CN111029656A - Lithium ion battery non-aqueous electrolyte and lithium ion battery thereof - Google Patents
Lithium ion battery non-aqueous electrolyte and lithium ion battery thereof Download PDFInfo
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- CN111029656A CN111029656A CN201911336230.4A CN201911336230A CN111029656A CN 111029656 A CN111029656 A CN 111029656A CN 201911336230 A CN201911336230 A CN 201911336230A CN 111029656 A CN111029656 A CN 111029656A
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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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- 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 invention discloses a lithium ion battery non-aqueous electrolyte, which comprises a lithium salt, an organic solvent and an additive, wherein the additive comprises the following components in percentage by mass in the lithium ion battery non-aqueous electrolyte: 0.5-2% of lithium salt additive, 0.2-1.0% of high-temperature additive and 0.2-5% of other additives. The invention also discloses a lithium ion battery. The lithium ion battery can give consideration to high and low temperature performances and broaden the temperature range of the lithium ion battery.
Description
Technical Field
The invention relates to the field of lithium ion batteries, in particular to a wide-temperature lithium ion battery non-aqueous electrolyte for high voltage and a lithium ion battery.
Background
The electrolyte in the lithium ion battery is a medium for connecting the positive electrode and the negative electrode, is a transmission medium of lithium ions, and has an extremely important function. Generally, the main components of the electrolyte include an organic solvent, a lithium salt, an additive, and the like. Wherein the lithium salt provides lithium ions for internal current transmission; the organic solvent functions to dissolve the lithium salt, producing solvated lithium ions; the additive has a plurality of types, and plays a role in improving the stability, the cyclicity, the safety and other aspects of the performance of the lithium ion battery.
The SEI film is a passivation film covering the surface of an electrode generated by the reaction of an electrode material and an electrolyte (a film forming agent) in the first charge-discharge cycle of the lithium ion battery. The performance of the SEI film greatly influences the electrochemical properties of the lithium ion battery, such as first irreversible capacity loss, rate capability, cycle life and the like. The ideal SEI film allows lithium ions to freely enter and exit from the electrode while insulating electron transport, prevents further reaction of the electrode material and the electrolyte, has a stable structure, and is insoluble in organic solvents.
At present, the main problem facing lithium ion batteries is that high and low temperatures cannot be considered, i.e. the lithium ion batteries cannot have excellent chemical properties at high and low temperatures. Under the high temperature condition, because the electrolyte in the lithium ion battery is easy to be catalytically decomposed on the surface of the anode, the battery expands, the capacity is reduced, and the like, a catalyst with excellent anode film-forming property is required to be added to complex metal ions, passivate the active sites of the anode, and the like; the addition of the additives can cause the impedance of the battery to be remarkably improved, and the rate capability and the low-temperature use effect of the battery are seriously influenced.
Disclosure of Invention
The invention aims to provide a lithium ion battery electrolyte and a lithium ion battery containing the same.
In order to achieve the purpose, the invention adopts the technical scheme that: the lithium ion battery non-aqueous electrolyte comprises a lithium salt, an organic solvent and an additive, wherein the additive comprises the following components in percentage by mass in the lithium ion battery non-aqueous electrolyte:
0.5 to 2 percent of lithium salt additive
0.2 to 1.0 percent of high-temperature additive
0.2 to 5 percent of other additives
In a preferred embodiment of the present invention, the lithium salt additive is lithium difluorophosphate and oxalate, and the structural formula of the lithium salt additive is as follows:
as a preferred embodiment of the present invention, the high temperature additive is selected from one or more of the compounds represented by the following structural formula:
in a preferred embodiment of the present invention, the lithium salt is preferably LiPF6、LiBF4、LiClO4、LiBOB、LiODFB、LiAsF6、LiN(SO2CF3)2、LiN(SO2F)2One or more of (a).
In a preferred embodiment of the present invention, the concentration of the lithium salt in the nonaqueous electrolyte solution of the lithium ion battery is 0.5 to 2 mol/L.
Other additives in the present invention may be at least one selected from the group consisting of Vinylene Carbonate (VC), Vinyl Ethylene Carbonate (VEC), fluoroethylene carbonate (FEC), 1, 3-Propane Sultone (PS), 1, 4-Butane Sultone (BS), ethylene sulfate (DTD), Methylene Methanedisulfonate (MMDS), propylene sulfate (TS), lithium Difluorophosphate (DFP), diphenyl carbonate (DPC), tolyl carbonate (MPC), Succinonitrile (SN), Adiponitrile (ADN), Hexanetricarbonitrile (HTCN), fluorobenzene, 3-fluorobiphenyl and 3, 5-difluorobiphenyl. The other additive is more preferably a mixture of vinylene carbonate, vinyl sulfate and lithium difluorophosphate, and the mass ratio of the vinylene carbonate, the vinyl sulfate and the lithium difluorophosphate in the mixture is preferably 1:0.5-2: 0.6-1.
