CN102956373A - Electrolyte and preparation method thereof - Google Patents
Electrolyte and preparation method thereof Download PDFInfo
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- CN102956373A CN102956373A CN2011102380016A CN201110238001A CN102956373A CN 102956373 A CN102956373 A CN 102956373A CN 2011102380016 A CN2011102380016 A CN 2011102380016A CN 201110238001 A CN201110238001 A CN 201110238001A CN 102956373 A CN102956373 A CN 102956373A
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- acid ester
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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
- Y02E60/13—Energy storage using capacitors
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- Electric Double-Layer Capacitors Or The Like (AREA)
Abstract
An electrolyte comprises methyl sulfate ionic liquid and alkylsilane dissolved in the methyl sulfate ionic liquid. The mass ratio of the methyl sulfate ionic liquid and the alkylsilane is 1:(0.001-1):0.05. In the above electrolyte, the added alkylsilane reacts with mineral acid impurities in the methyl sulfate ionic liquid, and accordingly the mineral acid impurities in the methyl sulfate ionic liquid are eliminated, the mineral acid impurities are prevented from corroding aluminum foil of a double-layer capacitor, stability of the double-layer capacitor using the methyl sulfate ionic liquid as the electrolyte can be greatly improved, the stability of the double-layer capacitor using the electrolyte can be enhanced by adding the alkylsilane, and cost is lowered.
Description
[technical field]
The present invention relates to a kind of electrolyte, relate in particular to a kind of electrolyte and compound method thereof that contains methylsulfuric acid ester salt ionic liquid.
[background technology]
Double electric layer capacitor is a kind of novel energy storage device, has the advantages such as high power density, high cycle life, fast charging and discharging performance be good, is widely used in the AC-battery power source of military field, device for mobile communication, computer and electric automobile etc.As the important component part of double electric layer capacitor, electrolyte has a significant impact the accumulate performance of double electric layer capacitor, is determining the equivalent internal resistance of capacitor, operating voltage range, accumulate capacity and working temperature and operational environment.
Ionic liquid is in room temperature or the organic liquid material that is comprised of ion fully under near the condition of room temperature.As a kind of novel electrolyte.Ionic liquid has the advantages such as electrochemical window is wide, non-volatile, not flammable, Heat stability is good as electrolyte.Methylsulfuric acid ester salt ionic liquid is one of il electrolyte that relatively has DEVELOPMENT PROSPECT because cost of material is low.Yet, containing more inorganic acids impurity in the methylsulfuric acid ester salt ionic liquid, inorganic acid can corrode the aluminium foil of double layer capacitor, and the stability of the double electric layer capacitor that causes using methylsulfuric acid ester salt ionic liquid to do electrolyte reduces.
[summary of the invention]
In view of above-mentioned condition, be necessary to provide electrolyte of a kind of stability that increases double layer capacitor and preparation method thereof.
A kind of electrolyte comprises methylsulfuric acid ester salt ionic liquid and is dissolved in alkyl silane in the described methylsulfuric acid ester salt ionic liquid that the mass ratio of described methylsulfuric acid ester salt ionic liquid and described alkyl silane is 1: 0.001～1: 0.05.
In a preferred embodiment, described alkyl silane is methyl triethyl silicane or butyl trimethylsilicane alkane.
In a preferred embodiment, described methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.
In a preferred embodiment, described imidazole salt cation is 1-butyl-3-methylimidazole cation, 1-propyl group-3-methylimidazole cation or 1-ethyl-3-methylimidazole cation, described quaternary ammonium salts cation is methyl triethyl group quaternary ammonium cation, tetraethyl quaternary ammonium cation or trimethyl propyl group quaternary ammonium cation, described pyrroles's salt cationoid is butyl methyl pyrroles cation, propyl group methylpyrrole cation or ethyl-methyl pyrroles cation, described season, the phosphonium salt cationoid was trimethyl hexyl season phosphine cation, triethyl group hexyl season phosphine cation or tri-methyl-amyl season the phosphine cation, described pyridiniujm cationoid is the butyl-pyridinium cation, pentyl pyridine cation or hexyl pyridylium.
