CN102856520A - Diaphragm for electrochemical power source system with nonsolid-state electrode and preparation method thereof - Google Patents
Diaphragm for electrochemical power source system with nonsolid-state electrode and preparation method thereof Download PDFInfo
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- CN102856520A CN102856520A CN2012100174875A CN201210017487A CN102856520A CN 102856520 A CN102856520 A CN 102856520A CN 2012100174875 A CN2012100174875 A CN 2012100174875A CN 201210017487 A CN201210017487 A CN 201210017487A CN 102856520 A CN102856520 A CN 102856520A
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- barrier film
- power source
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- source system
- state electrode
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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
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The invention relates to a diaphragm for a nonsolid-state electrode system, and components are selected from organic high-molecular polymers, and preferably selected from one or more than one of PMMA, PP, PE, PVDF, PTFE, PVA, PVC, PAN, PEO, CMC, starch, and polyacrylate lithium; the diaphragm allows alkali metal, alkaline earth metal ions or hydrogen ions to pass through, and does not allows transition metal ions to pass through. The diaphragm is low in manufacturing cost, easy to realize industrialization, and has potential application value in fields such as flow cells, air cells, and fuel cells.
Description
Technical field
The invention belongs to field of chemical power source, relate to the barrier film that a kind of chemical power source uses, specifically, the present invention relates to a kind of negative or positive electrode all or one of them is the non-solid-state used barrier film of battery system.
Background technology
Energy can exist with the form of solid, liquid or gas, and correspondingly, as the storage of energy with transform device, that chemical power source can adopt is solid-state, the electrode of liquid state or gaseous state.Solid state electrode is modal form.The primary cell such as alkaline Mn cell, zinc-silver oxide cell, lithium ion battery, lead-acid battery, Hawkins cell, ickel-cadmium cell, Ni-H cell, zinc-nickel cell, oxygen inflatable silver battery, can fill the secondary cells such as alkaline Mn cell, and electrochemical capacitor, its electrode that adopts is solid state electrode.In this class battery, because electronics is tied between electrode and the metallic conductor, be not need barrier film in theory, just for preventing that hypotelorism causes short circuit just to adopt barrier film between the positive and negative electrode.Therefore it is very simple to the barrier film requirement, as long as energy conducting ion has electronic isolation just.
Solid electrode has certain disadvantages, the dynamic performance that for example reaction mechanism of the mutually transformation of complexity and complications causes in the charge and discharge process is not enough, the manufacture craft process is drawn oversize and cause that cost rises, degradation under the qualification rate, impel people to consider other electrode shape.
The metal-air cell that uses at present or see, lithium addition, lithium thionyl chloride cell, zinc-bromine bettery and all-vanadium flow battery, siderochrome flow battery, hydrogen fuel cell etc., at least one electrode is in a liquid state or gaseous state in its negative or positive electrode, and have two kinds all are in a liquid state or all are gaseous state.This class battery is because good liquid or the gas of employing diffusion is electrode, can increase the compatibility with equipment, improve the flexibility of design and to the utilance in space, and can be with the quick charge of mechanical charge mode, in the electric automobile field great development potentiality is arranged, thereby development in recent years enjoys attention.Yet such battery is had relatively high expectations to barrier film, be that barrier film not only will be blocked electronics, also to block some ion wherein, preventing that it from carrying electronics and passing through, and cause internal short-circuit, simultaneously, the ion that allows not carry electronics passes through barrier film, to keep the inside battery charge balance, that is to say that this barrier film will have ion selectivity.
The ion selective membrane that satisfies at present above-mentioned requirements is the barrier film of a kind of being called as " amberplex ", its action principle is to have specific atoms group on this film, and this atomic group only has effect and exchange reaction occurs with specific ion, other ions can not carry out with it exchange reaction, thereby reach the purpose that only allows specific ion to pass through.General amberplex is the sulfonic group polymeric membrane, or inorganic solid electrolyte film, the Nafion film of for example commonly using in flow battery and the fuel cell, and the used solid-state ceramic film of high-temperature battery, itself or price are very high, and for example the present external product price of organic sulfonate polymeric membrane price surpasses 10,000 yuan of every square meters; The normal temperature ionic conducting property is poor, and the ionic conductivity of solid-state ceramic film is very low, to such an extent as to can't at room temperature use, only can be applied to the high temperature occasion, thereby cause large-area applications to be obstructed.
