CN101916836A - Polymer diaphragm for aqueous solution electrochemical devices - Google Patents
Polymer diaphragm for aqueous solution electrochemical devices Download PDFInfo
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- CN101916836A CN101916836A CN2010102214755A CN201010221475A CN101916836A CN 101916836 A CN101916836 A CN 101916836A CN 2010102214755 A CN2010102214755 A CN 2010102214755A CN 201010221475 A CN201010221475 A CN 201010221475A CN 101916836 A CN101916836 A CN 101916836A
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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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/13—Energy storage using capacitors
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Abstract
The invention discloses a polymer diaphragm for aqueous solution electrochemical devices. In the diaphragm, polysulfone engineering plastics and polyvinylpyrrolidone are used as raw materials and are dissolved in a solvent, the solutions are mixed, and the mixed solution is coated and cast to form films, low alcohol-containing electrolyte solution for the electrochemical devices is used for the hydrophilization of the films. The blended films obtained are homogeneous phases and compact and have advantageous chemical and thermal stability and high mechanical and conductive performance. The blended films can be used as a diaphragm material for aqueous solution electrochemical devices such as water electrolytic cells, batteries, super capacitors, fluid batteries and the like.
Description
Technical field
The invention belongs to technical field of electrochemistry, the membrane for polymer that particularly a kind of aqueous solution electrochemical devices is used.
Technical background
Membrane for polymer is the critical material in the electrochemical device used of Separation ﹠ Purification, water technology, chemical industry and Chemical Decomposition and thereafter electrochemical device fields such as (as chemical power source, water electrolysis, ultracapacitor and flow batteries) be used widely.Yet, cause being hindered based on its development of aqueous solution electrochemical devices because the restriction of the performance of membrane for polymer own is difficult to take into account between mechanical strength, chemical stability, thermal stability and ionic conductivity.For example, in industrial alkaline water electrolytic, the barrier film that adopts is mainly the porous asbestos diaphragm at present, but asbestos diaphragm is not the desirable diaphragm material of alkaline water electrolytic, and asbestos fibre can cause serious diseases such as asbestos are stagnant, celiothelioma, cancer; Asbestos diaphragm is a perforated membrane in addition, in order to reach very thick (being generally 200～300 millimeters) that good gas-barrier properties energy barrier film must be done, so directly cause barrier film face resistance bigger, thereby electrolysis energy consumption increases.But because the harsh service condition (80～90 ℃ of 30% (weight) potassium hydroxide aqueous solution) of alkaline water electrolytic and the restriction of the physicochemical properties of polymer own, the polymer that can satisfy its instructions for use is actually rare.
Polysulfones-like polymer is the engineering plastics that a class has excellent mechanical properties, acid-alkali-corrosive-resisting performance, antioxygenic property and thermal stability, but its strong hydrophobicity has had a strong impact on its application as diaphragm material.The more common method of improving these class engineering plastics is to adopt hydrophilic polymer or hydrophilic inorganic nanoparticles and hydrophobic polymer to form even casting film at present, adopts phase inversion to prepare hydrophilic barrier film then.The barrier film that phase inversion prepares is heterogeneous perforated membrane, and film-strength is relatively poor, and the factor that influences film form, pore structure is bigger, so reappearance is bad.For example employing inversion of phases such as Belgian R.Leysen is prepared porous polysulfones barrier film [R.Leysen, et al., Desalination, 1996,104,47] and commercial
Barrier film (ZrO
2Composite membrane with PSF) [R.Leysen, etal., Internationaljournal of Hydrogen Energy, 1998,23,321] all belong to this type, in order to reach good gas-barrier properties energy and enough mechanical performances, this class barrier film must reach certain thickness (reaching more than 0.5 millimeter), so directly causes barrier film face resistance bigger, causes electrolysis energy consumption to increase.
