CN108258309A - A kind of lithium-ion battery electrolytes containing alpha-fluorocarboxylate ester - Google Patents
A kind of lithium-ion battery electrolytes containing alpha-fluorocarboxylate ester Download PDFInfo
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- CN108258309A CN108258309A CN201611242192.2A CN201611242192A CN108258309A CN 108258309 A CN108258309 A CN 108258309A CN 201611242192 A CN201611242192 A CN 201611242192A CN 108258309 A CN108258309 A CN 108258309A
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- lithium
- ion battery
- carbonate
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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
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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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 discloses a kind of lithium-ion battery electrolytes, and including lithium salts, nonaqueous solvents and cathode film formation agent, wherein cathode film formation agent contains fluoric cyclic carboxylate or containing fluoric cyclic carboxylate and fluoro chain carboxylate.Electrolyte provided by the invention, is suitable for lithium ion battery.
Description
Technical field
The present invention relates to a kind of battery electrolyte, more particularly to a kind of lithium-ion battery electrolytes.
Background technology
Lithium ion battery compares traditional secondary battery, has higher gravimetric specific energy, energy density per unit volume and environmental-friendly
The advantages that, just gradually replace the batteries such as ni-mh, ni-Cd, plumbic acid, such as mobile phone, laptop in the every field of daily life
With the portable electronic devices such as digital product.In recent years, electric vehicle, scale energy storage industry high speed development, be lithium-ion electric
Pond industry also brings the development space of bigger.
In lithium ion battery, electrolyte is one of key building block, and performance is to the cycle life and performance of battery
There is important influence.Electrolyte is generally made of electric conducting lithium salt, nonaqueous solvents and functional additive.Current commercialized electrolysis
Liquid, generally with lithium hexafluoro phosphate (LiPF6) it is electric conducting lithium salt, with cyclic carbonate such as ethylene carbonate (EC), propene carbonate
(PC), linear carbonate such as dimethyl carbonate (DMC), diethyl carbonate (DEC) or methyl ethyl carbonate (EMC) are non-aqueous
Agent, then add some functional additives such as cathode film formation additive, flame-retardant additive, anode film for additive, electrolyte and stablize
Agent, improves conductivity additive etc. at wetting agent.
In functional additive, cathode film formation additive is extremely important, can be used in improving the high rate performance of battery and follow
It is the ring service life, currently used to have vinylene carbonate and vinylethylene carbonate etc..But vinylene carbonate and ethylene carbonate
Two kinds of additive costs of ethyl are higher.
Therefore, it is necessary to be further improved to electrolyte for lithium ion battery, it is lower especially to develop a kind of cost
Electrolyte for lithium ion battery.
Invention content
The purpose of the present invention is to provide a kind of lithium-ion battery electrolytes, good and at low cost with cathode film formation effect
Advantage.
The present invention provides following technical solution：
A kind of lithium-ion battery electrolytes, the electrolyte include：Lithium salts, nonaqueous solvents and cathode film formation agent,
The cathode film formation agent contains at least one of fluoric cyclic carboxylate shown in structure formula (II) or contains
At least one in the fluoro chain carboxylate shown in structure formula (I) and the fluoric cyclic carboxylate shown in structure formula (II)
Kind,
Wherein：Rf1、Rf2Independently selected from the alkyl of C1~C10 or the halogenated alkyl of C1~C10.
Electrolyte provided by the invention, the cathode film formation agent used contain selected from the fluoro chain carboxylic shown in structure formula (I)
At least one of fluoric cyclic carboxylate shown in acid esters and structure formula (II).I.e.：The cathode film formation agent can contain only
At least one of fluoric cyclic carboxylate shown in structure formula (II) can also contain selected from the fluoro shown in structure formula (I)
At least one of fluoric cyclic carboxylate shown in chain carboxylate and structure formula (II).
When the cathode film formation agent contains selected from shown in the fluoro chain carboxylate shown in structure formula (I) and structure formula (II)
At least one of fluoric cyclic carboxylate when, matching between fluoro chain carboxylate and fluoric cyclic carboxylate of the invention
Than no particular/special requirement.
Fluoro chain carboxylate shown in the structure formula (I) that the present invention uses, substituent R f1、Rf2Independently selected from C1
The alkyl of~C10 or the halogenated alkyl of C1~C10.
Preferably, the substituent R f1、Rf2Independently selected from the alkyl of C1~C6 or the halogenated alkyl of C1~C6.