Summary of the invention
The technical problem to be solved in the present invention is that the barrier film cost of existing non-solid state electrode use is too high, is not suitable for promoting on a large scale.The invention provides the ion blocking-up property film of a kind of low cost, room-temperature applications, it is to realize ion selectivity by the blocking-up larger solvation ion of some volume, so be called ion blocking-up property film, is applied in the non-solid state electrode system.Ion blocking-up property film manufacturing method of the present invention is simple, cost is low, is easy to realize industrialization, has potential using value in flow battery, air cell and fuel cell field.
A kind of non-solid state electrode system provided by the invention is blocked the property film with ion, it is characterized in that its a kind of microporous barrier, its component is selected from organic high molecular polymer, preferred PMMA (polymethyl methacrylate), polypropylene (PP), polyethylene (PE), PVDF (Kynoar), PTFE (polytetrafluoroethylene), PVA (polyvinyl alcohol), PVC (polyvinyl chloride), PAN (polyacrylonitrile), PEO (polyoxyethylene), CMC (sodium carboxymethylcellulose), starch, in the Lithium polyacrylate one or more, the size of its micropore allows alkali metal, alkaline-earth metal ions or hydrogen ion etc. pass through, and transition metal ions can't pass.
As preferably, can also add additive in the component of ion blocking-up property film, to increase mechanical strength, further reduce cost etc., preferred silicon dioxide, aluminium oxide, magnesium oxide or molecular sieve.
It is the solvent extraction that the present invention also provides the preparation method of this ion barrier film: add solvent orange 2 A in membrane component, solvent orange 2 A is selected from one or more mixtures in water, methyl alcohol, ethanol, ether, oxolane, dioxane, dioxolane, acetone, 1-Methyl-2-Pyrrolidone, dimethyl sulfoxide (DMSO), sulfolane, dimethyl formamide, the carbonates material etc., is prepared into film; Then with the solvent orange 2 A volatilization, making solvent proportion in whole barrier film is 0.1-5%; Again this barrier film immersed solvent B thereafter, residual solvent A dissolves in solvent B gradually, form microporous barrier, solvent B is selected from one or more mixtures in water, methyl alcohol, ethanol, ether, oxolane, dioxane, dioxolane, acetone, 1-Methyl-2-Pyrrolidone, dimethyl sulfoxide (DMSO), sulfolane, dimethyl formamide, the carbonates material etc., its selection principle is that solvent B can dissolve the residual solvent A in the matrix, but matrix that can not dissolving film.
In solvent extraction, can in membrane component, add the additive that dissolves in solvent B, to increase the uniformity of micropore, soluble additive is selected from customary acid, alkali and salt, preferably with electrolyte middle-jiao yang, function of the spleen and stomach Ion Phase acid, alkali and salt together, more preferably electrolyte itself.
The preparation method of the second ion barrier film provided by the invention is the situ extracting method: add solvent orange 2 A in membrane component, solvent orange 2 A is selected from one or more mixtures in water, methyl alcohol, ethanol, ether, oxolane, dioxane, dioxolane, acetone, 1-Methyl-2-Pyrrolidone, dimethyl sulfoxide (DMSO), sulfolane, dimethyl formamide, the carbonates material etc., is prepared into film; Then with the solvent orange 2 A volatilization, making solvent orange 2 A proportion in whole barrier film is 0.1-5%; Then barrier film is assemblied in the battery, adds electrolyte, solvent orange 2 A is the electrolyte suitable solvents, and electrolyte extracts solvent orange 2 A remaining in the barrier film, forms the original position micropore.
