CN104716353A - Porous membrane used for liquid flow cell and preparation and application thereof - Google Patents
Porous membrane used for liquid flow cell and preparation and application thereof Download PDFInfo
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- CN104716353A CN104716353A CN201310693038.7A CN201310693038A CN104716353A CN 104716353 A CN104716353 A CN 104716353A CN 201310693038 A CN201310693038 A CN 201310693038A CN 104716353 A CN104716353 A CN 104716353A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
- H01M8/184—Regeneration by electrochemical means
- H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0289—Means for holding the electrolyte
- H01M8/0293—Matrices for immobilising electrolyte solutions
-
- 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
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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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
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Abstract
The invention relates to a porous membrane used for a liquid flow cell and preparation and application thereof, the porous membrane is prepared from raw materials of one or more than two kinds of organic polymer resin and one or more than two degradable organic or inorganic components in the electrolyte; the degradable component content is 5 to 40 wt% by mass of the organic polymer resin; and the porous membrane is prepared by the preparation process in the condition of constant temperature and constant humidity. The porous membrane has a multi-stage pore structure, and can effectively achieve the separation between ions with different valences, and the ion-passing-selectivity of the ionic membrane of the membrane can be kept. The composite membrane is simple and environmentally-friendly in process, controllable in pore structure, and low in cost, and mass production is easy to realize.
Description
Technical field
The present invention relates to a kind of flow battery perforated membrane, particularly a kind of perforated membrane and Synthesis and applications thereof with hierarchical porous structure.
Background technology
Flow battery is a kind of electrochemical energy storage new technology, compared with other energy storage technology, have that energy conversion efficiency is high, system is flexible, capacitance of storage is large, addressing is free, can the advantage such as deep discharge, safety and environmental protection, maintenance cost be low, the aspects such as the energy storage of the renewable energy power generation such as wind energy, solar energy, emergency power system, stand-by station and electric power system peak load shifting can be widely used in.All-vanadium flow battery (Vanadium flow battery, VFB), because fail safe is high, good stability, efficiency are high, the life-span is long (life-span >15), low cost and other advantages, is considered to have good application prospect.
Battery diaphragm is the important component part in flow battery, and it plays and intercepts positive and negative electrode electrolyte, provides the effect of proton transmitting channel.Proton-conducting, the chemical stability and ion selectivity etc. of film directly will affect chemical property and the useful life of battery; Therefore require that film has lower active material permeability (namely having higher selectivity) and lower surface resistance (namely having higher ionic conductance), also should have good chemical stability and lower cost simultaneously.The Nafion film of the membrane material both at home and abroad used now mainly du pont company's exploitation, Nafion film has excellent performance in chemical property and useful life etc., but due to expensive, particularly be applied in all-vanadium flow battery shortcomings such as there is ion selectivity difference, thus limit the industrial applications of this film.Therefore, the battery diaphragm with high selectivity, high stability and low cost is developed most important.
In VFB, vanadium ion and proton all exist with the form of hydrated ion.Due to the difference of vanadium ion and hydrogen ion hydration radius, can be realized vanadium ion and hydrionic Selective Separation by porous diffusion barrier.Using perforated membrane as VFB barrier film, have that chemical stability is good, material selection wide ranges, technical maturity easily amplify, the advantages such as production cost is low.But perforated membrane is difficult to take into account to the selectivity of hydrogen ion and vanadium ion and proton-conducting, therefore improve perforated membrane selectivity, ionic conductivity, and then realize its sizable application and have great importance.
Imagine a kind of have in the hole of honeycomb structure barrier film be full of electrolyte, be conducive to the transmission of proton in film.If construct little duct on its hole wall, by the sieving actoion of hole wall layer by layer, effectively can improve the ion selectivity of film, there is good proton-conducting simultaneously.The exchange rate of solvent and non-solvent and the formation of gel time to the pore structure of film play conclusive effect, therefore it can be made to be formed by the relative steam content and temperature controlling the non-solvent in air and have cellular pore structure.In casting solution, add degradable organic or inorganic composition in the electrolytic solution simultaneously, can hierarchical porous structure be formed, effectively can improve ion selectivity and the proton-conducting of film, thus obtain better battery performance.