It may further be preferable that the substituent R f1、Rf2Independently selected from the alkyl of C1~C4 or the fluoroalkane of C1~C4
Base.
Electrolyte provided by the invention, the dosage satisfaction of lithium salts, nonaqueous solvents and cathode film formation agent make lithium ion battery just
Often operation.
Preferably, in the electrolyte, the mass fraction of lithium salts is 5~25%, and the mass fraction of nonaqueous solvents is 60
~90%, the mass fraction of cathode film formation agent is 0.1~20%.
It may further be preferable that in the electrolyte, the mass fraction of lithium salts is 8~15%, the quality point of nonaqueous solvents
Number is 75~85%, and the mass fraction of cathode film formation agent is 0.2~12%.
Electrolyte provided by the invention, the cathode film formation agent used, in addition to the fluoric cyclic shown in containing structure formula (II)
At least one of carboxylate or containing selected from shown in the fluoro chain carboxylate shown in structure formula (I) and structure formula (II)
At least one of fluoric cyclic carboxylate, can also further contain fluoro carbonic ester.
I.e. described cathode film formation agent, contains：
(1) component A：Selected from least one of fluoric cyclic carboxylate shown in structure formula (II) or selected from structure
At least one of fluoric cyclic carboxylate shown in fluoro chain carboxylate and structure formula (II) shown in formula (I)；With
(2) component B：Fluoro carbonic ester.
When the cathode film formation agent contains component A and component B, the present invention does not have component A and the quality proportioning of component B
Particular/special requirement.
Preferably, the quality proportioning of the component A and component B is 1~50%.
When it is component B to use fluoro carbonic ester, it is preferred that the fluoro carbonic ester is selected from fluorinated ethylene carbonate,
Difluoroethylene carbonate, three fluoropropylene carbonates, trifluoroethyl methyl carbonate, trifluoroethyl ethyl carbonate and double trifluoro second
At least one of base carbonic ester.
Electrolyte provided by the invention, the lithium salts used can be lithium salts commonly used in the art.
Preferably, the lithium salts is selected from LiBF4、LiPF6、LiFSI、LiTFSI、LiAsF6、LiClO4、LiSO3CF3、
LiC2O4BC2O4And LiF2BC2O4At least one of.
Electrolyte provided by the invention, the nonaqueous solvents used can be nonaqueous solvents commonly used in the art.
Preferably, the nonaqueous solvents be selected from ethylene carbonate, propene carbonate, gamma-butyrolacton, butylene carbonate,
Dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl ethyl ester and C3~C8 aliphatic monool synthesized with carbonic acid
At least one of carbonic acid ester derivative.
Electrolyte provided by the invention, can also be further according to need in addition to lithium salts, nonaqueous solvents and cathode film formation agent
It asks including other functional additives.
Other described functional additives can be selected from biphenyl, vinylene carbonate, vinylethylene carbonate, sulfurous acid third
Enester, butylene sulfite, 1,3- propane sultones, 1,4 butyl sultones, 1,3- (1- propylene) sultone, sulfurous acid ethylene
At least one of ester, sulfuric acid vinyl ester, cyclohexyl benzene, tert-butyl benzene, adiponitrile, succinonitrile and fluorine-containing ethers.
When in electrolyte, in addition to lithium salts, nonaqueous solvents and cathode film formation agent, further including other functional additives
When, the dosages of other functional additives is to meet functional requirements.
Preferably, the mass fraction of other described functional additives in the electrolytic solution is 0.1~10%.
Electrolyte prepared by the present invention, is suitable for lithium ion battery.It is especially suitable for the lithium using graphite as cathode
Ion battery.
FEC of the present invention is：Fluorinated ethylene carbonate
ETFA of the present invention is：Trifluoroacetic Acid Ethyl Ester
MTFA of the present invention is：
VC of the present invention is：Vinylene carbonate
Specific embodiment
With reference to specific embodiment, the invention will be further described, but it is specific not limit the invention to these
Embodiment.One skilled in the art would recognize that present invention encompasses the institutes that may include in Claims scope
There are alternative, improvement project and equivalent scheme.