In the present invention, the organic solvent may be one or more selected from the group consisting of chain carbonates, cyclic carbonates, carboxylic esters, fluoroethers, fluorocarbons and fluorocarboxylic ester organic solvents. As a preferred embodiment of the present invention, the organic solvent is preferably dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, dipropyl carbonate, ethylene carbonate, vinylene carbonate, propylene carbonate, ethyl acetate, ethyl propionate, methyl acetate, propyl acetate, methyl propionate, methyl butyrate, ethyl butyrate, fluoromethyl-1, 1,1,3,3, 3-hexafluoroisopropyl ether, 1,1,2, 2-tetrafluoroethyl ethyl ether, 2, 6-difluoroanisole, 1,1,1,3,3, 3-hexafluoroisopropyl methyl ether, tetrafluoromethylbutyl ether, 1,1,3,3, 3-pentafluoro-2-trifluoromethylpropyl methyl ether, 1,1,2, 2-tetrafluoroethyl-2, 2, 2-trifluoroethyl ether, 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether and 1,1,2, 2-tetrafluoroethyl-4-methylphenyl ether. The organic solvent is more preferably a mixture of ethylene carbonate, propylene carbonate, ethyl methyl carbonate and diethyl carbonate.
The invention also provides a lithium ion battery which comprises a positive pole piece, a negative pole piece, a diaphragm and the lithium ion battery non-aqueous electrolyte.
The lithium salt additive in the non-aqueous electrolyte can form a passivation film with excellent ion conductivity, reduces the impedance of the lithium ion battery, and has great benefit for improving the low-temperature circulation effect; the high-temperature additive can passivate active sites of the positive electrode, so that the non-aqueous electrolyte has good cyclicity at high temperature and high voltage, and the matching use of the lithium salt additive and the high-temperature additive can ensure that the lithium ion battery can give consideration to high and low temperature performances and widen the temperature range of the lithium ion battery. The inventor finds that the SEI film formed by the lithium salt additive has good lithium ion conducting performance, can obviously reduce the internal resistance of the battery, and has the high temperature resistance and stability of an inorganic film and the toughness and coverage of an organic film through a plurality of tests. The high-temperature additive can complex metal ions dissolved out of the positive electrode or cover active sites of the positive electrode, inhibit catalytic decomposition of the electrolyte and improve high-temperature cycle performance.
Compared with the prior art, the invention has the advantages that:
1. the lithium salt additive in the non-aqueous electrolyte can form a high-quality SEI film with high temperature resistance and stability of an inorganic film, toughness and coverage of an organic film, so that the SEI film has excellent high and low temperature performance, particularly the formed SEI film has good lithium ion conductivity, can obviously reduce the internal resistance of a battery, and has good low-temperature discharge performance and low-temperature cycle performance under the low-temperature condition;
2. the high-temperature additive in the non-aqueous electrolyte can complex metal ions dissolved out of the positive electrode or cover active sites of the positive electrode, inhibit catalytic decomposition of the electrolyte and improve high-temperature cycle performance;
3. the non-aqueous electrolyte enables the lithium ion battery to have high and low temperature performance through the optimized formula and the synergistic effect of the lithium salt additive and the high-temperature additive, and widens the working temperature range of the lithium ion battery.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It is to be understood that the following description is only illustrative of the present invention and is not to be construed as limiting the present invention.
The lithium salt additive in the examples is lithium difluorophosphate oxalate, the structural formula of which is shown below:
the characterization was as follows:
the high temperature additive structures in the examples and comparative examples are characterized as follows:
compound II is of the formula:
compound III is of the formula:
compound IV structural formula is as follows:
compound V is of the formula:
compound VI structural formula is as follows:
compound VII is of the formula:
compound VIII structural formula is as follows:
compound IX structural formula is as follows:
compound X is of the formula:
example 1
The non-aqueous electrolyte is prepared by the following method: in a glove box, Ethylene Carbonate (EC), Propylene Carbonate (PC), diethyl carbonate (DEC) and Ethyl Methyl Carbonate (EMC) were mixed in a weight ratio of 30:5:20:45 to obtain a mixed solution, and then lithium hexafluorophosphate (LiPF) was added to the mixed solution6) And dissolving to obtain a solution containing lithium hexafluorophosphate. Then, Vinylene Carbonate (VC), vinyl sulfate (DTD), lithium Difluorophosphate (DFP), compound II, and lithium difluorophosphate oxalate represented by structural formula I were added to the lithium hexafluorophosphate-containing solution, and stirred uniformly to obtain the nonaqueous electrolytic solution of example 1. The concentration of lithium hexafluorophosphate in the electrolyte was 1.15M, the mass percentage of Vinylene Carbonate (VC) in the electrolyte was 0.5%, and the ethylene sulfate (DTD) was chargedThe mass percentage of the electrolyte solution is 1%, the mass percentage of lithium Difluorophosphate (DFP) in the electrolyte solution is 0.5%, the mass percentage of Propane Sultone (PS) shown in a structural formula II in the electrolyte solution is 0.5%, and the mass percentage of lithium difluorophosphate oxalate shown in a structural formula I in the electrolyte solution is 0.5%.