Summary of the invention
For achieving the above object, the technical solution used in the present invention is as follows:
A kind of flow battery perforated membrane, described porous composite film is prepared from for raw material by one or two or more kinds of one or two or more kinds in organic polymer resin and degradable organic or inorganic composition in the electrolytic solution; Degradable component content is 5 ~ 40wt% of organic polymer resin quality;
Described organic polymer resin is one or two or more kinds in polysulfones, polyketone, polyacrylonitrile, polyimides, polyethers ketone, polytetrafluoroethylene, Kynoar, polybenzimidazoles or polyvinyl pyridine;
Described inorganic constituents is one or two or more kinds in silica, zirconia, titanium oxide, lead oxide, tungsten oxide or basic zirconium phosphate; Organic principle is one or two or more kinds in polyvinylpyrrolidone, polyethylene glycol.
Described perforated membrane is by macropore and be distributed in the hierarchical porous structure that the aperture on macropore hole wall forms; Perforated membrane thickness is 20 ~ 500 μm, and porosity is 5 ~ 60%; Wherein the aperture size of macropore is 50nm ~ 2 micron, and wherein the aperture size of aperture is 2 ~ 10nm, and wherein, aperture accounts for 0.1 ~ 5% of perforated membrane mesopore volume.
Described composite membrane adopts humidity phase inversion to be prepared from.
Described porous septum adopts following process to prepare:
(1) by organic polymer resin and in the electrolytic solution degradable component dissolves in organic solvent, at temperature be 20 ~ 100 DEG C, fully stir 0.5 ~ 10h make blend solution; Wherein organic polymer resin concentration is between 5 ~ 40wt%, and degradable component content is 5 ~ 40wt% of organic polymer resin quality;
Do not add in above-mentioned solvent or also can add effumability solvent, form mixed solvent, the concentration of effumability solvent in mixed solvent is 0 ~ 50wt%;
(2) blend solution prepared by step (1) be poured at the bottom of nonwoven fabric base or be poured directly on glass plate, solvent flashing 0 ~ 60 second, then its entirety is placed in climatic chamber, in climatic chamber the relative steam humidity of the poor solvent of resin 10% ~ 100%, temperature prepares film forming at-20 ~ 100 DEG C; The thickness of film is between 20 ~ 500 μm; Optimum condition is temperature 50 degree, humidity 100%;
(3) prepared film is placed in flow battery electrolyte solution to soak more than 24 hours, obtains required perforated membrane.
Described flow battery electrolyte solution can be all-vanadium flow battery pentavalent vanadium solution, ferric iron or hexavalent chromium solution in zinc-bromine flow battery bromine simple substance, siderochrome flow battery.
Described organic solvent is one or two or more kinds in DMSO, DMAC, NMP, DMF; Described effumability non-solvent is one or two or more kinds in methyl alcohol, oxolane or n-hexane, and the poor solvent of resin is one or two or more kinds in water, methyl alcohol, ethanol, propyl alcohol or isopropyl alcohol.
Described composite membrane can be used in flow battery, and described flow battery comprises all-vanadium flow battery, zinc/bromine flow battery, sodium polysulfide/bromine redox flow cell, iron/chrome liquor galvanic battery, vanadium/bromine flow battery or zinc/cerium flow battery.
Useful achievement of the present invention:
1. the composite membrane that prepared by the present invention is applied in flow battery, the exchange rate of solvent and non-solvent and the relativeness of gel time is regulated by the relative steam content and temperature that control the non-solvent in air, multi-stage porous can be formed, effectively can improve selectivity and the proton-conducting of film, thus obtain better battery performance.
