 1-10 hour, to remove air residual in the porous fenestra; Perforated membrane is taken out from vacuum drying chamber; At its surface sprinkling ionic liquid, ionic liquid is covered perforated membrane fully, it is stored in 20~60 ℃ the vacuum drying chamber left standstill 1~24 hour then; Wipe the ionic liquid of film remained on surface again with filter paper gently away, promptly make ionic liquid supporting liquid sheet.
3. according to claim 1ly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet, it is characterized in that described ionic liquid is that a kind of cation and a kind of anion or several cation and several kinds of anion constitute the mixture that at room temperature is in a liquid state.
4. according to claim 3ly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet, it is characterized in that described cation is imidazoles cation, phosphine cationoid, pyridines cation, guanidine cationoid or ammonium salt cation, described anion is BF
4 -, PF
6 -, Tf
2N
-, CF
3SO
3 -, amino acid group or contain the ion of similar amino acid structure.
5. according to claim 1ly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet; It is characterized in that; The material of described perforated membrane is macromolecule or inorganic porous membrane material; Described high-molecular porous membrane material is Kynoar (PVDF), polyether sulfone (PES), polytetrafluoroethylene (PTFE), polysulfones (PS) or polyacrylonitrile (PAN), and described inorganic porous membrane material is Woelm Alumina or molecular sieve.
6. according to claim 5ly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet, it is characterized in that the face shaping of described perforated membrane is flat or tubular type.
7. according to claim 1ly can be used for CO in the divided gas flow
2The preparation method of ionic liquid supporting liquid sheet, it is characterized in that described gas comprises the arbitrary gas in carbon dioxide and nitrogen, methane, carbon monoxide, hydrogen sulfide, hydrogen, the oxygen.
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Cited By (13)
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CN103721530A (en) * | 2012-10-10 | 2014-04-16 | 中国石油化工股份有限公司 | Method using ionic liquid as capturing solvent for membrane absorption for capturing carbon dioxide |
CN103752137A (en) * | 2014-01-20 | 2014-04-30 | 中国科学院过程工程研究所 | Method for capturing acid gases by adopting ether-base pyridine ionic liquid |
CN104707487A (en) * | 2015-01-28 | 2015-06-17 | 复旦大学 | Polyionic liquid functionalized charged composite film and production method thereof |
CN105120989A (en) * | 2013-03-29 | 2015-12-02 | 富士胶片株式会社 | Production method and production device for acid gas separation complex |
CN106268380A (en) * | 2016-09-19 | 2017-01-04 | 石河子大学 | A kind of polyelectrolyte film based on Glycine sodium and its preparation method and application |
CN106582328A (en) * | 2015-10-20 | 2017-04-26 | 中国科学院大连化学物理研究所 | Composite separation film |
CN106902648A (en) * | 2017-04-01 | 2017-06-30 | 浙江大学 | Prepare method and its application of ionic liquid/transition metal dichalcogenide gas separation membrane |
CN107803117A (en) * | 2016-09-09 | 2018-03-16 | 中国科学院青岛生物能源与过程研究所 | A kind of ionic liquid supporting liquid sheet of high stability mesoporous polymer confinement and its preparation method and application |
CN107875867A (en) * | 2017-11-09 | 2018-04-06 | 石河子大学 | A kind of faciliated diffusion film based on amino acid ion liquid and its preparation method and application |
CN110090566A (en) * | 2019-05-10 | 2019-08-06 | 郑州大学 | A kind of sulfonated polyether-ether-ketone-ionic liquid composite membrane, preparation method and its in CO2Application in separation |
CN114713046A (en) * | 2022-04-01 | 2022-07-08 | 福州大学 | Packaged ionic liquid supported liquid membrane and preparation method thereof |
CN114748986A (en) * | 2022-04-22 | 2022-07-15 | 昆明理工大学 | Synchronous defluorination and denitration method for composite absorbent |
CN116672901A (en) * | 2023-08-04 | 2023-09-01 | 西安金沃泰环保科技有限公司 | Nanofiltration material for acid-containing waste gas and preparation method thereof |
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CN106268380B (en) * | 2016-09-19 | 2019-07-09 | 石河子大学 | A kind of polyelectrolyte film and its preparation method and application based on Sodium Glycinate |
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CN107875867A (en) * | 2017-11-09 | 2018-04-06 | 石河子大学 | A kind of faciliated diffusion film based on amino acid ion liquid and its preparation method and application |
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CN116672901B (en) * | 2023-08-04 | 2023-10-27 | 西安金沃泰环保科技有限公司 | Nanofiltration material for acid-containing waste gas and preparation method thereof |
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