Examples 2 to 32
Examples 2-32 are also specific examples of electrolyte preparation, and the parameters and preparation method are the same as example 1 except for the parameters in Table 1. The electrolyte formulation is shown in table 1.
Comparative examples 1 to 23
Comparative examples 1-23 were prepared according to the same procedure as in example 1, except for the parameters shown in Table 1. The electrolyte formulation is shown in table 1.
TABLE 1 formulation composition of electrolyte in each example and comparative example
Note: the concentration of lithium salt is the molar concentration in the electrolyte;
the lithium salt additive, the high-temperature additive and other additives are contained in the electrolyte by mass percent;
the proportion of each component in the nonaqueous solvent is a weight ratio.
Lithium ion battery performance testing
Preparing a lithium ion battery:
the lithium ion batteries prepared in the examples and comparative examples were charged into a fully dried 4.35V NCM (nickel: cobalt: manganese ═ 6:2: 2)/graphite pouch battery, and the resultant was subjected to steps of standing at 45 ℃, high-temperature chucking, secondary sealing, and the like, to obtain a lithium ion battery. The cell performance tests were performed and the results are shown in table 2. Wherein:
1. normal temperature cycle performance
Under the condition of normal temperature (25 ℃), the lithium ion battery is charged to 4.35V under the constant current and the constant voltage of 1C, and then is discharged to 3.0V under the constant current of 1C. After 500 cycles of charge and discharge, capacity retention rate after 500 cycles was calculated:
×100％
2. high temperature cycle performance
Under the condition of high temperature (45 ℃), the lithium ion battery is charged to 4.35V under the constant current and constant voltage of 1C, and then is discharged to 3.0V under the constant current of 1C. After 500 cycles of charge and discharge, capacity retention rate after 500 cycles was calculated:
×100％
3. high temperature storage Properties
The lithium ion battery was subjected to primary 1C/1C charging and discharging (discharge capacity is designated DC) at room temperature (25 ℃ C.)0) Then charging the battery to 4.35V under the condition of 1C constant current and constant voltage; the lithium ion battery is stored in a high-temperature box at 60 ℃ for 7 days, and after being taken out, 1C discharge (the discharge capacity is recorded as DC) is carried out at normal temperature1) (ii) a Then, 1C/1C charging and discharging (discharge capacity is designated as DC) were carried out under ambient conditions2) Calculating the capacity retention rate and the capacity recovery rate of the lithium ion battery by using the following formulas:
4. low temperature discharge performance
The lithium ion battery was subjected to primary 1C/1C charging and discharging (discharge capacity is designated DC) at room temperature (25 ℃ C.)0) Then charging the battery to a 4.35V full state (100% SOC) under 1C constant current and voltage conditions; placing the battery in an environment with an ambient temperature of-20 +/-2 ℃ for 4h, carrying out 1C rate discharge test, and recording 1C discharge capacity DC at a low temperature of-20 DEG C1Calculating the low-temperature discharge efficiency of the lithium ion battery by using the following formula:
the results of the battery performance tests of the above examples and comparative examples are shown in table 2.
Table 2 results of cell performance test of each example and comparative example
The test result of the embodiment shows that the lithium salt additive shown in the structural formula I has good high-temperature and low-temperature performance, is a good wide-temperature electrolyte additive, and has certain improvements on low-temperature discharge and normal-temperature circulation along with the increase of the amount of the lithium salt additive shown in the structural formula I, and the addition amount of 1.5% has the best effect; the lithium salt additive has good discharge efficiency at low temperature of-20 ℃, which is probably caused by that a film formed by the lithium salt additive shown in the structural formula I is mainly inorganic components, has good lithium ion permeability and electronic insulation property and low impedance;
the test results of the embodiment show that the lithium salt additive shown in the structural formula I and the high-temperature additive shown in the structural formula II-X are matched for use, so that the circulation effect of the lithium battery can be ensured, the high-temperature storage performance of the battery can be improved to a greater extent, and the wide-temperature lithium ion battery electrolyte can be obtained.
