CN101789519A - Ionic liquid-based composite electrolyte - Google Patents
Ionic liquid-based composite electrolyte Download PDFInfo
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- CN101789519A CN101789519A CN201010100940A CN201010100940A CN101789519A CN 101789519 A CN101789519 A CN 101789519A CN 201010100940 A CN201010100940 A CN 201010100940A CN 201010100940 A CN201010100940 A CN 201010100940A CN 101789519 A CN101789519 A CN 101789519A
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Abstract
The invention discloses an all-solid-state or gel-state polymer electrolyte material with good thermal stability and excellent electrochemical performance, which is prepared by the composition with polymer material, based on ionic liquid material which is formed by the reaction between lithium bis(oxalate) borate ester and amide functional group-containing organic compound. Gel-state polymer electrolyte or all-solid-state polymer electrolyte with excellent performance is prepared by adjusting the constitution and proportion of the ionic liquid and performing addition with polymer on condition of the addition of a proper amount of plasticizer, or by directly compositing with the amide functional group-containing polymer material through conducting salts, and the electrolyte has extensive application prospect in chemical power supply, especially in the aspect of novel electrochemical energy storage system orienting the requirements of high power, high energy density and high safety.
Description
Technical field
The invention belongs to the electrolyte technical field, mainly towards the application of high energy battery such as the electrokinetic cell of high power, high-energy-density, lithium ion battery, electric chemical super capacitor, lithium-sulfur cell and electronic equipment technical field.
Technical background
The conventional ion compound at room temperature is a solid owing to strong ionic bond effect, and has high melt point, boiling point and hardness.And the introducing of big and asymmetric zwitterion, because steric restriction destroys original orderly crystal structure, the interionic effect reduces, and forms the salt that is in a liquid state under the room temperature, i.e. room temperature fused salt (ionic liquid, Ionic liquids).Ionic liquid is the liquid of being made up of ion fully, is the salt that is in a liquid state under the low temperature (＜100 ℃), generally is made up of organic cation and inorganic anion.Ionic liquid is being subjected to extensive attention as green solvent aspect organic and the Polymer Synthesizing in recent years, and has carried out deep research aspect electrochemistry.Compare with electrolyte with traditional organic solvent, ionic liquid has a series of outstanding advantages: (1) does not almost have vapour pressure, and is non-volatile; Colourless, nothing is smelt; (2) has bigger stable temperature scope, the electrochemical stability potential window of better chemical stability and broad; (3) its dissolubility of design scalable by zwitterion to inorganic matter, water, organic substance and polymer, and its acidity can transfer to super acid or the like.At present synthetic, the physical and chemical performance that ion liquid research is mainly concentrated on novel ion liquid characterizes and as aspects such as solvent and electrolyte electrochemical application.
The advantage of present widely used liquid electrolyte is the conductivity height, but owing to contain inflammable, volatile organic solvent, it discharges fuel gas in charge and discharge process, particularly under some unconventional condition of work (as high-powerly discharge and recharge, super-charge super-discharge etc.) generation that produces big calorimetric meeting accelerating gas, cause inner pressure of battery to increase, gas-liquid is leaked, even blast on fire, thereby has serious potential safety hazard.Liquid electrolytic plastidome also exists poor heat stability, the high deficiency of solidifying point simultaneously, and conductivity sharply descends at low temperatures, and electrolyte easily decomposes rotten under the high temperature.These problems have all seriously restricted the particularly development of high-power performance of novel battery and capacitor.