A kind of electrolyte comprises the product that can be obtained by following chemical reaction:
Step 1, mass ratio is provided is 1: 0.001～1: 0.05 methylsulfuric acid ester salt ionic liquid and alkyl silane, contains inevitable impurity in the described methylsulfuric acid ester salt ionic liquid, and described impurity is inorganic acid;
Step 2, add alkyl silane and stirring and dissolving in the described methylsulfuric acid ester salt ionic liquid.
In a preferred embodiment, the mass ratio of described methylsulfuric acid ester salt ionic liquid and described alkyl silane is 1: 0.01～1: 0.04.
In a preferred embodiment, described alkyl silane is methyl triethyl silicane or butyl trimethylsilicane alkane.
A kind of compound method of electrolyte may further comprise the steps:
Step 1, mass ratio is provided is 1: 0.001～1: 0.05 methylsulfuric acid ester salt ionic liquid and alkyl silane;
Step 2, add described alkyl silane and stirring and dissolving in the described methylsulfuric acid ester salt ionic liquid.
In a preferred embodiment, described methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.
In a preferred embodiment, described alkyl silane is methyl triethyl silicane or butyl trimethylsilicane alkane.
Above-mentioned electrolyte, by adding alkyl silane, alkyl silane can with trifluoroacetic acid salt ionic liquid in inorganic acid impurity react, thereby remove the inorganic acid impurity in the methylsulfuric acid ester salt ionic liquid, avoid the aluminium foil of inorganic acid corrosion double layer capacitor, can improve the stability of using this methylsulfuric acid ester salt ionic liquid to do the double layer capacitor of electrolyte; And the interpolation of alkyl silane can increase the stability of the double layer capacitor that uses this electrolyte, reduces cost.
[description of drawings]
Fig. 1 is the double layer capacitor of the electrolyte among the use embodiment one and the traditional ratio capacitance of double layer capacitor under different cycle-indexes.
[embodiment]
Below in conjunction with specific embodiment electrolyte and compound method thereof are described in further details.
The electrolyte of one execution mode comprises methylsulfuric acid ester salt ionic liquid and is dissolved in alkyl silane in the described methylsulfuric acid ester salt ionic liquid that the mass ratio of described methylsulfuric acid ester salt ionic liquid and described alkyl silane is 1: 0.001～1: 0.05.
Methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.Contain inevitable inorganic acid impurity in the methylsulfuric acid ester salt ionic liquid, inorganic acid impurity is at least a in sulfuric acid and the hydrochloric acid.
Preferably, the imidazole salt cation is 1-butyl-3-methylimidazole cation, 1-propyl group-3-methylimidazole cation or 1-ethyl-3-methylimidazole cation.
Preferably, the quaternary ammonium salts cation is methyl triethyl group quaternary ammonium cation, tetraethyl quaternary ammonium cation or trimethyl propyl group quaternary ammonium cation.
Preferably, the pyroles cation is butyl methyl pyrroles cation, propyl group methylpyrrole cation or ethyl-methyl pyrroles cation.
Preferably, season the phosphonium salt cationoid be trimethyl hexyl season phosphine cation, triethyl group hexyl season phosphine cation or tri-methyl-amyl season the phosphine cation.
Preferably, the pyridiniujm cationoid is butyl-pyridinium cation, pentyl pyridine cation or hexyl pyridylium.
Alkyl silane is preferably methyl triethyl silicane or butyl trimethylsilicane alkane.Be appreciated that alkyl silane is not limited to methyl triethyl silicane or butyl trimethylsilicane alkane, so long as can with methylsulfuric acid ester salt ionic liquid in inorganic acid impurity react and get final product.
The mass ratio of methylsulfuric acid ester salt ionic liquid and alkyl silane is preferably 1: 0.01～and 1: 0.04.