2. the composite membrane that prepared by the present invention by changing the kind of non-solvent kind, biodegradable component, can regulate and control selectivity and the conductibility of such film.
3. the composite membrane prepared of the present invention, pore structure is adjustable, with low cost, easily realizes producing in enormous quantities.
4. the present invention has widened kind and the scope of application of flow battery membrane material.
5. the present invention can realize the controllability to flow battery efficiency.
Such film has hierarchical porous structure, by the sieving actoion of hole wall layer by layer, effectively can improve ion selectivity and the proton-conducting of film.
Accompanying drawing explanation
Fig. 1 is perforated membrane SEM photo prepared by embodiment 1;
The monocell charging and discharging curve of Fig. 2 perforated membrane prepared by embodiment 1.
Embodiment
The following examples further illustrate of the present invention, instead of limit the scope of the invention.
Embodiment 1
8 grams of polyether sulfones and 4 grams of polyvinylpyrrolidones are dissolved in 20mLDMAC, stir 8 hours, the polymer solution of formation, be laid in glass plate, then put into rapidly the climatic chamber that wetness is 100%, temperature is 50 DEG C, solidify 10 minutes, form perforated membrane, film thickness is 130 μm.Prepared film is soaked 48 hours as in the sulfuric acid solution of the 3M of 1.5M pentavalent vanadium.Obtain the porous diffusion barrier with hierarchical porous structure as can be seen from Figure 1.
Porous composite film assembling all-vanadium flow battery prepared by utilization, wherein Catalytic Layer is activated carbon-fiber felt, and bipolar plates is graphite cake, and the effective area of film is 6cm
-2, both positive and negative polarity electrolyte volume is 30mL, and wherein vanadium ion concentration is 1.50mol L
-1, H
2sO
4concentration is 3mol L
-1.Can find out from Fig. 2 charging and discharging curve, battery charging and discharging current density is 80mA cm
-2, battery coulombic efficiency is 93%, and energy efficiency is 79%.
Embodiment 2
With embodiment 1, change polyether sulfone into polyacrylonitrile, prepare porous composite film.The flow battery current efficiency of assembling is 89%, and energy efficiency is 76%.
Embodiment 3
With embodiment 1, change polyvinylpyrrolidone into silica, prepare porous composite film.The flow battery current efficiency of assembling is 91%, and energy efficiency is 78.5%.
Embodiment 4
With embodiment 1, change steam into alcohol vapor, prepare porous composite film.The flow battery current efficiency of assembling is 92%, and energy efficiency is 76%.
Embodiment 5
Humidity is changed into 90% with embodiment 1.The flow battery current efficiency of assembling is 95%, and energy efficiency is 76%.
Embodiment 6
Humidity is changed into 80% with embodiment 1.The flow battery current efficiency of assembling is 96%, and energy efficiency is 75%.
Claims (6)
1. a flow battery perforated membrane, is characterized in that: described perforated membrane is prepared from for raw material by one or two or more kinds of one or two or more kinds in organic polymer resin and degradable organic or inorganic composition in the electrolytic solution; Degradable component content is 5 ~ 40wt% of organic polymer resin quality;
Described organic polymer resin is one or two or more kinds in polysulfones, polyketone, polyacrylonitrile, polyimides, polyethers ketone, polytetrafluoroethylene, Kynoar, polybenzimidazoles or polyvinyl pyridine;
Described inorganic constituents is one or two or more kinds in silica, zirconia, titanium oxide, lead oxide, tungsten oxide or basic zirconium phosphate; Organic principle is one or two or more kinds in polyvinylpyrrolidone, polyethylene glycol.
2. perforated membrane according to claim 1, is characterized in that: described perforated membrane is by macropore and be distributed in the hierarchical porous structure that the aperture on macropore hole wall forms; Perforated membrane thickness is 20 ~ 500 μm, and porosity is 5 ~ 60%; Wherein the aperture size of macropore is 50nm ~ 2 micron, and wherein the aperture size of aperture is 2 ~ 10nm, and wherein, aperture accounts for 0.1 ~ 5% of perforated membrane mesopore volume.