Summary of the invention
Purpose of the present invention is exactly the situation at above-mentioned prior art, need not under the prerequisite of inversion of phases, utilizes polysulfones-like polymer to make the membrane for polymer that a kind of aqueous solution electrochemical devices is used.
Technical scheme of the present invention is: get the membrane for polymer of expecting and making a kind of aqueous solution electrochemical devices through following step according to quality ratio polysulfones engineering plastics/polyvinylpyrrolidone 〉=0.1 by polysulfones engineering plastics and polyvinylpyrrolidone:
1, polysulfones engineering plastics and kollidon are mixed with polymer solution with its dissolution with solvents and after mixing;
2, will go up the polymer solution that obtains of step is coated with and casts blend film;
3, in the electrolyte solution that aqueous solution electrochemical devices is used, add an amount of lower alcohol, make the film treatment fluid;
4, blend film is inserted in the film Treatment Solution fully soak after, take out washing.
As preferably, in the such scheme:
1, lower alcohol content 〉=1% in the film treatment fluid
2, the polysulfones engineering plastics comprise the phenolic polyether sulphone engineering plastics, polyarylsulfone (PAS) engineering plastics and polyether sulfone engineering plastics;
3, the solvent of dissolving polysulfones engineering plastics and kollidon is N, dinethylformamide, N, N-dimethylacetylamide, N-methyl pyrrolidone, dimethyl sulfoxide (DMSO).
A kind of aqueous solution electrochemical devices membrane for polymer manufactured according to the present invention: 1, adopting polysulfones engineering plastics and polyvinylpyrrolidone is raw material, has utilized excellent mechanical properties, acid-alkali-corrosive-resisting performance, antioxygenic property and the thermal stability of polysulfones-like polymer preferably.2, after aqueous solution electrochemical devices adds an amount of lower alcohol in electrolyte solution, soak, solved the strong hydrophobicity of polysulfones engineering plastics preferably by above-mentioned two kinds of barrier films that material makes.3, homogeneous phase, densification have superior chemistry and thermal stability, and excellent mechanical performance and good electric conductivity, can be used as the diaphragm material of aqueous solution electrochemical devices such as water electrolysis, battery, ultracapacitor, flow battery.
Embodiment
Further describe the membrane for polymer that a kind of aqueous solution electrochemical devices involved in the present invention is used by the following examples.
Embodiment 1:
The present embodiment barrier film is got material by phenolic polyether sulphone and polyvinylpyrrolidone by quality ratio phenolic polyether sulphone/polyvinylpyrrolidone=1, and makes through following step:
The phenolic polyether sulphone that takes by weighing 1 unit of weight is dissolved in N, and in the dinethylformamide, stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 1 unit of weight is dissolved in N, and in the dinethylformamide, stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring, with after the mixed solution vacuumize degassing 40 ℃ of following The tape casting film forming.Is methyl alcohol with the gained blend film at mass ratio: water: soak the back in the film treatment fluid of NaOH=2: 7: 1 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes phenolic polyether sulphone with polyarylsulfone (PAS) or polyether sulfone; (2) with N, a kind of alternative N in N-dimethylacetylamide, N-methyl pyrrolidone or the dimethyl sulfoxide (DMSO), dinethylformamide; (3) replace The tape casting with other film build method; (4) with the methyl alcohol in other lower alcohol alternative membrane treatment fluid; (5) with the NaOH in other electrolyte replacement film treatment fluid.
Embodiment 2:
The present embodiment barrier film is got material by polyarylsulfone (PAS) and polyvinylpyrrolidone by its quality ratio polyarylsulfone (PAS)/polyvinylpyrrolidone=2 and is made through following step:
The polyarylsulfone (PAS) that takes by weighing 1 unit of weight is dissolved in N, and in the N-dimethylacetylamide, stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 0.5 unit of weight is dissolved in N, and in the N-dimethylacetylamide, stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring, will descend static casting method film forming at 60 ℃ after the mixed solution vacuumize degassing.Is ethanol with the gained blend film at mass ratio: water: soak the back in the film treatment fluid of sodium chloride=5: 4: 1 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes polyarylsulfone (PAS) with phenolic polyether sulphone or polyether sulfone; (2) with N, a kind of alternative N in dinethylformamide, N-methyl pyrrolidone, the dimethyl sulfoxide (DMSO), N-dimethylacetylamide; (3) replace static casting method with other film build method; (4) with the ethanol in other lower alcohol alternative membrane treatment fluid; (5) with the sodium chloride in other electrolyte replacement film treatment fluid.
