CN110034333A - A kind of high temperature resistant nonaqueous electrolytic solution - Google Patents
A kind of high temperature resistant nonaqueous electrolytic solution Download PDFInfo
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- CN110034333A CN110034333A CN201910303287.8A CN201910303287A CN110034333A CN 110034333 A CN110034333 A CN 110034333A CN 201910303287 A CN201910303287 A CN 201910303287A CN 110034333 A CN110034333 A CN 110034333A
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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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
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Abstract
The present invention relates to chemical field more particularly to a kind of high temperature resistant nonaqueous electrolytic solutions.The high temperature resistant nonaqueous electrolytic solution includes: 2 ~ 20 parts of lithium salts in parts by weight, and 75 ~ 85 parts of nonaqueous solvents, 1 ~ 6 part of high temperature resistant additive, 1 ~ 10 part of additive, wherein the high temperature resistant additive is the alkyl-substituted zirconate of C3 ~ C6.Tests prove that due to the effect of zirconate in above-mentioned electrolyte, prepared battery stored 30 days at a high temperature of 60 DEG C after thickness swelling still less than 5%, there is good storage performance.It is especially added with the lithium ion battery of four n-propyl zirconates, the thickness swelling at 60 DEG C after high temperature storage 30 days is minimum, and high-temperature storage performance is best.
Description
Technical field
The present invention relates to chemical fields, are related to battery electrolyte research field more particularly to a kind of high temperature resistant non-aqueous solution electrolysis
Liquid.
Background technique
Lithium battery has the advantages such as operating high voltage, high specific energy, long circulation life, low self-discharge rate, pollution-free, extensively
It is general dynamic in electric car (EV) and mixing for miniaturized electronics such as mobile phone, portable computer, digital products, and
Wide application prospect and powerful growth momentum are shown on the vehicles such as power automobile (HEV).
Lithium battery is mainly made of positive and negative pole material, diaphragm and electrolyte.And the solvent and additive of electrolyte are to inhibition
The thickness swelling of battery core at high temperature plays a significant role.In order to inhibit the thickness swelling of battery core under high temperature, has patent and use
The method of associated additives is added in the electrolytic solution.
The wide range of applications of zirconium is mainly applied to the neck such as ceramics, refractory material in the form of zirconium silicate, zirconium oxide
Domain.Zirconium just will form oxidation film as a kind of active metal at room temperature, and it is excellent that this layer of oxidation film has zirconium and its alloy
Corrosion resistance.Zirconium has good mechanics and heat transfer property again simultaneously, adds significant cost advantage, makes it and work as
The excellent corrosion resistance structure material of modern petrochemical industry.
Summary of the invention
The present invention is in view of the shortcomings of the prior art, provide a kind of high temperature resistant nonaqueous electrolytic solution.In order to achieve the above object, this hair
Bright technical solution are as follows:
A kind of high temperature resistant nonaqueous electrolytic solution characterized by comprising lithium salts, nonaqueous solvents and additive, which is characterized in that institute
State high temperature resistant nonaqueous electrolytic solution includes: in parts by weight
2 ~ 20 parts of lithium salts
75 ~ 85 parts of nonaqueous solvents
1 ~ 6 part of high temperature resistant additive
1 ~ 10 part of additive
The general structure of the additive are as follows:
Wherein R1、R2、R3And R4The alkyl for being 3 ~ 6 for carbon atom number.
Further, the high temperature resistant nonaqueous electrolytic solution includes: in parts by weight
14 parts of lithium salts
75 parts of nonaqueous solvents
6 parts of high temperature resistant additive
5 parts of additive
Further, the high temperature resistant additive is four n-propyl zirconates.
Further, the nonaqueous solvents is ethylene carbonate, diethyl carbonate, methyl ethyl carbonate, propene carbonate, four
Hydrogen furans, 2- methyltetrahydrofuran, dimethyl carbonate, acetonitrile, dimethyl sulfone, methyl butyrate, methyl acetate, dioxolanes, fourth
One or more of acetoacetic ester.
