CN109818060A - Nonaqueous electrolytic solution and lithium ion battery containing the nonaqueous electrolytic solution - Google Patents
Nonaqueous electrolytic solution and lithium ion battery containing the nonaqueous electrolytic solution Download PDFInfo
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- CN109818060A CN109818060A CN201910100098.0A CN201910100098A CN109818060A CN 109818060 A CN109818060 A CN 109818060A CN 201910100098 A CN201910100098 A CN 201910100098A CN 109818060 A CN109818060 A CN 109818060A
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- electrolytic solution
- nonaqueous electrolytic
- lithium
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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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- 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
-
- 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
-
- 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
A kind of nonaqueous electrolytic solution and the lithium ion battery containing the nonaqueous electrolytic solution, belong to technical field of lithium ion.The nonaqueous electrolytic solution includes non-aqueous organic solvent, electric conducting lithium salt and additive.Additive includes at least one phosphate type lithium salt compound and at least one compound containing S=O.The phosphate type lithium salt compound is bis- (malonic acid) lithium phosphates of divinyl, bis- (malonic acid) lithium phosphates of diphenyl, bis- (malonic acid) lithium phosphates of difluoro.The compound containing S=O is methane-disulfonic acid methylene ester, sulfuric acid vinyl ester, sulfuric acid acrylic ester, 1,3-propane sultone, Isosorbide-5-Nitrae-butyl sultone, vinyl sulfonic acid lactone, 1,3- propene sultone or Isosorbide-5-Nitrae-butylene sultones.The invention has the advantages that passing through the synergistic effect of phosphate type lithium salt compound and the compound containing S=O, stable and low impedance interfacial film is formed, there is preferable high temperature circulation stability and low-temperature characteristics.
Description
Technical field
The invention belongs to technical field of lithium ion, and in particular to a kind of nonaqueous electrolytic solution and contain the nonaqueous electrolytic solution
Lithium ion battery.
Background technique
In recent years, lithium ion battery is as energy storage device in the electronic equipments such as smart phone, tablet computer, bluetooth headset
It is widely used.But with the diversification of the diversification of electronic equipment and function, cruising ability of the consumer to electronic equipment
It is required that also higher and higher.Therefore, the energy density for improving lithium ion battery is current research hotspot.
On the one hand the promotion of energy density is by improving battery charging voltage to obtain higher capacity；On the other hand
It is the anode or negative electrode material using high capacity.Unfortunately, the either raising of cell voltage or novel anode or negative
The application of pole material, the problem of all bringing electrolyte severe decomposition.Currently, the application of film forming electrolysis additive is to solve electricity
Solve the important means that liquid decomposes.But current electrolysis additive is often difficult to combine high temperature performance.Therefore, really
It is necessary to develop one kind to apply the electrolyte in high energy density cells, promoting lithium ion battery to have widely makes
With.
Summary of the invention
The purpose of the present invention is to solve the undesirable problems of existing electrolysis additive high temperature performance, provide one
Kind nonaqueous electrolytic solution and the lithium ion battery containing the nonaqueous electrolytic solution, the electrolyte can form height in anode and negative terminal surface
The interfacial film of lithium ion and high stability is led, so that battery has long cycle life at high temperature, is had at low temperature good
Performance.
To achieve the above object, the technical solution adopted by the present invention is as follows:
A kind of nonaqueous electrolytic solution, including non-aqueous organic solvent, electric conducting lithium salt and additive, the additive is by least one
Kind phosphate type lithium salt compound and at least one compound composition containing S=O.
Further, the phosphate type lithium salt compound has general structure shown in formula (I):
Wherein, R1、R4For hydrogen, C1~4Alkylidene, C1~4Halogeno alkylen or C1~4Alkenylene；R2、R3For hydrogen, halogen, C1~4
Alkyl, C1~4Halogenated alkyl, C6~10Aryl, C6~10Halogenated aryl, C1-C4Itrile group, C1-C6Alkenyl, alkoxy or carboxyl.
Preferably, the phosphate type lithium salt compound is bis- (malonic acid) lithium phosphates of divinyl, diphenyl bis- (third
Diacid) one or more of lithium phosphate, bis- (malonic acid) lithium phosphates of difluoro or bis- (the 4- fluorine malonic acid) lithium phosphates of difluoro it is mixed
Object is closed, dosage accounts for the 0.1%~10% of nonaqueous electrolytic solution gross mass.