The objective of the invention is provides a kind of safe, ionic liquid-based composite electrolyte that chemical property is good for the deficiency that solves prior art.This electrolytical main constituent, both by under di-oxalate lithium borate and the room temperature be organic compound solid, dystectic amide-containing functional group mixed ionic liquid.Di-oxalate lithium borate (LiBOB) has the chemical property of high decomposition temperature and stability, and particularly than traditional lithium salts, the filming performance on the high-temperature stability of LiBOB and graphite-like negative material surface is remarkable.Corresponding to the anodal battery of forming of the Ni-based mixed oxide of graphite cathode and lithium, there is not significant capacity attenuation at 60 ℃ of higher temperatures or 70 ℃ of following circulation times based on the electrolyte of LiBOB.Research is simultaneously also found, at spinelle LiMnO
2, LiCo
1/3Ni
1/3Mn
1/3O
2And LiFePO
4In several anode material for lithium-ion batteries, under the condition of overcharging, the heat that uses LiBOB electrolyte to be produced is lower than use LiPF
6Electrolyte.This shows that LiBOB electrolyte can effectively improve the thermal stability of anodal and negative material, significantly improves the fail safe of lithium ion battery.The eighties in 20th century occurred the low-temperature molten salt that a class is made up of acid amides and alkali nitrates or ammonium nitrate, discovered, urea (mol ratio χ=0.591)-NH
4NO
3(mol ratio χ=0.409) (fusing point T
m=63.5 ℃), urea-acetamide-NH
4NO
3(fusing point T
m==7 ℃) etc. the fused salt that forms of nitrate and short-chain fat amine have tangible super cooling tendency, crossing the sloppy heat body, can both to keep the liquid state a few days-20 ℃ under be to cause the several months.Caldeira etc. have studied the room temperature fused salt of urea-acetamide-alkali nitrates or ammonium nitrate composition, and its room-temperature conductivity is higher than 10
-3Scm
-1, electrochemical window is about 2V, can be used as battery such as normal temperature lithium thermal cell or surface-treated electrolyte such as titanium and titanium alloy anode oxidation.Zhao Yingxin etc. separate out with the crystal of inhibition system by polyethylene glycol oxide being added in urea-acetamide-alkali metal lithium nitrate low-temperature eutectic salt.The new type low temperature fused salt that MacFarlane etc. design is the plastic crystal network, and this kind lattice has rotation randomness and have the room, but lithium ion doped wherein after fast moving.This seminar has successively reported the ionic liquid of several classes based on LiTFSI and amide-containing functional group organic substance (as urea etc.), physical and chemical performance studies show that system has good thermal stability and chemical property, and synthetic easily, raw material is cheap.In the above-mentioned research, the organic compound of amide-containing functional group has the physical characteristic (high-k and dissociation constant) like water more, therefore often be used to organicly or inorganic compound forms in the research of eutectic system, can effectively reduce the fusing point of hybrid system with other.
Compare with the traditional liquid electrolyte, thermal stability height, the conductivity of the ion liquid system that is prepared by above-mentioned two class materials is big, electrochemical window is wide, can effectively be used in electrochemical systems such as lithium ion battery, capacitor.By directly carrying out compound ionic liquid and macromolecular material or conducting salt with the macromolecular material that contains amide groups functional group, and add an amount of plasticizer and prepare full solid state polymer electrolyte or gel polymer electrolyte, it not only has the characteristics that thermoplastic polymer easily shapes, realize that simultaneously barrier film contacts with the complete of electrode, improved the compactness of adhering at interface, thereby reduced the interface impedance and the internal resistance of cell of electrolyte and electrode, helped large current density.In conjunction with characteristics such as its Heat stability is good, ionic conductivity height, chemical property be good, therefore can produce, be easy to design continuously, technology is simple, safe, at aspects such as lithium ion battery, electric chemical super capacitors wide application prospect is arranged, also be applicable to a plurality of fields such as communication, Aero-Space, new-energy automobile of demand high security, high-energy-density and high-power novel physical chemistry power supply.