Embodiment 3:
The present embodiment barrier film is got material by polyether sulfone and polyvinylpyrrolidone by ratio polyether sulfone/polyvinylpyrrolidone=5 of quality, and makes through following step:
The polyether sulfone that takes by weighing 1 unit of weight is dissolved in the N-methyl pyrrolidone, and stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 0.2 unit of weight is dissolved in the N-methyl pyrrolidone, and stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring, with after the mixed solution vacuumize degassing 80 ℃ of following The tape casting film forming.Is propyl alcohol with the gained blend film at mass ratio: water: soak the back in the film treatment fluid of potassium sulfate=7: 2: 1 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes polyether sulfone with phenolic polyether sulphone or polyarylsulfone (PAS); (2) with N, dinethylformamide, N, a kind of alternative N-methyl pyrrolidone in N-dimethylacetylamide, the dimethyl sulfoxide (DMSO); (3) replace The tape casting with other film build method; (4) with the propyl alcohol in other lower alcohol alternative membrane treatment fluid; (5) with the potassium sulfate in other electrolyte replacement film treatment fluid.
Embodiment 4:
The present embodiment barrier film is got material by phenolic polyether sulphone and polyvinylpyrrolidone by quality ratio phenolic polyether sulphone/polyvinylpyrrolidone=10 and is made through following step:
The phenolic polyether sulphone that takes by weighing 1 unit of weight is dissolved in N, and in the dinethylformamide, stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 0.1 unit of weight is dissolved in N, and in the dinethylformamide, stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring, with after the mixed solution vacuumize degassing 120 ℃ of following The tape casting film forming.Is propyl alcohol with gained homogeneous phase blend film at mass ratio: water: soak the back in the film treatment fluid of hydrochloric acid=9: 0.3: 0.7 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes phenolic polyether sulphone with polyarylsulfone (PAS) or polyether sulfone; (2) with N, a kind of alternative N in N-dimethylacetylamide, N-methyl pyrrolidone or the dimethyl sulfoxide (DMSO), dinethylformamide; (3) replace The tape casting with other film build method; (4) with the propyl alcohol in other lower alcohol alternative membrane treatment fluid; (5) with the hydrochloric acid in other electrolyte replacement film treatment fluid.
Embodiment 5:
The present embodiment barrier film is got material by phenolic polyether sulphone and polyvinylpyrrolidone by quality ratio phenolic polyether sulphone/polyvinylpyrrolidone=0.1, and makes through following step:
The phenolic polyether sulphone that takes by weighing 1 unit of weight is dissolved in the methyl-sulfoxide, and stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 10 unit of weights is dissolved in the methyl-sulfoxide, and stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring, will descend static casting method film forming at 100 ℃ after the mixed solution vacuumize degassing.Is isopropyl alcohol with gained homogeneous phase blend film at mass ratio: water: soak the back in the film treatment fluid of sulfuric acid=0.1: 8: 1.9 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes phenolic polyether sulphone with polyarylsulfone (PAS) or polyether sulfone; (2) with N, dinethylformamide, N, a kind of alternative dimethyl sulfoxide (DMSO) in N-dimethylacetylamide, the N-methyl pyrrolidone; (3) replace static casting method with other film build method; (4) with the isopropyl alcohol in other lower alcohol alternative membrane treatment fluid; (5) with the sulfuric acid in other electrolyte replacement film treatment fluid.