Embodiment 1
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC, ETFA, MTFA and VC, addition mass ratio is respectively 10%, 3%, 3%, 2% as electrolysis additive.Finally, to
LiPF is added in solution6, its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 2
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC, ETFA, MTFA and VC, addition mass ratio is respectively 10%, 1.5%, 1.5%, 2% as electrolysis additive.Most
Afterwards, LiPF is added in into solution6, its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 3
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC, ETFA, MTFA and VC, addition mass ratio is respectively 10%, 0.5%, 0.5%, 2% as electrolysis additive.Most
Afterwards, LiPF is added in into solution6, its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 4
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding MTFA and VC, addition mass ratio is respectively 1.5% and 2% as electrolysis additive.Finally, LiPF is added in into solution6,
Its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 5
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC and MTFA, addition mass ratio is respectively 10% and 1.5% as electrolysis additive.Finally, it is added in into solution
LiPF6, its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 6
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC, MTFA and VC, addition mass ratio is respectively 10%, 1.5%, 2% as electrolysis additive.Finally, add into solution
Enter LiPF6, its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 7
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC, ETFA, addition mass ratio is respectively 10% and 1.5% as electrolysis additive.Finally, it is added in into solution
LiPF6, its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 8
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding ETFA and VC, addition mass ratio is respectively 1.5% and 2% as electrolysis additive.Finally, LiPF is added in into solution6,
Its mass ratio is made to reach the 10% of final solution, obtains lithium-ion battery electrolytes.
Embodiment 9
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding ETFA, addition mass ratio is respectively 1.5% as electrolysis additive.Finally, LiPF is added in into solution6, make its quality
Than reach final solution 10%, lithium-ion battery electrolytes are obtained.
Embodiment 10
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding ETFA, addition mass ratio is respectively 1.0% as electrolysis additive.Finally, LiPF is added in into solution6, make its quality
Than reach final solution 10%, lithium-ion battery electrolytes are obtained.
Comparative example 1
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC and VC, addition mass ratio is respectively 10% and 2% as electrolysis additive.Finally, LiPF is added in into solution6, make
Its mass ratio reaches the 10% of final solution, obtains lithium-ion battery electrolytes.
Comparative example 2
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding VC, addition mass ratio is respectively 2% as electrolysis additive.Finally, LiPF is added in into solution6, reach its mass ratio
To the 10% of final solution, lithium-ion battery electrolytes are obtained.
Comparative example 3
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then add into mixed solution
Adding FEC, addition mass ratio is respectively 10% as electrolysis additive.Finally, LiPF is added in into solution6, make its mass ratio
Reach the 10% of final solution, obtain lithium-ion battery electrolytes.
Comparative example 4
A kind of lithium-ion battery electrolytes, including two kinds of ethylene carbonate, methyl ethyl carbonate carbonate solvents, with LiPF6
For lithium salts.Preparation method is：By 3: 7 mixing by volume of ethylene carbonate, methyl ethyl carbonate, then added in into solution
LiPF6, mass ratio reaches final solution 10% is allowed to, obtains lithium-ion battery electrolytes.
The present invention is tested electrolyte made from embodiment 1 to 10 and comparative example 1 to 4, respectively test finger below
Mark：
Electrolyte is to the profit visual angle of diaphragm at (1) 20 DEG C；
(2) graphite/Li half-cells are assembled using different electrolyte, tests the library for the first time of different batteries at 20 DEG C
Capacity retention ratio after human relations efficiency and 0.2C charge-discharge cycles 100 times.
Test, which was met, see the table below 1.
Table 1
In the art, if the native graphite using any processing of surface free is cathode, it is difficult to obtain preferable
It is extremely difficult to want the promotion 1~2% on coulombic efficiency for the first time and cycle performance for coulombic efficiency and cycle performance for the first time.From
1 data of table using cathode film formation agent it is found that can not only be substantially reduced between electrolyte and diaphragm in electrolyte of the present invention
Angle of wetting, and the coulombic efficiency for the first time and cycle performance of graphite/Li half-cells can be significantly improved so that circulating battery is stablized
Property further improves.
Claims (13)
1. a kind of lithium-ion battery electrolytes, it is characterised in that the electrolyte includes：Lithium salts, nonaqueous solvents and cathode film formation
Agent,
The cathode film formation agent contain at least one of fluoric cyclic carboxylate shown in structure formula (II) or containing selected from
At least one of fluoric cyclic carboxylate shown in fluoro chain carboxylate and structure formula (II) shown in structure formula (I),
Wherein：Rf1、Rf2Independently selected from the alkyl of C1~C10 or the halogenated alkyl of C1~C10.