Further, the lithium salts is in LiBF4, lithium hexafluoro phosphate, double fluorine sulfonamide lithiums and trifluoromethanesulfonic acid lithium
One or more.
Further, the additive be biphenyl, vinylene carbonate, vinylethylene carbonate, fluorinated ethylene carbonate,
1,3-propane sultone, Isosorbide-5-Nitrae-butyl sultone, 1,3- (1- propylene) sultone, ethylene sulfite, sulfuric acid vinyl ester, ring
One or more of hexyl benzene, tert-butyl benzene, tert-amyl benzene and fourth dicyan.
Further, the high temperature resistant nonaqueous electrolytic solution is mainly used in disposable lithium-battery or serondary lithium battery.
Beneficial effects of the present invention are that it is anti-that oxidation occurs during the initial charge of battery for zirconate used in the present invention
It answers, oxidation product zirconium dioxide solid portion is covered on positive electrode surface and forms one layer of fine and close passivating film, plays protection anode
Effect prevents reacting for anode and electrolyte when high temperature, it is suppressed that decomposition of the anode to electrolyte, to significantly improve
The high-temperature storage performance of battery.
Specific embodiment
To better understand the objects, features and advantages of the present invention, right combined with specific embodiments below
The present invention is described further.It should be noted that in the absence of conflict, the spy in embodiments herein and embodiment
Sign can be combined with each other.
In the following description, numerous specific details are set forth in order to facilitate a full understanding of the present invention, still, the present invention may be used also
To be implemented using other modes described herein are different from, therefore, the present invention is not limited to the specific of specification is described below
The limitation of embodiment.
Comparative example
The preparation of electrolyte: ethylene carbonate, diethyl carbonate, methyl ethyl carbonate, propene carbonate according to 35:30:30:5
The ratio of (weight ratio) mixes, and additive biphenyl, vinylene carbonate, vinylethylene carbonate, fluorinated ethylene carbonate are pressed
According to the ratio mixing of 25:25:25:25 (weight ratio), then with this mixed solvent of 75 parts by weight and adding for 10 parts by weight
Add agent to be uniformly mixed, adds 15 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6Concentration is the electrolyte of 1mol/L.
The production of anode pole piece: by positive active material cobalt acid lithium (LiCoO2), conductive agent acetylene black, binder it is poly- inclined
Difluoroethylene (PVDF) is thoroughly mixed uniformly by weight 96:2:2 in N- methyl pyrrolidone solvent system
Afterwards, it is coated on Al foil, drying, cold pressing, cut-parts obtain anode pole piece.
The production of cathode pole piece: by negative electrode active material graphite, conductive agent acetylene black, binder butadiene-styrene rubber (SBR),
Thickener sodium carboxymethylcellulose (CMC) is sufficiently stirred in deionized water solvent system mixed according to weight ratio 95:2:2:1
After closing uniformly, it is coated on drying on Cu foil, cold pressing, cut-parts, obtains cathode pole piece.
Using PE porous polymer film as diaphragm.
The production of lithium ion battery: anode pole piece, diaphragm, cathode pole piece are folded in order, and diaphragm is made to be in anode and cathode
Isolation is played the role of in centre, and winds and obtain battery core.Battery core is placed in plastic-aluminum combined film package bag, the electrolysis prepared is injected
Liquid simultaneously encapsulates.Primary charging is carried out to battery, is then vacuum-evacuated, battery production is completed in encapsulation again.
Embodiment 1
The preparation of electrolyte: ethylene carbonate, diethyl carbonate, methyl ethyl carbonate, propene carbonate according to 35:30:30:5
The ratio of (weight ratio) mixes, and additive biphenyl, vinylene carbonate, vinylethylene carbonate, fluorinated ethylene carbonate are pressed
According to the ratio mixing of 25:25:25:25 (weight ratio), then with the four of this mixed solvent of 75 parts by weight and 1 parts by weight
N-propyl zirconate, the additive of 10 parts by weight are uniformly mixed, add 14 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into
LiPF6Concentration is the electrolyte of 1mol/L.