Summary of the invention
Main contents of the present invention are:
1. ionic liquid-based composite electrolyte is characterized in that: the ionic liquid that this ionic liquid-based composite electrolyte is formed by two oxalic acid borate lithiums and the organic compound effect that contains amide groups functional group as main constituent and: all solid state material that 1. is composited, does not contain or contain small amount of plasticizer with macromolecular material; 2. the gel state material that is composited with macromolecular material and a large amount of plasticizer; Perhaps this ionic liquid-based composite electrolyte by two oxalic acid borate lithiums directly with the macromolecular material that contains amide groups functional group compound and: 1. do not contain or add small amount of plasticizer and all solid state material that forms; 2. the gel state material that adds a large amount of plasticizer and form;
Described pair of oxalic acid borate lithium structure is as follows:
The described organic compound that contains amide groups functional group is a kind of in the following structure at least:
R wherein
1-R
5Identical or different, optionally by the direct keyed jointing mutually of singly-bound or two key, and have following implication :-H ,-halogen ,-phenyl ,-trifluoromethyl or-alkyl; Wherein the H in the alkyl can partially or completely be replaced by other groups; The above-mentioned organic compound that contains amide groups functional group can be urea, methyl urea, dimethyl urea, dimethyl formamide, tetramethylurea, acetamide, antifebrin, lactams, pyrrolidones, N-methylacetamide, trifluoroacetyl aniline, imidazolone, N-N-dimethyl-imidazolinone etc.;
Described macromolecular material is the polyethers based material based on polyethylene glycol oxide at least, reaches by copolymerization, doping salt, adds the porous polyoxyethylene film that improved polymer electrolyte of plasticizer or fiber or powder strengthen; It with the polyacrylonitrile porous polypropylene nitrile film that the polymer dielectric of base or copolymerization, plasticising prepare; Polymethacrylates; Kynoar based polymer and porous Kynoar paraphase film or noninvert film; Polypropylene, polythene material and composite membrane thereof; Poly-phosphine piperazine; Multiple polymers is compound or add a kind of in the composite polymeric materials that inorganic powder prepares;
Described plasticizer comprises carbonic ester; Carboxylic acid esters; Sulfurous esters; Organic phosphorus compound; Silanes; Ethers; Low molecular polymer; In the above-mentioned organic solvent: carbonates can be vinyl carbonate, propylene carbonate, butylene carbonic ester, diethyl carbonate, dimethyl carbonate, the first and second basic carbonic esters, three fluoro propene carbonates etc.; Carboxylic acid esters can be toluic acid ester, methyl acetic acid ester, methylpropionate, butyrolactone, two fluoro ethyl acetate, two fluoro methyl acetates etc.; Sulfurous esters can be ethylene sulfite, propylene sulfite, sulfurous acid butene esters, diethyl sulfite, dimethyl sulfite, the first and second basic sulfites etc.; Organic phosphorus compound can be alkyl phosphate (as trimethyl phosphate, triethyl phosphate, tributyl phosphate, triphenyl phosphate, dimethyl methyl phosphonate acid esters, propylidene etherophosphoric acid), alkyl phosphite ester (Trimethyl phosphite, three-(2,2, the 2-trifluoroethyl) phosphite ester), the fluorinated phosphate ester (three-(2,2, the 2-trifluoroethyl) phosphate, two-(2,2, the 2-trifluoroethyl)-methyl phosphorodithioate, (2,2,2-trifluoroethyl)-diethyl phosphate, benzene octyl group phosphate) and phosphonitrile compounds (as the hexamethyl phosphonitrile); Silanes can be tetramethoxy-silicane, tetraethoxysilane, methyltrimethoxy silane, methyl triethoxysilane etc.; Ethers can be that dimethoxymethane, dimethoxy ethane, diethoxyethane, epoxy hexane, epoxy pentane, oxolane, fluoromethane are for butyl ether etc.; In the full solid state polymer electrolyte material, the shared mass ratio of plasticizer is in 0%～5% scope; In the gel-type polymer electrolyte material, the shared mass percent of plasticizer is in 20～80% scopes;
The described macromolecular material that contains amide groups functional group promptly has-polymer-polyamide of NHCO-group, comprises and contains the described precursor structure of claim 3 in the polymer monomer structure; Polyamide can be polyamide-6 ([NH (CH
2)
5CO]), polyamide-66 ([NH (CH
2)
6NHCO (CH
2)
4CO]) and polyamide-610 ([NH (CH
2)
6NHCO (CH
2)
8CO]) etc.
2. a kind of ionic liquid-based composite electrolyte according to claim 1, it is characterized in that: by the composition and the proportioning of lithium salts and organic compound in the adjusting ionic liquid, carry out addition with macromolecular material, plasticizer, or directly compound with the macromolecular material that contains amide groups functional group, form all solid state or ionic liquid-based composite electrolyte of gel state.
Below in conjunction with embodiment the present invention is done further narration:
Embodiment:
Embodiment 1:
To put into glove box after two oxalic acid borate lithiums and the urea drying, weighing 10g and 20g sample mix in measuring cup respectively, at room temperature form homogeneous liquid through fully stirring, and obtain ionic liquid, and its conductivity (25 ℃) is 1mS/cm.