Preferably, the compound containing S=O be methane-disulfonic acid methylene ester, sulfuric acid vinyl ester, sulfuric acid acrylic ester,
1,3-propane sultone, Isosorbide-5-Nitrae-butyl sultone, vinyl sulfonic acid lactone, 1,3- propene sultone, Isosorbide-5-Nitrae-butylene sultones,
1- methyl-1,3- propene sultone, divinylsulfone, dimethyl sulfone, diethyl sulfone, Methylethyl sulfone or methyl ethylene sulfone
One or more of mixture, dosage accounts for the 0.1%~10% of nonaqueous electrolytic solution gross mass.
Preferably, the non-aqueous organic solvent is made of cyclic solvent and linear solvents, wherein the cyclic solvent
For one of ethylene carbonate, propene carbonate, fluorinated ethylene carbonate, gamma-butyrolacton and gamma-valerolactone or a variety of groups
It closes；The linear solvents are dimethyl carbonate, methyl ethyl carbonate, diethyl carbonate, methyl propyl carbonate, ethyl propionate, propionic acid
Ethyl ester, 1,1,2,3- tetra- fluoro ethyl -2,2, one of 3,3- tetrafluoro propyl ethers or multiple combinations, interworking total amount are non-water power
Solve the 55%~89.8% of liquid gross mass.
Preferably, the electric conducting lithium salt is lithium hexafluoro phosphate, double fluorine sulfimide lithiums, difluorine oxalic acid boracic acid lithium, bis- (three
Methyl fluoride sulphonyl) one of imine lithium and di-oxalate lithium borate or a variety of, interworking total amount is nonaqueous electrolytic solution gross mass
10%~25%.
A kind of lithium ion battery containing above-mentioned nonaqueous electrolytic solution, the lithium ion battery include nonaqueous electrolytic solution,
Positive plate, negative electrode tab and diaphragm.
The beneficial effect of the present invention compared with the existing technology is: nonaqueous electrolytic solution of the invention, the addition of phosphate type lithium salts
Agent can form the organic matter containing lithium in anode and negative terminal surface, lead lithium ion with high；Meanwhile compound containing S=O
The inorganic matter of high stable is formed in electrode surface.The synergistic effect of the two, so that battery has cycle life long at high temperature
With performance good under low temperature.
Specific embodiment
Below with reference to embodiment, further description of the technical solution of the present invention, and however, it is not limited to this, all right
Technical solution of the present invention is modified or equivalent replacement, without departing from the spirit of the technical scheme of the invention range, should all cover
Among protection scope of the present invention.
Embodiment 1
A kind of nonaqueous electrolytic solution is made of non-aqueous organic solvent, electric conducting lithium salt and additive, and the non-aqueous organic solvent accounts for
The 84.9% of nonaqueous electrolytic solution gross mass is made of, carbon cyclic solvent (ethylene carbonate) and linear solvent (methyl ethyl carbonate)
The mass ratio of vinyl acetate and methyl ethyl carbonate is 1:2.The electric conducting lithium salt is lithium hexafluoro phosphate, accounts for nonaqueous electrolytic solution gross mass
10%.The additive is bis- (malonic acid) lithium phosphates of 0.1% divinyl and 5% methane-disulfonic acid methylene ester.By this reality
The electrolyte of example is applied for LiNi0.6Co0.2Mn0.2O2In/graphite soft-package battery.
Embodiment 2
In the nonaqueous electrolytic solution of the present embodiment, non-aqueous organic solvent accounts for the 72.9% of nonaqueous electrolytic solution gross mass, by ring-type
The mass ratio of solvent (ethylene carbonate) and linear solvent (methyl ethyl carbonate) composition, ethylene carbonate and methyl ethyl carbonate is 1:
2.Electric conducting lithium salt is lithium hexafluoro phosphate, accounts for the 25% of nonaqueous electrolytic solution gross mass.Electrolysis additive is 2% diphenyl bis- (third
Diacid) lithium phosphate and 0.1%1,4- butyl sultone.The electrolyte of the present embodiment is used for LiNi0.5Co0.2Mn0.3O2/ graphite
In soft-package battery.