Above-mentioned electrolyte, by adding alkyl silane, inorganic acid thereby the inorganic acid impurity in alkyl silane and the methylsulfuric acid ester salt ionic liquid reacts in the removal methylsulfuric acid ester salt ionic liquid, avoid the aluminium foil of inorganic acid corrosion double layer capacitor, can greatly improve the stability of using this methylsulfuric acid ester salt ionic liquid to do the double layer capacitor of electrolyte; And the interpolation of alkyl silane can increase the stability of the double layer capacitor that uses this electrolyte, reduces cost.
The electrolyte of one execution mode comprises the product that can be obtained by following chemical reaction:
Step 1, mass ratio is provided is 1: 0.001～1: 0.05 methylsulfuric acid ester salt ionic liquid and alkyl silane, contains inevitable impurity in the methylsulfuric acid ester salt ionic liquid, and described impurity is inorganic acid.
Methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.
Preferably, the imidazole salt cation is 1-butyl-3-methylimidazole cation, 1-propyl group-3-methylimidazole cation or 1-ethyl-3-methylimidazole cation.
Preferably, the quaternary ammonium salts cation is methyl triethyl group quaternary ammonium cation, tetraethyl quaternary ammonium cation or trimethyl propyl group quaternary ammonium cation.
Preferably, the pyroles cation is butyl methyl pyrroles cation, propyl group methylpyrrole cation or ethyl-methyl pyrroles cation.
Preferably, season the phosphonium salt cationoid be trimethyl hexyl season phosphine cation, triethyl group hexyl season phosphine cation or tri-methyl-amyl season the phosphine cation.
Preferably, the pyridiniujm cationoid is butyl-pyridinium cation, pentyl pyridine cation or hexyl pyridylium.
Inorganic acid is a kind of in sulfuric acid and the hydrochloric acid.
Alkyl silane is preferably methyl triethyl silicane or butyl trimethylsilicane alkane.Be appreciated that alkyl silane is not limited to methyl triethyl silicane or butyl trimethylsilicane alkane, so long as can with methylsulfuric acid ester salt ionic liquid in inorganic acid impurity react and get final product.
The mass ratio of methylsulfuric acid ester salt ionic liquid and alkyl silane is preferably 1: 0.01～and 1: 0.04.
Step 2, add alkyl silane and stirring and dissolving in the methylsulfuric acid ester salt ionic liquid.
When above-mentioned electrolyte prepares, by in methylsulfuric acid ester salt ionic liquid, adding alkyl silane, thereby the inorganic acid in the methylsulfuric acid ester salt ionic liquid occurs to remove in the inorganic acid impurity in alkyl silane and the methylsulfuric acid ester salt ionic liquid, avoid the aluminium foil of inorganic acid corrosion double layer capacitor, can greatly improve the stability of using this methylsulfuric acid ester salt ionic liquid to do the double layer capacitor of electrolyte; And the interpolation of alkyl silane can increase the stability of the double layer capacitor that uses this electrolyte, reduces cost.
The compound method of the electrolyte of one execution mode may further comprise the steps:
Step 1, mass ratio is provided is 1: 0.001～1: 0.05 methylsulfuric acid ester salt ionic liquid and alkyl silane.
Methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.Contain inevitable inorganic acid impurity in the methylsulfuric acid ester salt ionic liquid, inorganic acid impurity is at least a in sulfuric acid and the hydrochloric acid.
Preferably, the imidazole salt cation is 1-butyl-3-methylimidazole cation, 1-propyl group-3-methylimidazole cation or 1-ethyl-3-methylimidazole cation.
Preferably, the quaternary ammonium salts cation is methyl triethyl group quaternary ammonium cation, tetraethyl quaternary ammonium cation or trimethyl propyl group quaternary ammonium cation.
Preferably, the pyroles cation is butyl methyl pyrroles cation, propyl group methylpyrrole cation or ethyl-methyl pyrroles cation.