2. lithium-ion battery electrolytes described in accordance with the claim 1, it is characterised in that：The Rf1、Rf2Independently selected from C1~
The alkyl of C6 or the halogenated alkyl of C1~C6.
3. lithium-ion battery electrolytes described in accordance with the claim 2, it is characterised in that the Rf1、Rf2Independently selected from C1~
The alkyl of C4 or the fluoro-alkyl of C1~C4.
4. lithium-ion battery electrolytes described in accordance with the claim 1, it is characterised in that in the electrolyte, the electrolyte
In, the mass fraction of lithium salts is 5~25%, and the mass fraction of nonaqueous solvents is 60~90%, the mass fraction of cathode film formation agent
It is 0.1~20%.
5. according to the lithium-ion battery electrolytes described in claim 4, it is characterised in that in the electrolyte, the quality point of lithium salts
Number is 8~15%, and the mass fraction of nonaqueous solvents is 75~85%, and the mass fraction of cathode film formation agent is 0.2~12%.
6. lithium-ion battery electrolytes described in accordance with the claim 1, it is characterised in that the cathode film formation agent contains：
(1) component A：Selected from least one of fluoric cyclic carboxylate shown in structure formula (II) or selected from structure formula (I)
At least one of fluoric cyclic carboxylate shown in shown fluoro chain carboxylate and structure formula (II)；With
(2) component B：Fluoro carbonic ester.
7. according to the lithium-ion battery electrolytes described in claim 6, it is characterised in that the quality of the component A and component B is matched
Than being 1~50%.
8. according to the lithium-ion battery electrolytes described in claim 6, it is characterised in that the fluoro carbonic ester is selected from fluoro carbon
Vinyl acetate, difluoroethylene carbonate, three fluoropropylene carbonates, trifluoroethyl methyl carbonate, trifluoroethyl ethyl carbonate
At least one of with double trifluoroethyl carbonic esters.
9. lithium-ion battery electrolytes described in accordance with the claim 1, it is characterised in that the lithium salts is selected from LiBF4、LiPF6、
LiFSI、LiTFSI、LiAsF6、LiClO4、LiSO3CF3、LiC2O4BC2O4And LiF2BC2O4At least one of.
10. lithium-ion battery electrolytes described in accordance with the claim 1, it is characterised in that the nonaqueous solvents is selected from ethylene carbonate
Ester, propene carbonate, gamma-butyrolacton, butylene carbonate, dimethyl carbonate, diethyl carbonate, dipropyl carbonate, methyl
At least one of carbonic acid ester derivative that the aliphatic monool of ethyl ester and C3~C8 are synthesized with carbonic acid.
11. lithium-ion battery electrolytes described in accordance with the claim 1, it is characterised in that the electrolyte further includes it
His functional additive,
Other described functional additives are selected from biphenyl, vinylene carbonate, vinylethylene carbonate, propylene sulfite, sulfurous
Sour butene esters, 1,3- propane sultones, 1,4 butyl sultones, 1,3- (1- propylene) sultone, ethylene sulfite, sulfuric acid second
At least one of enester, cyclohexyl benzene, tert-butyl benzene, adiponitrile, succinonitrile and fluorine-containing ethers,
The mass fraction of other described functional additives in the electrolytic solution is 0.1~10%.
12. a kind of application of lithium-ion battery electrolytes, it is characterised in that the electrolyte is used for lithium ion battery.
13. according to the application of the lithium-ion battery electrolytes described in claim 12, it is characterised in that the electrolyte be used for
Lithium ion battery of the graphite as cathode.
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| CN109301327A (en) * | 2018-09-29 | 2019-02-01 | 桑顿新能源科技有限公司 | A kind of electrolyte and a kind of lithium ion battery |
| CN109301327B (en) * | 2018-09-29 | 2021-05-18 | 桑顿新能源科技有限公司 | Electrolyte and lithium ion battery |
| CN109461967A (en) * | 2018-11-01 | 2019-03-12 | 江西优锂新材股份有限公司 | A kind of nickelic tertiary cathode material electrolyte thereof and preparation method |
| CN110085914A (en) * | 2019-06-04 | 2019-08-02 | 东莞维科电池有限公司 | A kind of Soft Roll high-voltage lithium-ion battery electrolyte and a kind of lithium ion battery |
| CN110854432A (en) * | 2019-11-05 | 2020-02-28 | 宁德新能源科技有限公司 | Electrolyte solution, and electrochemical device and electronic device using same |
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Application publication date: 20180706 |