The production of anode pole piece: by positive active material cobalt acid lithium (LiCoO2), conductive agent acetylene black, binder it is poly- inclined
Difluoroethylene (PVDF) is thoroughly mixed uniformly by weight 96:2:2 in N- methyl pyrrolidone solvent system
Afterwards, it is coated on Al foil, drying, cold pressing, cut-parts obtain anode pole piece.
The production of cathode pole piece: by negative electrode active material graphite, conductive agent acetylene black, binder butadiene-styrene rubber (SBR),
Thickener sodium carboxymethylcellulose (CMC) is sufficiently stirred in deionized water solvent system mixed according to weight ratio 95:2:2:1
After closing uniformly, it is coated on drying on Cu foil, cold pressing, cut-parts, obtains cathode pole piece.
Using PE porous polymer film as diaphragm.
The production of lithium ion battery: anode pole piece, diaphragm, cathode pole piece are folded in order, and diaphragm is made to be in anode and cathode
Isolation is played the role of in centre, and winds and obtain battery core.Battery core is placed in plastic-aluminum combined film package bag, the electrolysis prepared is injected
Liquid simultaneously encapsulates.Primary charging is carried out to battery, is then vacuum-evacuated, battery production is completed in encapsulation again.
Embodiment 2
The preparation of electrolyte unlike embodiment 1: tetrahydrofuran, 2- methyltetrahydrofuran, dimethyl carbonate, acetonitrile
It is mixed according to the ratio of 35:30:30:5 (weight ratio), by additive 1,3-propane sultone, Isosorbide-5-Nitrae-butyl sultone, 1,3-
(1- propylene) sultone, ethylene sulfite are mixed according to the ratio of 25:25:25:25 (weight ratio), then with 70 weights
This mixed solvent of amount part is uniformly mixed with the additive of four n-propyl zirconates of 3 parts by weight, 7 parts by weight, adds 20 weights
Measure part lithium hexafluoro phosphate (LiPF6), it is made into LiPF6Concentration is the electrolyte of 1.2mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 3
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, dioxolanes according to
The ratio of 35:30:30:5 (weight ratio) mixes, and additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, tert-amyl benzene are pressed
According to the ratio mixing of 25:25:25:25 (weight ratio), then with the four of this mixed solvent of 85 parts by weight and 6 parts by weight
N-propyl zirconate, the additive of 1 parts by weight are uniformly mixed, add 8 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6
Concentration is the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 4
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, ethyl butyrate according to
The ratio of 35:30:30:5 (weight ratio) mixes, by additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, fourth dicyan according to
The ratio of 25:25:25:25 (weight ratio) mixes, then just with the four of this mixed solvent of 75 parts by weight and 6 parts by weight
Propyl zirconate, the additive of 5 parts by weight are uniformly mixed, add 14 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6It is dense
Degree is the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 5
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, ethyl butyrate according to
The ratio of 35:30:30:5 (weight ratio) mixes, by additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, fourth dicyan according to
The ratio of 25:25:25:25 (weight ratio) mixes, then with the four positive third of this mixed solvent of 85 parts by weight and 6 parts by weight
Base zirconate, the additive of 5 parts by weight are uniformly mixed, add 4 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6Concentration
For the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 6
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, ethyl butyrate according to
The ratio of 35:30:30:5 (weight ratio) mixes, by additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, fourth dicyan according to
The ratio of 25:25:25:25 (weight ratio) mixes, then with four benzene of this mixed solvent of 75 parts by weight and 6 parts by weight
Base zirconate, the additive of 5 parts by weight are uniformly mixed, add 14 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6Concentration
For the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 7
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, ethyl butyrate according to
The ratio of 35:30:30:5 (weight ratio) mixes, by additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, fourth dicyan according to