3. a preparation method for perforated membrane according to claim 1, is characterized in that:
Described perforated membrane adopts following steps preparation:
(1) by organic polymer resin and in the electrolytic solution degradable component dissolves in organic solvent, at temperature be 20 ~ 100 DEG C, fully stir 0.5 ~ 10h make blend solution; Wherein organic polymer resin concentration is between 5 ~ 40wt%, and degradable component content is 5 ~ 40wt% of organic polymer resin quality;
Do not add in above-mentioned solvent or also can add effumability solvent, form mixed solvent, the concentration of effumability solvent in mixed solvent is 0 ~ 50wt%;
(2) blend solution prepared by step (1) be poured at the bottom of nonwoven fabric base or be poured directly on glass plate, solvent flashing 0 ~ 60 second, then its entirety is placed in climatic chamber, in climatic chamber the relative steam humidity of the poor solvent of resin 10% ~ 100%, temperature prepares film forming at-20 ~ 100 DEG C; The thickness of film is between 20 ~ 500 μm; Optimum condition is temperature 50 degree, humidity 100%;
(3) prepared film is placed in flow battery electrolyte solution to soak more than 24 hours, obtains required perforated membrane.
4. preparation method according to claim 3, is characterized in that:
Described flow battery electrolyte solution can be ferric iron or hexavalent chromium solution in all-vanadium flow battery pentavalent vanadium solution, zinc-bromine flow battery bromine simple substance, siderochrome flow battery.
5. preparation method according to claim 3, is characterized in that:
Described organic solvent is one or two or more kinds in DMSO, DMAC, NMP, DMF; Described effumability non-solvent is one or two or more kinds in methyl alcohol, oxolane or n-hexane, and the poor solvent of resin is one or two or more kinds in water, methyl alcohol, ethanol, propyl alcohol or isopropyl alcohol.
6. an application for perforated membrane described in claim 1 or 2, is characterized in that: described flow battery comprises all-vanadium flow battery, vanadium/bromine flow battery or iron/chrome liquor galvanic battery.
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Cited By (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106532104A (en) * | 2015-09-09 | 2017-03-22 | 中国科学院大连化学物理研究所 | Gel electrolyte porous electrode for lithium-sulfur battery and preparation and application of gel electrolyte porous electrode |
| CN107546399A (en) * | 2016-06-29 | 2018-01-05 | 中国科学院大连化学物理研究所 | The amberplex and its preparation and application that main chain separates with ion-exchange group |
| CN107546397A (en) * | 2016-06-29 | 2018-01-05 | 中国科学院大连化学物理研究所 | A kind of flow battery porous ion conductive membranes and its preparation and application |
| 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 |
| CN108129612A (en) * | 2016-12-01 | 2018-06-08 | 中国科学院大连化学物理研究所 | The preparation of phosphoric acid functionalized multistage pore canal hybrid integral material and material and application |
| CN108134107A (en) * | 2016-12-01 | 2018-06-08 | 中国科学院大连化学物理研究所 | A kind of perforated membrane is in the application of Alkaline Zinc iron liquid galvanic battery |
| CN109659589A (en) * | 2017-10-11 | 2019-04-19 | 中国科学院大连化学物理研究所 | The screening technique of flow battery polyalcohol stephanoporate ion-conductive membranes in a kind of solvent treatment process |
| CN110943238A (en) * | 2018-09-21 | 2020-03-31 | 中国科学院大连化学物理研究所 | Ion-conducting membrane for flow battery and preparation and application thereof |