Embodiment 6:
The present embodiment barrier film is got material by polyether sulfone and polyvinylpyrrolidone by quality ratio polyether sulfone/polyvinylpyrrolidone=0.25, and makes through following step:
The polyether sulfone that takes by weighing 1 unit of weight is dissolved in N, and in the N-dimethylacetylamide, stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 4 unit of weights is dissolved in N, and in the N-dimethylacetylamide, stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring, will descend static casting method film forming at 80 ℃ after the mixed solution vacuumize degassing.Is ethanol with the gained blend film at mass ratio: water: soak the back in the film treatment fluid of potassium hydroxide=0.5: 8.5: 1 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes polyether sulfone with phenolic polyether sulphone or polyarylsulfone (PAS); (2) with N, a kind of alternative N in dinethylformamide, N-methyl pyrrolidone, the dimethyl sulfoxide (DMSO), N-dimethylacetylamide; (3) replace static casting method with other film build method; (4) with the ethanol in other lower alcohol alternative membrane treatment fluid; (5) with the potassium hydroxide in other electrolyte replacement film treatment fluid.
Embodiment 7:
The present embodiment barrier film is got material by polyarylsulfone (PAS) and polyvinylpyrrolidone by quality ratio polyarylsulfone (PAS)/polyvinylpyrrolidone=0.5, and makes through following step:
The polyarylsulfone (PAS) that takes by weighing 1 unit of weight is dissolved in the N-methyl pyrrolidone of 9 unit of weights, and stirring becomes clear solution until dissolving; The polyvinylpyrrolidone that takes by weighing 2 unit of weights is dissolved in the N-methyl pyrrolidone of 9 unit of weights, and stirring becomes clear solution until dissolving; Two kinds of polymer solutions are mixed stirring 10 hours, will descend static casting method film forming at 80 ℃ after the mixed solution vacuumize degassing.Is methyl alcohol with gained homogeneous phase blend film at mass ratio: water: soak the back in the film treatment fluid of sulfuric acid=1: 7.5: 1.5 and take out washing, promptly obtain the hydrophilic polymer barrier film.
The concentration of polysulfones engineering plastics polymer solution and polyvinyl pyrrolidone polymers solution does not influence the performance of blend film during above-mentioned preparation blend film.
Adopt the following barrier film that condition all can obtain similarity that substitutes in the present embodiment: (1) substitutes polyarylsulfone (PAS) with phenolic polyether sulphone or polyether sulfone; (2) with N, dinethylformamide, N, a kind of alternative N-methyl pyrrolidone in N-dimethylacetylamide, the dimethyl sulfoxide (DMSO); (3) replace static casting method with other film build method; (4) with the methyl alcohol in other lower alcohol alternative membrane treatment fluid; (5) with the sulfuric acid in other electrolyte replacement film treatment fluid.
Claims (4)
1. membrane for polymer that aqueous solution electrochemical devices is used is characterized in that:
Described membrane for polymer is to be got material according to quality ratio polysulfones engineering plastics/polyvinylpyrrolidone 〉=0.1 and made through following step by polysulfones engineering plastics and polyvinylpyrrolidone:
1) polysulfones engineering plastics and kollidon are mixed with polymer solution with its dissolution with solvents and after mixing;
2) will go up the polymer solution that obtains of step is coated with and casts blend film;
3) in the electrolyte solution that aqueous solution electrochemical devices is used, add an amount of lower alcohol, make the film treatment fluid;
4) blend film is inserted in the film treatment fluid fully soak after, take out washing.
2. the membrane for polymer that a kind of aqueous solution electrochemical devices according to claim 1 is used is characterized in that: in the described film treatment fluid, and the mass content of its lower alcohol 〉=1%.
3. the membrane for polymer that a kind of aqueous solution electrochemical devices according to claim 1 and 2 is used is characterized in that: described polysulfones engineering plastics comprise phenolic polyether sulphone engineering plastics, polyarylsulfone (PAS) engineering plastics, polyether sulfone engineering plastics.