The ratio of 25:25:25:25 (weight ratio) mixes, then with four uncles of this mixed solvent of 75 parts by weight and 6 parts by weight
Butyl zirconate, the additive of 5 parts by weight are uniformly mixed, add 14 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6It is dense
Degree is the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 8
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, ethyl butyrate according to
The ratio of 35:30:30:5 (weight ratio) mixes, by additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, fourth dicyan according to
The ratio of 25:25:25:25 (weight ratio) mixes, then just with the four of this mixed solvent of 75 parts by weight and 6 parts by weight
Butyl zirconate, the additive of 5 parts by weight are uniformly mixed, add 14 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6It is dense
Degree is the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Embodiment 9
The preparation of electrolyte unlike embodiment 1: dimethyl sulfone, methyl butyrate, methyl acetate, ethyl butyrate according to
The ratio of 35:30:30:5 (weight ratio) mixes, by additive sulfur vinyl acetate, cyclohexyl benzene, tert-butyl benzene, fourth dicyan according to
The ratio of 25:25:25:25 (weight ratio) mixes, then with the 4 penta of this mixed solvent of 75 parts by weight and 6 parts by weight
Base zirconate, the additive of 5 parts by weight are uniformly mixed, add 14 parts by weight lithium hexafluoro phosphate (LiPF6), it is made into LiPF6Concentration
For the electrolyte of 0.8mol/L.
Remaining is with embodiment 1, and which is not described herein again.
Battery high-temperature storage test
The battery of comparative example, embodiment 1~8 is respectively taken 3, it is permanent with the multiplying power of 0.5C under room temperature (25 ± 2 DEG C)
To 4.2V, it is 0.05C that electric current is further charged under 4.2V constant voltage, and it is full to be at 4.2V for constant-current charge
Fill state.The thickness for testing battery fully charged state is denoted as thickness before storage;Battery is placed in 60 DEG C of baking ovens, is surveyed within every 5 days
A thickness is tried, the thickness swelling before being calculated as follows relative to storage:
Thickness before thickness swelling=(thickness before thickness-storage after storage) ÷ is stored
The average thickness expansion rate of every group of 3 batteries is calculated, it is as a result shown in table 1.
It can be seen that from the result of table 1 after adding zirconate in electrolyte of the invention, battery height can be significantly reduced
The thickness swelling of gentle storage.After the lithium ion battery of comparative example stores 20 days, battery starts to produce gas, therefore generates apparent thick
Degree expansion;And the battery in embodiment 1 to 9, due to the effect of zirconate in electrolyte, battery is deposited at a high temperature of 60 DEG C
Thickness swelling after storage 30 days is also both less than 5%, has good storage performance.Especially it is added with four n-propyl zirconic acids
The lithium ion battery of ester, the thickness swelling at 60 DEG C after high temperature storage 30 days is minimum, and high-temperature storage performance is best.
Table 1: battery full charge to 4.2V stores at 60 DEG C, cell thickness expansion rate with storage time variation.
The above described is only a preferred embodiment of the present invention, being not that the invention has other forms of limitations, appoint
What those skilled in the art changed or be modified as possibly also with the technology contents of the disclosure above equivalent variations etc.
It imitates embodiment and is applied to other fields, but without departing from the technical solutions of the present invention, according to the technical essence of the invention
Any simple modification, equivalent variations and remodeling to the above embodiments, still fall within the protection scope of technical solution of the present invention.
Claims (7)
1. a kind of high temperature resistant nonaqueous electrolytic solution characterized by comprising lithium salts, nonaqueous solvents, high temperature resistant additive and addition
Agent, which is characterized in that the high temperature resistant nonaqueous electrolytic solution includes: in parts by weight
2 ~ 20 parts of lithium salts
75 ~ 85 parts of nonaqueous solvents
1 ~ 6 part of high temperature resistant additive
1 ~ 10 part of additive
The general structure of the additive are as follows:
Wherein R1、R2、R3And R4The alkyl for being 3 ~ 6 for carbon atom number.