Based on the good electrochemistry of above-mentioned ionic liquid, thermal property, itself and porous polyoxyethylene film is compound, and 25 ℃ of conductivity of room temperature can reach 0.26mS/cm; Conductivity under the sample different temperatures is measured, and conductivity varies with temperature curved line relation and meets the Arrhenius equation.
Embodiment 2:
To put into glove box after two oxalic acid borate lithiums and the methyl urea drying, weighing 10g and 20g sample mix in measuring cup respectively, at room temperature form homogeneous liquid through fully stirring, and obtain ionic liquid, and its conductivity (25 ℃) is 0.4mS/cm.Itself and vinylidene fluoride-hexafluoropropylene copolymer and EC+PC plasticizer are compounded to form gel polymer electrolyte.
Embodiment 3:
To put into glove box after two oxalic acid borate lithiums and the dimethyl urea drying, weighing 10g and 20g sample mix in measuring cup respectively, at room temperature form homogeneous liquid through fully stirring, and obtain ionic liquid, and its conductivity (25 ℃) is 2.1mS/cm.Itself and polyethylene film is compound, and 25 ℃ of conductivity of room temperature can reach 0.48mS/cm; Itself and vinylidene fluoride-hexafluoropropylene copolymer and EC+ oxolane plasticizer are compounded to form gel polymer electrolyte, and 25 ℃ of conductivity of room temperature can reach 1.5mS/cm; Respectively that itself and porous polyoxyethylene film, porous polypropylene nitrile film, polymethacrylates, poly-phosphine piperazine is compound, the PC+ gamma-butyrolacton of interpolation 20% and 1% propylene sulfite+triethyl phosphate obtain stable ionic liquid compound electrolyte as plasticizer.
Embodiment 4:
Put into glove box after two oxalic acid borate lithiums of weighing 10g and the caprolactam drying of 25g and mix, after heating abundant stirring, form homogeneous liquid, obtain ionic liquid after naturally cooling to room temperature.System is stable, shelves in glove box for a long time, all keeps stable liquid state.It is combined formation composite gel type polymer dielectric with Kynoar or vinylidene fluoride-hexafluoropropylene copolymer.
Embodiment 5:
To put into glove box after two oxalic acid borate lithiums and the imidazolone drying, weighing 10g and 30g sample mix in measuring cup respectively, form homogeneous liquid after heating abundant stirring, obtain ionic liquid after naturally cooling to room temperature.Itself and polypropylene screen is compound, obtain ionic liquid-based composite electrolyte.
Embodiment 6:
To put into glove box after two oxalic acid borate lithiums and the N-N-dimethyl-imidazolinone drying, weighing 10g and 30g sample mix in measuring cup respectively, obtain ionic liquid after fully stirring formation homogeneous liquid, and conductivity (25 ℃) is 3.6mS/cm.With itself and interpolation nanometer SiO
2Vinylidene fluoride-hexafluoropropylene copolymer and EC+PC plasticizer compound, all obtain the stabilizing gel polymer dielectric.
Embodiment 7:
Put into glove box after two oxalic acid borate lithiums of weighing 10g and the pyrrolidones drying of 25g and mix, after heating abundant stirring, form homogeneous liquid, obtain ionic liquid after naturally cooling to room temperature.System is stable, shelves in glove box for a long time, all keeps stable liquid state.Itself and polypropylene screen is compound, obtain ionic liquid-based composite electrolyte.
Embodiment 8:
To put into glove box after two oxalic acid borate lithiums and the tetramethylurea drying, weighing 10g and 25g sample mix in measuring cup respectively, form homogeneous liquid after heating abundant stirring, obtain ionic liquid after naturally cooling to room temperature.Itself and porous polyoxyethylene film is compound, obtain all solid state ionic liquid-based composite electrolyte.
Embodiment 9:
To put into glove box after two oxalic acid borate lithiums and the acetamide drying, weighing 10g and 25g sample mix in measuring cup respectively, at room temperature form homogeneous liquid through fully stirring, and obtain ionic liquid, and its conductivity (25 ℃) is 2.4mS/cm.
Based on the good electrochemistry of above-mentioned ionic liquid, thermal property, itself and porous polyoxyethylene film is compound, and 25 ℃ of conductivity of room temperature can reach 0.82mS/cm; Conductivity under the sample different temperatures is measured, and conductivity varies with temperature curved line relation and meets the Arrhenius equation.