Embodiment 3
In the nonaqueous electrolytic solution of the present embodiment, non-aqueous organic solvent accounts for the 80% of nonaqueous electrolytic solution gross mass, by cyclic annular molten
Agent (ethylene carbonate) and linear solvents (methyl ethyl carbonate, dimethyl carbonate) composition, ethylene carbonate, methyl ethyl carbonate and carbon
The mass ratio of dimethyl phthalate is 1:1:1.Lithium hexafluoro phosphate accounts for the 15% of nonaqueous electrolytic solution gross mass.Electrolysis additive is
Bis- (the 4- fluorine malonic acid) lithium phosphates of bis- (malonic acid) lithium phosphates of 0.5% difluoro, 0.5% difluoro, 4% vinyl sulfonic acid lactone.It incite somebody to action this
The electrolyte of embodiment is used for LiNi0.8Co0.15Al0.05O2In/graphite soft-package battery.
Embodiment 4
In the nonaqueous electrolytic solution of the present embodiment, non-aqueous organic solvent accounts for the 87% of nonaqueous electrolytic solution gross mass, by cyclic annular molten
Agent (ethylene carbonate) and linear solvents (methyl ethyl carbonate, diethyl carbonate) composition, ethylene carbonate, methyl ethyl carbonate and carbon
The mass ratio of diethyl phthalate is 1:1:1.Lithium hexafluoro phosphate accounts for the 12% of nonaqueous electrolytic solution gross mass.Electrolysis additive is
0.3% difluoro bis- (4- fluorine malonic acid) lithium phosphates, 0.7% sulfuric acid vinyl ester.The electrolyte of the present embodiment is used for
LiNi0.5Co0.2Mn0.3O2In the compound soft-package battery of/silicon-carbon.
Comparative example 1
The electrolyte of this comparative example unlike the first embodiment, does not use bis- (malonic acid) the lithium phosphate chemical combination of divinyl
This electrolyte is applied to test its performance in battery by object in the same manner as shown in Example 1.
Comparative example 2
The electrolyte of this comparative example unlike the first embodiment, does not use methane-disulfonic acid methylene ester, this electrolyte is pressed
It is applied to test its performance in battery according to method same as Example 1.
Comparative example 3
The electrolyte of this comparative example as different from Example 2, does not use bis- (malonic acid) lithium phosphates of diphenyl, by this electricity
Solution liquid is applied to test its performance in battery according to method same as Example 2.
Comparative example 4
The electrolyte of this comparative example as different from Example 2, do not use Isosorbide-5-Nitrae-butyl sultone, by this electrolyte according to
Method same as Example 2 is applied to test its performance in battery.
Comparative example 5
The electrolyte of this comparative example as different from Example 3, do not use vinyl sulfonic acid lactone, by this electrolyte according to
The identical method of embodiment 3 is applied to test its performance in battery.
Comparative example 6
The electrolyte of this comparative example is as different from Example 3, double without using bis- (malonic acid) lithium phosphates of difluoro and difluoro
This electrolyte is applied to test its performance in battery according to method same as Example 3 by (4- fluorine malonic acid) lithium phosphate.
Comparative example 7
The electrolyte of this comparative example as different from Example 4, does not use bis- (the 4- fluorine malonic acid) lithium phosphates of difluoro, by this
Electrolyte is applied to test its performance in battery according to method same as Example 4.
Comparative example 8
The electrolyte of this comparative example as different from Example 4, do not use sulfuric acid vinyl ester, by this electrolyte according to reality
The identical method of example 4 is applied to be applied to test its performance in battery.
The application experiment of embodiment and comparative example:
45 degree of loop tests: in order to measure the high-temperature behavior using lithium ion battery made from nonaqueous electrolytic solution of the present invention,
Perform the following operation: battery is placed in 45 degree with charge and discharge cycles under 2.75~4.35V 1C multiplying power.