| CN112447994A (en) * | 2019-08-28 | 2021-03-05 | 中国科学院大连化学物理研究所 | Application of ion-conducting membrane containing chlorinated polyvinyl chloride in flow battery |
| CN114044853A (en) * | 2021-11-15 | 2022-02-15 | 湖北工程学院 | Biomass-based EC-g-PSSA graft copolymer and preparation method and application thereof |
| CN117317331A (en) * | 2023-11-28 | 2023-12-29 | 华中科技大学 | Positive electrode electrolyte of chromium chelate and flow battery |
| CN117855541A (en) * | 2023-12-12 | 2024-04-09 | 广州高新区能源技术研究院有限公司 | Ion exchange membrane, preparation method thereof and flow battery |
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Cited By (18)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN106532104A (en) * | 2015-09-09 | 2017-03-22 | 中国科学院大连化学物理研究所 | Gel electrolyte porous electrode for lithium-sulfur battery and preparation and application of gel electrolyte porous electrode |
| CN106532104B (en) * | 2015-09-09 | 2019-03-19 | 中国科学院大连化学物理研究所 | A kind of lithium-sulfur cell gel electrolyte porous electrode and its preparation and application |
| CN107546399A (en) * | 2016-06-29 | 2018-01-05 | 中国科学院大连化学物理研究所 | The amberplex and its preparation and application that main chain separates with ion-exchange group |
| CN107546397A (en) * | 2016-06-29 | 2018-01-05 | 中国科学院大连化学物理研究所 | A kind of flow battery porous ion conductive membranes and its preparation and application |
| CN107546399B (en) * | 2016-06-29 | 2020-04-07 | 中国科学院大连化学物理研究所 | Ion exchange membrane with main chain separated from ion exchange group and preparation and application thereof |
| CN107546397B (en) * | 2016-06-29 | 2020-02-21 | 中国科学院大连化学物理研究所 | Porous ion conduction membrane for flow battery and preparation and application thereof |
| 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 |
| CN108129612B (en) * | 2016-12-01 | 2020-01-14 | 中国科学院大连化学物理研究所 | Preparation of phosphoric acid functionalized multistage pore hybrid monolithic material, and material and application thereof |
| CN108134107A (en) * | 2016-12-01 | 2018-06-08 | 中国科学院大连化学物理研究所 | A kind of perforated membrane is in the application of Alkaline Zinc iron liquid galvanic battery |
| CN108129612A (en) * | 2016-12-01 | 2018-06-08 | 中国科学院大连化学物理研究所 | The preparation of phosphoric acid functionalized multistage pore canal hybrid integral material and material and application |
| CN109659589A (en) * | 2017-10-11 | 2019-04-19 | 中国科学院大连化学物理研究所 | The screening technique of flow battery polyalcohol stephanoporate ion-conductive membranes in a kind of solvent treatment process |
| CN110943238A (en) * | 2018-09-21 | 2020-03-31 | 中国科学院大连化学物理研究所 | Ion-conducting membrane for flow battery and preparation and application thereof |
| CN110943238B (en) * | 2018-09-21 | 2020-11-20 | 中国科学院大连化学物理研究所 | Ion-conducting membrane for flow battery and preparation and application thereof |
| CN112447994A (en) * | 2019-08-28 | 2021-03-05 | 中国科学院大连化学物理研究所 | Application of ion-conducting membrane containing chlorinated polyvinyl chloride in flow battery |
| CN112447994B (en) * | 2019-08-28 | 2022-03-08 | 中国科学院大连化学物理研究所 | Application of ion-conducting membrane containing chlorinated polyvinyl chloride in flow battery |
| CN114044853A (en) * | 2021-11-15 | 2022-02-15 | 湖北工程学院 | Biomass-based EC-g-PSSA graft copolymer and preparation method and application thereof |
| CN117317331A (en) * | 2023-11-28 | 2023-12-29 | 华中科技大学 | Positive electrode electrolyte of chromium chelate and flow battery |
| CN117855541A (en) * | 2023-12-12 | 2024-04-09 | 广州高新区能源技术研究院有限公司 | Ion exchange membrane, preparation method thereof and flow battery |
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