Embodiment 10:
Based on good electrochemistry, the thermal property of embodiment 9 preparation ionic liquids, itself and polyacrylonitrile film is compound, and 25 ℃ of conductivity of room temperature can reach 0.65mS/cm; Conductivity under the sample different temperatures is measured, and conductivity varies with temperature curved line relation and meets the Arrhenius equation.
Embodiment 11:
Based on good electrochemistry, the thermal property of embodiment 9 preparation ionic liquids, itself and vinylidene fluoride-hexafluoropropylene copolymer and EC+PC plasticizer are compounded to form gel polymer electrolyte.This plural gel polymer dielectric is packed in the Analog battery die, and pole piece is a stainless steel substrates, and take out from glove box the sealing back.Use the CHI660a electrochemical workstation to adopt the AC impedance method to measure its conductivity in the 1Hz-100KHz scope, 25 ℃ of conductivity of room temperature can reach 1.3mS/cm.
Embodiment 12:
Based on good electrochemistry, the thermal property of embodiment 9 preparation ionic liquids, respectively that itself and porous polyoxyethylene film, porous polypropylene nitrile film, polymethacrylates, poly-phosphine piperazine is compound, the PC+ gamma-butyrolacton of interpolation 20% and 1% propylene sulfite+triethyl phosphate obtain stable ionic liquid-based composite electrolyte as plasticizer.
Embodiment 13:
Two oxalic acid borate lithiums and polyamide-6 is compound and add 20% butyrolactone film forming, obtain the gel-type polymer electrolyte material, membrane surface is evenly smooth.
Embodiment 14:
Two oxalic acid borate lithiums and polyamide-66 is compound and add 2% oxolane+2% sulfurous acid butene esters film forming, obtain the full solid state polymer electrolyte material, barrier film has excellent mechanical intensity.
Embodiment 15:
Two oxalic acid borate lithiums and polyamide-610 is compound and add 20% butyrolactone film forming, obtain the gel-type polymer electrolyte material, membrane surface is evenly smooth.
Embodiment 16:
Two oxalic acid borate lithiums are directly compound and add 5% epoxy hexane film forming with polyamide-6, polyamide-66 and polyamide-610 respectively, obtain the full solid state polymer electrolyte material, barrier film has excellent mechanical intensity.
Claims (2)
1. ionic liquid-based composite electrolyte is characterized in that: the ionic liquid that this ionic liquid-based composite electrolyte is formed by two oxalic acid borate lithiums and the organic compound effect that contains amide groups functional group as main constituent and: all solid state material that 1. is composited, does not contain or contain small amount of plasticizer with macromolecular material; 2. the gel state material that is composited with macromolecular material and a large amount of plasticizer; Perhaps this ionic liquid-based composite electrolyte by two oxalic acid borate lithiums directly with the macromolecular material that contains amide groups functional group compound and: 1. do not contain or add small amount of plasticizer and all solid state material that forms; 2. the gel state material that adds a large amount of plasticizer and form;
Described pair of oxalic acid borate lithium structure is as follows:
The described organic compound that contains amide groups functional group is a kind of in the following structure at least:
R wherein
1-R
5Identical or different, optionally by the direct keyed jointing mutually of singly-bound or two key, and have following implication :-H ,-halogen ,-phenyl ,-trifluoromethyl or-alkyl; Wherein the H in the alkyl can partially or completely be replaced by other groups;
Described macromolecular material is the polyethers based material based on polyethylene glycol oxide at least, reaches by copolymerization, doping salt, adds the porous polyoxyethylene film that improved polymer electrolyte of plasticizer or fiber or powder strengthen; It with the polyacrylonitrile porous polypropylene nitrile film that the polymer dielectric of base or copolymerization, plasticising prepare; Polymethacrylates; Kynoar based polymer and porous Kynoar paraphase film or noninvert film; Polypropylene, polythene material and composite membrane thereof; Poly-phosphine piperazine; Multiple polymers is compound or add a kind of in the composite polymeric materials that inorganic powder prepares;
Described plasticizer comprises carbonic ester; Carboxylic acid esters; Sulfurous esters; Organic phosphorus compound; Silanes; Ethers; Low molecular polymer;
In the full solid state polymer electrolyte material, the shared mass ratio of plasticizer is in 0%～5% scope; In the gel-type polymer electrolyte material, the shared mass percent of plasticizer is in 20～80% scopes;
The described macromolecular material that contains amide groups functional group promptly has-polymer-polyamide of NHCO-group, comprises and contains the described precursor structure of claim 3 in the polymer monomer structure.