Low temperature discharge test: the cryogenic property in order to measure lithium ion battery produced by the present invention performs the following operation: will
Battery normal temperature circulation one week, discharge capacity remembered Q0；Then by battery it is fully charged be placed on -30 degree shelve 4 hours after 0.5C multiplying power
Electric discharge, capacity remember Q1.Discharge capacitance=Q1/Q0
The high temperature cyclic performance and low temperature discharge test result table of 1 embodiment and comparative example of table
As can be seen from Table 1, when phosphate type lithium salt compound and compound containing S=O are simultaneously in use, the height of battery
Temperature stability and cryogenic property are significantly improved, and the present invention uses phosphate type lithium salt compound and the compound containing S=O
The lithium ion battery of combination preparation has advantage outstanding, is mainly manifested in the high temperature circulation capacity retention ratio for improving battery and mentions
Rise battery low temperature discharge capacity conservation rate.Examples 1 to 4 is substantially better than its comparative example.Therefore non-aqueous solution electrolysis of the invention is applied
Liquid can make battery have high cryogenic property and durability, have high market value and social benefit.
Claims (7)
1. a kind of nonaqueous electrolytic solution, including non-aqueous organic solvent, electric conducting lithium salt and additive, it is characterised in that: the addition
Agent is made of at least one phosphate type lithium salt compound and at least one compound containing S=O.
2. nonaqueous electrolytic solution according to claim 1, it is characterised in that: the phosphate type lithium salt compound has formula
(I) general structure shown in:
Wherein, R1、R4For hydrogen, C1~4Alkylidene, C1~4Halogeno alkylen or C1~4Alkenylene；R2、R3For hydrogen, halogen, C1~4Alkyl,
C1~4Halogenated alkyl, C6~10Aryl, C6~10Halogenated aryl, C1-C4Itrile group, C1-C6Alkenyl, alkoxy or carboxyl.
3. nonaqueous electrolytic solution according to claim 2, it is characterised in that: the phosphate type lithium salt compound is diethyl
Bis- (malonic acid) lithium phosphates of alkenyl, bis- (malonic acid) lithium phosphates of diphenyl, bis- (malonic acid) lithium phosphates of difluoro or bis- (the 4- fluorine of difluoro
Malonic acid) one or more of lithium phosphate mixture, dosage accounts for the 0.1%~10% of nonaqueous electrolytic solution gross mass.
4. nonaqueous electrolytic solution according to claim 1, it is characterised in that: the compound containing S=O is two sulphur of methane
Sour methylene ester, sulfuric acid vinyl ester, sulfuric acid acrylic ester, 1,3-propane sultone, Isosorbide-5-Nitrae-butyl sultone, vinyl sulfonic acid lactone, 1,
3- propene sultone, Isosorbide-5-Nitrae-butylene sultones, 1- methyl-1,3- propene sultone, divinylsulfone, dimethyl sulfone,
The mixture of one or more of diethyl sulfone, Methylethyl sulfone or methyl ethylene sulfone, it is total that dosage accounts for nonaqueous electrolytic solution
The 0.1%~10% of quality.
5. nonaqueous electrolytic solution according to claim 1, it is characterised in that: the non-aqueous organic solvent by cyclic solvent and
Linear solvents composition, wherein the cyclic solvent is ethylene carbonate, propene carbonate, fluorinated ethylene carbonate, γ-fourth
One of lactone and gamma-valerolactone or multiple combinations；The linear solvents are dimethyl carbonate, methyl ethyl carbonate, carbonic acid
Diethylester, methyl propyl carbonate, ethyl propionate, ethyl propionate, 1,1,2,3- tetra- fluoro ethyl -2,2, one in 3,3- tetrafluoro propyl ethers
Kind or multiple combinations, interworking total amount are the 55%~89.8% of nonaqueous electrolytic solution gross mass.
6. nonaqueous electrolytic solution according to claim 1, it is characterised in that: the electric conducting lithium salt is lithium hexafluoro phosphate, double
Fluorine sulfimide lithium, difluorine oxalic acid boracic acid lithium, bis- (trimethyl fluoride sulfonyl) one of imine lithiums and di-oxalate lithium borate or more
Kind, interworking total amount is the 10%~25% of nonaqueous electrolytic solution gross mass.