In the extraction, can add the electrolyte soluble additive in membrane component in position, soluble additive is selected from customary acid, alkali and salt, preferably with electrolyte middle-jiao yang, function of the spleen and stomach Ion Phase acid, alkali and salt together, more preferably electrolyte itself.At this moment, the residual solvent of matrix or soluble additive can dissolve in solvent or electrolyte gradually in the film-forming process, thereby stay the hole in matrix, this hole size can be regulated and control with molecular size and the concentration thereof of residual solvent or soluble additive, thereby obtains ion blocking-up property film.
Block the property film by the ion that said method obtains, can form individual layer, bilayer or multilayer complex films with the film of other types, also can form composite membrane according to blend, copolymerization or crosslinked mode with the film of other types, to improve mechanical strength, to improve ionic conductivity etc.In addition, for battery system that electrode is solid in two electrodes, for example the metal-air battery system can directly be coated film the solid state electrode surface with the method for coating.
Although do not wish to be subject to the constraint of any theory, the inventor thinks that metal ion exists with the solvation ionic species in solution, transition metal ions, for example V
3+, VO
2+, Cr
3+, Fe
3+, Mn
2+, Co
2+, Ni
2+Deng solvation stronger, in solution, can form the larger solvation ion of volume, even produce chemical bond, forms stable complex, thereby this ion cluster volume increase.And light-weight metal, such as alkali metal or alkaline-earth metal ions and hydrogen ion etc., itself small volume, a little less than the solvation, compare transition metal ions, easy desolvation, this just causes the ability of this two classes ion by the ion barrier film time different, by controlling the size of the micropore that forms, less light-weight metal ion is passed through, and the solvation ion of larger transition metal can not pass through, and the film that obtains like this has ion selectivity equally, still, the homo-ion exchange membrane of this ion selectivity has essence different, it is to realize by blocking large ion, thereby is the barrier film of a class newtype, i.e. ion blocking-up property film.
The invention provides ion blocking-up type film characteristics is low cost of manufactures, is easy to realize industrialization, has potential using value in flow battery, air cell and fuel cell field." obtain the above operating voltage of 1.1V, circulating has no capacity attenuation 20 times " among the embodiment, " open circuit voltage that records battery is 0.7V, and maximum power density is 43mW/cm
2" show when it is used for non-solid state electrode barrier film, functional, consistent with the sulfonate type ion-exchange film properties that price is high.
Embodiment
The present invention below will be described in more detail by reference example, but protection scope of the present invention is not limited to these embodiment.
Embodiment 1
Get polyacrylonitrile (PAN), be dissolved in the dimethyl sulfoxide (DMSO), be mixed with the solution of concentration 5%, get this solution of 5ml, coat after mixing on porous PP-PE film, 75 ℃ of heating in vacuum 10 hours, then cover another layer PP-PE film thereon, obtain the interlayer barrier film.With soaking 3 hours in this film immersion aqueous solution, obtain solvent-extracted ion blocking-up type film.This film is assembled in the H type electrolytic cell, and both sides add respectively 1mol/L VOSO
4, 2mol/L H
2SO
4Solution and 1mol/L V
3+, 2mol/L H
2SO
4, the result obtains the above operating voltage of 1.2V.Circulating has no capacity attenuation 50 times, and its efficiency for charge-discharge is 89%, consistent with the organic sulfonic acid type amberplex that records.
Embodiment 2
Get poly-(biasfluoroethylene-hexafluoropropylene), be dissolved in the dimethyl formamide, be mixed with the solution of concentration 3%, get this solution of 5ml, to wherein adding 1% nano silicon, coat on the glass plate after mixing, 75 ℃ of heating in vacuum 12 hours.This film is assembled in the H type electrolytic cell, on one side add the mixed solution of chromium sulfate and lithium sulfate at electrolytic cell, opposite side is LiMn2O4, carbon black, and polytetrafluoroethylene is assembled in the lithium sulfate solution in the electrode that 8: 1: 1 ratios form.Along with the carrying out of charge and discharge process, both sides electrolyte extracts a small amount of dimethyl formamide gradually, obtains thus the ion barrier film of situ extracting, and the result obtains the above operating voltage of 1.1V, and circulating has no capacity attenuation 20 times.Its efficiency for charge-discharge is 97%, and the organic sulfonic acid type ion-exchange film system efficiency for charge-discharge that records under the same terms is 83%.