2. a kind of ionic liquid-based composite electrolyte according to claim 1, it is characterized in that: by the composition and the proportioning of lithium salts and organic compound in the adjusting ionic liquid, carry out addition with macromolecular material, plasticizer, or directly compound with the macromolecular material that contains amide groups functional group, form all solid state or ionic liquid-based composite electrolyte of gel state.
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|---|---|---|---|
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102130364A (en) * | 2011-02-12 | 2011-07-20 | 中南大学 | Gel-type polymer electrolyte used for lithium-sulfur secondary battery system and preparation method |
| CN102208680A (en) * | 2011-05-05 | 2011-10-05 | 中国东方电气集团有限公司 | Gel electrolyte and preparation method thereof and corresponding anode and lithium sulfur battery |
| CN103151560A (en) * | 2013-02-05 | 2013-06-12 | 东莞新能源科技有限公司 | Lithium ion battery electrolyte solution and its additive |
| CN105745778A (en) * | 2013-08-29 | 2016-07-06 | 联邦科学和工业研究机构 | Lithium-sulfur electric current producing cell |
| CN106229547A (en) * | 2016-09-20 | 2016-12-14 | 复旦大学 | A kind of boracic solid polymer electrolyte and its preparation method and application |
| CN107623103A (en) * | 2016-07-14 | 2018-01-23 | 福特全球技术公司 | Lithium sulfur battery cells electrode |
| CN110998951A (en) * | 2017-08-10 | 2020-04-10 | 仓敷纺绩株式会社 | Electrode sheet manufacturing method, all-solid-state battery, and all-solid-state battery manufacturing method |
| CN112701346A (en) * | 2019-10-22 | 2021-04-23 | 辉能科技股份有限公司 | Solid electrolyte contact surface conditioning material and mixed electrolyte system thereof |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100516126C (en) * | 2006-09-06 | 2009-07-22 | 北京理工大学 | Ion liquid |
-
2010
- 2010-01-25 CN CN201010100940.XA patent/CN101789519B/en active Active
Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102130364A (en) * | 2011-02-12 | 2011-07-20 | 中南大学 | Gel-type polymer electrolyte used for lithium-sulfur secondary battery system and preparation method |
| CN102208680A (en) * | 2011-05-05 | 2011-10-05 | 中国东方电气集团有限公司 | Gel electrolyte and preparation method thereof and corresponding anode and lithium sulfur battery |
| CN103151560A (en) * | 2013-02-05 | 2013-06-12 | 东莞新能源科技有限公司 | Lithium ion battery electrolyte solution and its additive |
| CN103151560B (en) * | 2013-02-05 | 2017-04-26 | 东莞新能源科技有限公司 | Lithium ion battery electrolyte solution and its additive |
| CN105745778A (en) * | 2013-08-29 | 2016-07-06 | 联邦科学和工业研究机构 | Lithium-sulfur electric current producing cell |
| CN105745778B (en) * | 2013-08-29 | 2019-06-28 | 联邦科学和工业研究机构 | Generate the lithium-sulfur cell of electric current |
| CN107623103A (en) * | 2016-07-14 | 2018-01-23 | 福特全球技术公司 | Lithium sulfur battery cells electrode |
| CN106229547A (en) * | 2016-09-20 | 2016-12-14 | 复旦大学 | A kind of boracic solid polymer electrolyte and its preparation method and application |
| CN110998951A (en) * | 2017-08-10 | 2020-04-10 | 仓敷纺绩株式会社 | Electrode sheet manufacturing method, all-solid-state battery, and all-solid-state battery manufacturing method |
| CN112701346A (en) * | 2019-10-22 | 2021-04-23 | 辉能科技股份有限公司 | Solid electrolyte contact surface conditioning material and mixed electrolyte system thereof |
| TWI737011B (en) * | 2019-10-22 | 2021-08-21 | 輝能科技股份有限公司 | Adjusting material for contact surface of solid electrolyte and composite electrolyte system thereof |
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| CN101789519B (en) | 2014-06-04 |
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