Preferably, season the phosphonium salt cationoid be trimethyl hexyl season phosphine cation, triethyl group hexyl season phosphine cation or tri-methyl-amyl season the phosphine cation.
Preferably, the pyridiniujm cationoid is butyl-pyridinium cation, pentyl pyridine cation or hexyl pyridylium.
Alkyl silane is preferably methyl triethyl silicane or butyl trimethylsilicane alkane.Be appreciated that alkyl silane is not limited to methyl triethyl silicane or butyl trimethylsilicane alkane, so long as can with methylsulfuric acid ester salt ionic liquid in inorganic acid impurity react and get final product.
The mass ratio of methylsulfuric acid ester salt ionic liquid and alkyl silane is preferably 1: 0.01～and 1: 0.04.
Step 2, add alkyl silane and stirring and dissolving in the methylsulfuric acid ester salt ionic liquid.
The compound method of above-mentioned electrolyte, in methylsulfuric acid ester salt ionic liquid, add alkyl silane, thereby the inorganic acid in the methylsulfuric acid ester salt ionic liquid occurs to remove in the inorganic acid impurity in alkyl silane and the methylsulfuric acid ester salt ionic liquid, avoid the aluminium foil of inorganic acid corrosion double layer capacitor, can greatly improve the stability of using this methylsulfuric acid ester salt ionic liquid to do the double layer capacitor of electrolyte; And the interpolation of alkyl silane can increase the stability of the double layer capacitor that uses this electrolyte, reduces cost.
Below be the embodiment part:
Embodiment one
Alkyl silane is added in the methylsulfuric acid ester salt ionic liquid, be stirred to dissolving and can obtain electrolyte.
In the present embodiment, alkyl silane is the methyl triethyl silicane, and methylsulfuric acid ester salt ionic liquid is 1-ethyl-3-methylimidazole methylsulfuric acid ester salt, and the mass ratio of methylsulfuric acid ester salt ionic liquid and alkyl silane is 1: 0.04.
In the present embodiment, during preparation electrolyte, in glove box, carry out, with stirring in the methyl triethyl silicane adding 1-ethyl-3-methylimidazole methylsulfuric acid ester salt methyl triethyl silicane is dissolved in the 1-ethyl-3-methylimidazole methylsulfuric acid ester salt.
Above-mentioned electrolyte is applied to double layer capacitor and measures this double layer capacitor stability.
During measuring stability, take Graphene as electrode material, use the electrolyte of embodiment one preparation, be assembled into button cell, utilize the CHI660A electrochemical workstation that it is carried out the constant current charge-discharge test, record it than electric capacity conservation rate, namely under 30 degrees celsius, in 0～2.5v window ranges, with the ratio electric capacity and the ratio of first charge-discharge than electric capacity after 1000 circulations of constant current repeated charge of 1A/g.
See also Fig. 1, Fig. 1 does not add the methylsulfuric acid ester salt ionic liquid of methyl triethyl silicane as the ratio capacitance of double layer capacitor under different cycle-indexes of electrolyte for the double layer capacitor that uses the electrolyte in the present embodiment from use.As can be seen from Figure 1, use the first charge-discharge of the double layer capacitor of the electrolyte that the present embodiment provides to be 108.66F/g than electric capacity, the ratio electric capacity that circulates after 1000 times is 102.48F/g, and its conservation rate is 94.31%; And use the methylsulfuric acid ester salt ionic liquid that do not add the methyl triethyl silicane to be 108.7F/g as the first charge-discharge of the double layer capacitor of electrolyte than electric capacity, and the ratio electric capacity that circulates after 1000 times is 83.03F/g, its conservation rate is 76.38%; Use the present embodiment electrolyte double layer capacitor the methylsulfuric acid ester salt ionic liquid 1-ethyl-3-methylimidazole methylsulfuric acid ester salt that does not add the methyl triethyl silicane than the use that records under the equal conditions than electric capacity conservation rate as the double layer capacitor of electrolyte improved 17.93% than electric capacity conservation rate, use the stability of double layer capacitor of the electrolyte of the present embodiment to be greatly improved.