7. a kind of lithium ion battery containing nonaqueous electrolytic solution described in claim 1~6 any claim, feature exist
In: the lithium ion battery includes nonaqueous electrolytic solution, positive plate, negative electrode tab and diaphragm.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201910100098.0A CN109818060A (en) | 2019-01-31 | 2019-01-31 | Nonaqueous electrolytic solution and lithium ion battery containing the nonaqueous electrolytic solution |
| PCT/CN2020/073012 WO2020156282A1 (en) | 2019-01-31 | 2020-01-19 | Non-aqueous electrolyte solution and lithium ion battery containing non-aqueous electrolyte solution |
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| CN201910100098.0A CN109818060A (en) | 2019-01-31 | 2019-01-31 | Nonaqueous electrolytic solution and lithium ion battery containing the nonaqueous electrolytic solution |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111293362A (en) * | 2020-04-08 | 2020-06-16 | 河南华瑞高新材料有限公司 | Electrolyte suitable for nickel-manganese system |
| WO2020156282A1 (en) * | 2019-01-31 | 2020-08-06 | 珠海冠宇电池股份有限公司 | Non-aqueous electrolyte solution and lithium ion battery containing non-aqueous electrolyte solution |
| CN111883842A (en) * | 2020-08-07 | 2020-11-03 | 香河昆仑化学制品有限公司 | Functional non-aqueous organic additive for non-aqueous electrolyte |
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| CN102893442A (en) * | 2010-05-12 | 2013-01-23 | 三菱化学株式会社 | Non-aqueous electrolytic solution, and non-aqueous electrolyte secondary battery |
| CN103098290A (en) * | 2010-10-22 | 2013-05-08 | 三井化学株式会社 | Cyclic sulfate compound, non-aqueous electrolyte solution containing same, and lithium secondary battery |
| WO2016208738A1 (en) * | 2015-06-26 | 2016-12-29 | セントラル硝子株式会社 | Additive for nonaqueous electrolyte solution, manufacturing method for same, nonaqueous electrolyte solution, nonaqueous electrolyte secondary battery |
| CN107534185A (en) * | 2015-05-26 | 2018-01-02 | 三井化学株式会社 | Nonaqueous electrolyte for battery and lithium secondary battery |
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| JP2006032300A (en) * | 2004-07-21 | 2006-02-02 | Sony Corp | Electrolyte and battery |
| JP6913159B2 (en) * | 2017-03-30 | 2021-08-04 | 三井化学株式会社 | Non-aqueous electrolyte for batteries and lithium secondary battery |
| CN109818060A (en) * | 2019-01-31 | 2019-05-28 | 珠海光宇电池有限公司 | Nonaqueous electrolytic solution and lithium ion battery containing the nonaqueous electrolytic solution |
-
2019
- 2019-01-31 CN CN201910100098.0A patent/CN109818060A/en active Pending
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- 2020-01-19 WO PCT/CN2020/073012 patent/WO2020156282A1/en active Application Filing
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102893442A (en) * | 2010-05-12 | 2013-01-23 | 三菱化学株式会社 | Non-aqueous electrolytic solution, and non-aqueous electrolyte secondary battery |
| CN103098290A (en) * | 2010-10-22 | 2013-05-08 | 三井化学株式会社 | Cyclic sulfate compound, non-aqueous electrolyte solution containing same, and lithium secondary battery |
| CN107534185A (en) * | 2015-05-26 | 2018-01-02 | 三井化学株式会社 | Nonaqueous electrolyte for battery and lithium secondary battery |
| WO2016208738A1 (en) * | 2015-06-26 | 2016-12-29 | セントラル硝子株式会社 | Additive for nonaqueous electrolyte solution, manufacturing method for same, nonaqueous electrolyte solution, nonaqueous electrolyte secondary battery |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2020156282A1 (en) * | 2019-01-31 | 2020-08-06 | 珠海冠宇电池股份有限公司 | Non-aqueous electrolyte solution and lithium ion battery containing non-aqueous electrolyte solution |
| CN111293362A (en) * | 2020-04-08 | 2020-06-16 | 河南华瑞高新材料有限公司 | Electrolyte suitable for nickel-manganese system |
| CN111883842A (en) * | 2020-08-07 | 2020-11-03 | 香河昆仑化学制品有限公司 | Functional non-aqueous organic additive for non-aqueous electrolyte |
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| WO2020156282A1 (en) | 2020-08-06 |
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Address after: 519180 No. 209 Pearl Peak Avenue, Jingan Town, Doumen District, Zhuhai City, Guangdong Province Applicant after: Zhuhai Guanyu Battery Co., Ltd Address before: 519180 No. 209 Pearl Peak Avenue, Jingan Town, Doumen District, Zhuhai City, Guangdong Province Applicant before: ZHUHAI COSLIGHT BATTERY Co.,Ltd. |
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Application publication date: 20190528 |