4. the membrane for polymer that a kind of aqueous solution electrochemical devices according to claim 1 and 2 is used, it is characterized in that: the solvent of described dissolving polysulfones engineering plastics and kollidon is N, dinethylformamide, N, N-dimethylacetylamide, N-methyl pyrrolidone, dimethyl sulfoxide (DMSO).
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102280251A (en) * | 2011-05-27 | 2011-12-14 | 吉林大学 | Super capacitor based on graphene and polyarylether and preparation method thereof |
| CN104377042A (en) * | 2014-10-17 | 2015-02-25 | 超威电源有限公司 | Ion selective membrane for pseudo-electric super capacitor |
| CN107591545A (en) * | 2016-07-07 | 2018-01-16 | 中国科学院大连化学物理研究所 | A kind of application of blended porous membrane in flow battery |
| CN108123155A (en) * | 2016-11-28 | 2018-06-05 | 中国科学院金属研究所 | A kind of preparation method of non-fluorine porous composite film used for all-vanadium redox flow battery |
| CN111004508A (en) * | 2019-11-11 | 2020-04-14 | 北京航空航天大学 | Hydrophilic single-layer porous membrane and preparation method and application thereof |
| CN111471204A (en) * | 2020-04-14 | 2020-07-31 | 北京航空航天大学 | Hydrophobic anisotropic surface and preparation method and application thereof |
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| CN1560117A (en) * | 2004-02-26 | 2005-01-05 | 武汉大学 | Preparation process of strong basic polymer electrolyte film |
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2010
- 2010-07-02 CN CN2010102214755A patent/CN101916836A/en active Pending
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| CN1560117A (en) * | 2004-02-26 | 2005-01-05 | 武汉大学 | Preparation process of strong basic polymer electrolyte film |
Non-Patent Citations (2)
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| 《2005年全国高分子学术论文报告会论文摘要集》 20051231 黄爱宾; 卢善富; 肖超渤; 庄林 新型隔膜碱性水电解的初步研究 全文 1-4 , * |
| 《第十三次全国电化学会议论文摘要集（下集）》 20051231 卢善富; 黄爱宾; 庄林; 陆君涛 一种碱性水电解用新型隔膜 410-411 1-4 , * |
Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102280251A (en) * | 2011-05-27 | 2011-12-14 | 吉林大学 | Super capacitor based on graphene and polyarylether and preparation method thereof |
| CN104377042A (en) * | 2014-10-17 | 2015-02-25 | 超威电源有限公司 | Ion selective membrane for pseudo-electric super capacitor |
| CN104377042B (en) * | 2014-10-17 | 2017-04-26 | 超威电源有限公司 | Ion selective membrane for pseudo-electric super capacitor |
| CN107591545A (en) * | 2016-07-07 | 2018-01-16 | 中国科学院大连化学物理研究所 | A kind of application of blended porous membrane in flow battery |
| CN108123155A (en) * | 2016-11-28 | 2018-06-05 | 中国科学院金属研究所 | A kind of preparation method of non-fluorine porous composite film used for all-vanadium redox flow battery |
| CN111004508A (en) * | 2019-11-11 | 2020-04-14 | 北京航空航天大学 | Hydrophilic single-layer porous membrane and preparation method and application thereof |
| CN111004508B (en) * | 2019-11-11 | 2022-02-11 | 北京航空航天大学 | Hydrophilic single-layer porous membrane and preparation method and application thereof |
| CN111471204A (en) * | 2020-04-14 | 2020-07-31 | 北京航空航天大学 | Hydrophobic anisotropic surface and preparation method and application thereof |
| CN111471204B (en) * | 2020-04-14 | 2021-06-08 | 北京航空航天大学 | Hydrophobic anisotropic surface and preparation method and application thereof |
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Application publication date: 20101215 |