Embodiment two to 18
Among the embodiment two to 18, alkyl silane is added in the methylsulfuric acid ester salt ionic liquid, be stirred to dissolving and can obtain electrolyte.During preparation electrolyte, in glove box, carry out.
Among the embodiment two to 18, the ratio that improves than electric capacity conservation rate and than electric capacity conservation rate after proportioning, mixing time, the circulation of alkyl silane, methylsulfuric acid ester salt ionic liquid, methylsulfuric acid ester salt ionic liquid and alkyl silane 1000 times is referring to table 1.
Table 1 embodiment two to 18 electrolyte prescription and test results
Among the embodiment two to 18, than identical among electric capacity conservation rate condition determination and the embodiment one; The ratio that improves than electric capacity conservation rate does not add alkyl silane for the use than recording under electric capacity conservation rate and the equal conditions of the double layer capacitor of the electrolyte that uses corresponding embodiment corresponding methylsulfuric acid ester salt ionic liquid is compared the percentage of raising as the double layer capacitor of electrolyte than electric capacity conservation rate.
As can be seen from the above table, use being greatly improved than electric capacity conservation rate of double layer capacitor of electrolyte provided by the invention, use the stability of the double layer capacitor of electrolyte provided by the invention to be improved.
The above embodiment has only expressed several execution mode of the present invention, and it describes comparatively concrete and detailed, but can not therefore be interpreted as the restriction to claim of the present invention.Should be pointed out that for the person of ordinary skill of the art, without departing from the inventive concept of the premise, can also make some distortion and improvement, these all belong to protection scope of the present invention.Therefore, the protection range of patent of the present invention should be as the criterion with claims.
Claims (10)
1. electrolyte, it is characterized in that: comprise methylsulfuric acid ester salt ionic liquid and be dissolved in alkyl silane in the described methylsulfuric acid ester salt ionic liquid, the mass ratio of described methylsulfuric acid ester salt ionic liquid and described alkyl silane is 1: 0.001～1: 0.05.
2. electrolyte as claimed in claim 1, it is characterized in that: described alkyl silane is methyl triethyl silicane or butyl trimethylsilicane alkane.
3. electrolyte as claimed in claim 1 is characterized in that: described methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.
4. electrolyte as claimed in claim 3, it is characterized in that: described imidazole salt cation is 1-butyl-3-methylimidazole cation, 1-propyl group-3-methylimidazole cation or 1-ethyl-3-methylimidazole cation, described quaternary ammonium salts cation is methyl triethyl group quaternary ammonium cation, tetraethyl quaternary ammonium cation or trimethyl propyl group quaternary ammonium cation, described pyrroles's salt cationoid is butyl methyl pyrroles cation, propyl group methylpyrrole cation or ethyl-methyl pyrroles cation, described season, the phosphonium salt cationoid was trimethyl hexyl season phosphine cation, triethyl group hexyl season phosphine cation or tri-methyl-amyl season the phosphine cation, described pyridiniujm cationoid is the butyl-pyridinium cation, pentyl pyridine cation or hexyl pyridylium.
5. an electrolyte is characterized in that, comprises the product that can be obtained by following chemical reaction:
Step 1, mass ratio is provided is 1: 0.001～1: 0.05 methylsulfuric acid ester salt ionic liquid and alkyl silane, contains inevitable impurity in the described methylsulfuric acid ester salt ionic liquid, and described impurity is inorganic acid;
Step 2, add alkyl silane and stirring and dissolving in the described methylsulfuric acid ester salt ionic liquid.
6. electrolyte as claimed in claim 5, it is characterized in that: the mass ratio of described methylsulfuric acid ester salt ionic liquid and described alkyl silane is 1: 0.01～1: 0.04.