Embodiment 3
Get polyvinyl chloride (PVC), be dissolved in the 1-Methyl-2-Pyrrolidone (NMP), be mixed with the solution of concentration 5%, get this solution of 5ml, nmp solution 1ml to wherein adding 0.5mol/L di-oxalate lithium borate (LiBOB) coats after mixing on the LiMn2O4 electrode.The preparation method of LiMn2O4 electrode is for getting LiMn2O4, and carbon black, polytetrafluoroethylene mix in 8: 1: 1 ratios suppresses film forming, is pressed in 100 ℃ of vacuumize 10h on the nickel screen.The surface is scribbled 50 ℃ of dry 10h of LiMn2O4 electrode of PVC-LiBOB, be soaked in the 20% lithium sulfate electrolyte, obtain the micropore ion barrier film electrode through the electrolyte extraction.This electrode is immersed in the mixed solution of vanadic sulfate and lithium sulfate, the result obtains the above operating voltage of 1.2V, and circulating has no capacity attenuation 20 times.And under the same terms, capability retention only has 47% after the sulfonic acid type ion exchange membrane-LiMn2O4 electrode system circulation 20 times.
Embodiment 4
Get polymethyl methacrylate (PMMA), be dissolved in 1: 1 mixed solvent of propene carbonate-dimethyl carbonate, be mixed with the solution of concentration 5%, get this solution of 5ml, to 1: 1 mixed solution 1ml of the propene carbonate-dimethyl carbonate that wherein adds the 0.5mol/L lithium perchlorate, coat on porous PP-PE film 75 ℃ of heating in vacuum 10 hours after mixing, then cover another layer PP-PE film thereon, obtain the interlayer ion blocking-up type microporous barrier of situ extracting.This film is assembled in the H type electrolytic cell, the mixed solution that adds vanadic sulfate and lithium sulfate at electrolytic cell on one side, opposite side is LiMn2O4, carbon black, polytetrafluoroethylene is assembled in the lithium sulfate solution in the electrode of 8: 1: 1 ratio compositions, and the result obtains the above operating voltage of 1.1V, circulating has no capacity attenuation 20 times, shows that this battery system has a good application prospect.
Take above-mentioned foundation desirable embodiment of the present invention as enlightenment, by above-mentioned description, the relevant staff can in the scope that does not depart from this invention technological thought, carry out various change and modification fully.The technical scope of this invention is not limited to the content on the specification, must determine its technical scope according to the claim scope.
Claims (11)
1. chemical power source system barrier film that contains non-solid state electrode, it is characterized by it is a kind of ion blocking-up property microporous barrier, component is selected from organic high molecular polymer, only allow alkali metal, alkaline-earth metal ions or hydrogen ion etc. to pass through, and transition metal ions can't pass.
2. the chemical power source system barrier film that contains non-solid state electrode claimed in claim 1 is characterized by in the preferred PMMA of component, PP, PE, PVDF, PTFE, PVA, PVC, PAN, PEO, CMC, starch, the Lithium polyacrylate one or more.
3. the chemical power source system barrier film that contains non-solid state electrode claimed in claim 1 is characterized by the additive that contains the energy enhance mechanical strength in the component, is selected from silicon dioxide, aluminium oxide, magnesium oxide or molecular sieve.
4. the chemical power source system barrier film that contains non-solid state electrode claimed in claim 1, it is characterized by with polymeric membrane and form one or more layers composite membrane by means such as blend, crosslinked, copolymerization, polymeric membrane is selected from one or more in organic sulfonic acid basement membrane, PMMA, PP, PE, PVDF, PTFE, PVA, PVC, PAN, PEO, CMC, starch, the Lithium polyacrylate.
5. the chemical power source system barrier film that contains non-solid state electrode claimed in claim 1 is characterized by and directly coats solid state electrode or collection liquid surface, to reduce contact resistance.