2. a kind of high temperature resistant nonaqueous electrolytic solution according to claim 1, which is characterized in that the high temperature resistant nonaqueous electrolytic solution
Include: in parts by weight
14 parts of lithium salts
75 parts of nonaqueous solvents
6 parts of high temperature resistant additive
5 parts of additive.
3. a kind of high temperature resistant nonaqueous electrolytic solution according to claim 1, which is characterized in that the high temperature resistant additive is four
N-propyl zirconate.
4. a kind of high temperature resistant nonaqueous electrolytic solution according to claim 1, which is characterized in that the nonaqueous solvents is carbonic acid second
Enester, diethyl carbonate, methyl ethyl carbonate, propene carbonate, tetrahydrofuran, 2- methyltetrahydrofuran, dimethyl carbonate, second
One or more of nitrile, dimethyl sulfone, methyl butyrate, methyl acetate, dioxolanes, ethyl butyrate.
5. a kind of high temperature resistant nonaqueous electrolytic solution according to claim 1, which is characterized in that the lithium salts is tetrafluoro boric acid
One or more of lithium, lithium hexafluoro phosphate, double fluorine sulfonamide lithiums and trifluoromethanesulfonic acid lithium.
6. a kind of high temperature resistant nonaqueous electrolytic solution according to claim 1, which is characterized in that the additive is biphenyl, carbon
Sour vinylene, vinylethylene carbonate, fluorinated ethylene carbonate, 1,3-propane sultone, Isosorbide-5-Nitrae-butyl sultone, 1,3-
In (1- propylene) sultone, ethylene sulfite, sulfuric acid vinyl ester, cyclohexyl benzene, tert-butyl benzene, tert-amyl benzene and fourth dicyan
One or more.
7. a kind of high temperature resistant nonaqueous electrolytic solution according to claim 1, which is characterized in that the high temperature resistant nonaqueous electrolytic solution
It is mainly used in disposable lithium-battery or serondary lithium battery.
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
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CN110233293A (en) * | 2019-07-23 | 2019-09-13 | 河源市聚芯源科技有限公司 | A kind of electrolyte and its preparation process improving high-temperature lithium ion battery performance |
WO2023060554A1 (en) * | 2021-10-15 | 2023-04-20 | 宁德时代新能源科技股份有限公司 | Electrolyte, secondary battery, and power device |
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CN102593512A (en) * | 2012-02-14 | 2012-07-18 | 东莞新能源科技有限公司 | Lithium ion battery and electrolyte solution thereof |
CN109449395A (en) * | 2018-10-19 | 2019-03-08 | 中国科学院大学 | A kind of preparation method of lithium ion conductor coating modification sodium-ion battery positive material |
CN109585919A (en) * | 2018-11-06 | 2019-04-05 | 欣旺达电子股份有限公司 | Lithium ion battery and its electrolyte |
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Patent Citations (3)
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CN102593512A (en) * | 2012-02-14 | 2012-07-18 | 东莞新能源科技有限公司 | Lithium ion battery and electrolyte solution thereof |
CN109449395A (en) * | 2018-10-19 | 2019-03-08 | 中国科学院大学 | A kind of preparation method of lithium ion conductor coating modification sodium-ion battery positive material |
CN109585919A (en) * | 2018-11-06 | 2019-04-05 | 欣旺达电子股份有限公司 | Lithium ion battery and its electrolyte |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
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CN110233293A (en) * | 2019-07-23 | 2019-09-13 | 河源市聚芯源科技有限公司 | A kind of electrolyte and its preparation process improving high-temperature lithium ion battery performance |
WO2023060554A1 (en) * | 2021-10-15 | 2023-04-20 | 宁德时代新能源科技股份有限公司 | Electrolyte, secondary battery, and power device |
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Application publication date: 20190719 |