7. electrolyte as claimed in claim 5, it is characterized in that: described alkyl silane is methyl triethyl silicane or butyl trimethylsilicane alkane.
8. the compound method of an electrolyte may further comprise the steps:
Step 1, mass ratio is provided is 1: 0.001～1: 0.05 methylsulfuric acid ester salt ionic liquid and alkyl silane;
Step 2, add described alkyl silane and stirring and dissolving in the described methylsulfuric acid ester salt ionic liquid.
9. the compound method of electrolyte as claimed in claim 8 is characterized in that: described methylsulfuric acid ester salt ionic liquid by methylsulfuric acid ester anion and imidazole salt cation, quaternary ammonium salts cation, pyrroles's salt cationoid, season the phosphonium salt cationoid or the pyridiniujm cationoid consist of.
10. the compound method of electrolyte as claimed in claim 8, it is characterized in that: described alkyl silane is methyl triethyl silicane or butyl trimethylsilicane alkane.
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Cited By (4)
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| US20160122938A1 (en) * | 2013-05-14 | 2016-05-05 | Eksen Makine Sanayi Ve Ticaret A.S. | Chemically stable, stain-, abrasion- and temperature-resistant, easy-to-clean metalware for use in elevated temperatures |
| EP2983233A4 (en) * | 2013-04-01 | 2016-10-12 | Ube Industries | Nonaqueous electrolyte solution and electricity storage device using same |
| CN109071570A (en) * | 2016-04-21 | 2018-12-21 | 日清纺控股株式会社 | Sulfuric acid containing silicon |
| JP2020098720A (en) * | 2018-12-18 | 2020-06-25 | トヨタ自動車株式会社 | Electrolyte for lithium secondary battery and lithium secondary battery |
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| CN101284791A (en) * | 2001-03-26 | 2008-10-15 | 日清纺织株式会社 | Electrolytic solution for storage device, and electric double layer capacitor |
| CN102089348A (en) * | 2008-07-11 | 2011-06-08 | 徐光锡 | Organic solvent-dispersible conductive polymer and method for manufacture thereof |
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| CN1471743A (en) * | 2000-09-07 | 2004-01-28 | ������������ʽ���� | Additive for non-aqueous liquid electrolyte, non-aqueous liquid electrolyte secondary cell and no-aqueous liquid electrolyte electric double layer capacitor |
| CN101284791A (en) * | 2001-03-26 | 2008-10-15 | 日清纺织株式会社 | Electrolytic solution for storage device, and electric double layer capacitor |
| JP2003297700A (en) * | 2002-03-29 | 2003-10-17 | Meidensha Corp | Electric double-layer capacitor and its manufacturing method |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP2983233A4 (en) * | 2013-04-01 | 2016-10-12 | Ube Industries | Nonaqueous electrolyte solution and electricity storage device using same |
| US9934911B2 (en) | 2013-04-01 | 2018-04-03 | Ube Industries, Ltd. | Nonaqueous electrolyte solution and electricity storage device using same |
| US20160122938A1 (en) * | 2013-05-14 | 2016-05-05 | Eksen Makine Sanayi Ve Ticaret A.S. | Chemically stable, stain-, abrasion- and temperature-resistant, easy-to-clean metalware for use in elevated temperatures |
| CN109071570A (en) * | 2016-04-21 | 2018-12-21 | 日清纺控股株式会社 | Sulfuric acid containing silicon |
| CN109071570B (en) * | 2016-04-21 | 2021-05-18 | 日清纺控股株式会社 | Silicon-containing sulfuric acid ester salts |
| JP2020098720A (en) * | 2018-12-18 | 2020-06-25 | トヨタ自動車株式会社 | Electrolyte for lithium secondary battery and lithium secondary battery |
| JP7085139B2 (en) | 2018-12-18 | 2022-06-16 | トヨタ自動車株式会社 | Electrolyte for lithium secondary battery and lithium secondary battery |
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