6. each described chemical power source system of non-solid state electrode that contains of claim 1-5 is with the preparation method of barrier film: add solvent orange 2 A in the film matrix component, solvent orange 2 A is selected from one or more mixtures in water, ethanol, ether, oxolane, dioxane, dioxolane, acetone, 1-Methyl-2-Pyrrolidone, dimethyl sulfoxide (DMSO), sulfolane, dimethyl formamide, the carbonates material etc., is prepared into film; Then solvent orange 2 A is evaporated into content 0.1-5%; Again this barrier film immersed solvent B thereafter, solvent B is selected from one or more mixtures in water, ethanol, ether, oxolane, dioxane, dioxolane, acetone, 1-Methyl-2-Pyrrolidone, dimethyl formamide, the carbonates material etc., the feature of solvent B is that it can dissolve the residual solvent A in the matrix, but can not dissolve matrix, residual solvent A dissolves in solvent B gradually, forms microporous barrier.
7. each described chemical power source system of non-solid state electrode that contains of claim 1-5 is with the preparation method of barrier film: add solvent orange 2 A in membrane component, solvent orange 2 A is selected from one or more mixtures in water, methyl alcohol, ethanol, ether, oxolane, dioxane, dioxolane, acetone, 1-Methyl-2-Pyrrolidone, dimethyl sulfoxide (DMSO), sulfolane, dimethyl formamide, the carbonates material etc., is prepared into film; Then with the solvent orange 2 A volatilization, making solvent orange 2 A proportion in whole barrier film is 0.1-5%; Then barrier film is assemblied in the battery, adds electrolyte, solvent orange 2 A is the electrolyte suitable solvents, and electrolyte extracts solvent orange 2 A remaining in the barrier film, forms the original position micropore.
8. the chemical power source system of non-solid state electrode that contains claimed in claim 6 is characterized in that can add the additive that dissolves in solvent B in membrane component that with the preparation method of barrier film soluble additive is selected from customary acid, alkali and salt.
9. the chemical power source system of non-solid state electrode that contains claimed in claim 7 is characterized by and can add the electrolyte soluble additive in membrane component with the preparation method of barrier film, and soluble additive is selected from customary acid, alkali and salt.
10. the chemical power source system that contains non-solid state electrode claimed in claim 9 is with the preparation method of barrier film, it is characterized by soluble additive for electrolyte middle-jiao yang, function of the spleen and stomach Ion Phase with acid, alkali and salt.
11. the chemical power source system that the contains non-solid state electrode claimed in claim 10 preparation method of barrier film, it is characterized by soluble additive is electrolyte itself.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103413973A (en) * | 2013-06-19 | 2013-11-27 | 江苏科技大学 | Preparation method of PAALi-g-SiO2-doped nanofiber-based composite gel polymer electrolyte |
| CN104530588A (en) * | 2014-12-10 | 2015-04-22 | 南通瑞达电子材料有限公司 | Electrolyte film and preparation method thereof |
| CN108400365A (en) * | 2018-03-01 | 2018-08-14 | 犀望新能源科技（昆山）有限公司 | zinc-bromine flow battery |
| CN109841863A (en) * | 2017-11-28 | 2019-06-04 | 中国科学院大连化学物理研究所 | A kind of application of composite porous polymetafluoroethylefilm film in flow battery |
| CN112768836A (en) * | 2021-01-12 | 2021-05-07 | 东华大学 | Zinc ion selective transmission diaphragm and preparation method thereof |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103413973A (en) * | 2013-06-19 | 2013-11-27 | 江苏科技大学 | Preparation method of PAALi-g-SiO2-doped nanofiber-based composite gel polymer electrolyte |
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| CN112768836A (en) * | 2021-01-12 | 2021-05-07 | 东华大学 | Zinc ion selective transmission diaphragm and preparation method thereof |
| CN112768836B (en) * | 2021-01-12 | 2022-12-20 | 东华大学 | Zinc ion selective transmission diaphragm and preparation method thereof |
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