Through the experiments of the embodiment and the comparative example, the electrolyte disclosed by the invention can improve the high-temperature performance of the battery, inhibit the gas generation of the battery in a high-temperature environment and effectively reduce the expansion of the battery on the basis of ensuring the cycle performance.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. The non-aqueous electrolyte of the lithium ion battery comprises a lithium salt, an organic solvent and an additive, and is characterized in that the additive comprises the following components in percentage by mass in the non-aqueous electrolyte of the lithium ion battery:
0.5 to 2 percent of lithium salt additive
0.2 to 1.0 percent of high-temperature additive
0.2-5% of other additives.
2. The nonaqueous electrolyte solution for a lithium ion battery according to claim 1, wherein the lithium salt additive is lithium difluorophosphate oxalate.
3. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the high-temperature additive is one or more selected from compounds represented by the following structural formula:
4. the nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the lithium salt is LiPF6、LiBF4、LiClO4、LiBOB、LiODFB、LiAsF6、LiN(SO2CF3)2、LiN(SO2F)2One or more of (a).
5. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the concentration of the lithium salt in the nonaqueous electrolyte solution for lithium ion batteries is 0.5 to 2 mol/L.
6. The nonaqueous electrolyte solution for a lithium ion battery according to claim 1, wherein the other additive is at least one of vinylene carbonate, ethylene carbonate, fluoroethylene carbonate, 1, 3-propane sultone, 1, 4-butane sultone, ethylene sulfate, methylene methanedisulfonate, propylene sulfate, lithium difluorophosphate, diphenyl carbonate, tolyl carbonate, succinonitrile, adiponitrile, hexanetrinitrile, fluorobenzene, 3-fluorobiphenyl, and 3, 5-difluorobiphenyl.
7. The nonaqueous electrolyte for lithium ion batteries according to claim 6, wherein the other additive is a mixture of vinylene carbonate, vinyl sulfate and lithium difluorophosphate, and the mass ratio of vinylene carbonate, vinyl sulfate and lithium difluorophosphate in the mixture is 1:0.5-2: 0.6-1.
8. The nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the organic solvent is dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, dipropyl carbonate, ethylene carbonate, vinylene carbonate, propylene carbonate, ethyl acetate, ethyl propionate, methyl acetate, propyl acetate, methyl propionate, methyl butyrate, ethyl butyrate, fluoromethyl-1, 1,1,3,3, 3-hexafluoroisopropyl ether, 1,1,2, 2-tetrafluoroethyl ethyl ether, 2, 6-difluoroanisole, 1,1,1,3,3, 3-hexafluoroisopropyl methyl ether, tetrafluoromethylbutyl ether, 1,1,3,3, 3-pentafluoro-2-trifluoromethylpropyl methyl ether, 1,1,2, 2-tetrafluoroethyl-2, 2, 2-trifluoroethyl ether, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, dipropyl carbonate, ethylene carbonate, vinylene carbonate, propylene carbonate, ethyl acetate, ethyl propionate, methyl acetate, methyl propionate, methyl butyrate, ethyl butyrate, fluoromethyl-1, 1,1,3, 3-hexafluoro, 1,1,2, 2-tetrafluoroethyl-2, 2,3, 3-tetrafluoropropyl ether and 1,1,2, 2-tetrafluoroethyl-4-methylphenyl ether.
9. The nonaqueous electrolyte solution for lithium ion batteries according to claim 8, wherein the organic solvent is a mixture of ethylene carbonate, propylene carbonate, ethyl methyl carbonate and diethyl carbonate.
10. A lithium ion battery comprising a positive electrode sheet, a negative electrode sheet, a separator and the lithium ion battery nonaqueous electrolyte solution according to any one of claims 1 to 9.
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Cited By (7)
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| CN111883827A (en) * | 2020-07-16 | 2020-11-03 | 香河昆仑化学制品有限公司 | Non-aqueous electrolyte of lithium ion battery and lithium ion battery |
| CN112038697A (en) * | 2020-08-28 | 2020-12-04 | 香河昆仑化学制品有限公司 | Lithium ion battery non-aqueous electrolyte and lithium ion battery |
| CN112271338A (en) * | 2020-11-27 | 2021-01-26 | 凯博能源科技有限公司 | Electrolyte and lithium ion battery containing same |
| CN113675400A (en) * | 2020-05-15 | 2021-11-19 | 比亚迪股份有限公司 | Positive electrode, preparation method thereof and lithium ion battery |
| CN114649589A (en) * | 2020-12-18 | 2022-06-21 | 张家港市国泰华荣化工新材料有限公司 | Electrolyte and lithium secondary battery |
| WO2024021962A1 (en) * | 2022-07-28 | 2024-02-01 | 张家港市国泰华荣化工新材料有限公司 | Non-aqueous electrolyte solution and lithium ion battery |
| CN117855608A (en) * | 2024-03-07 | 2024-04-09 | 宁德新能源科技有限公司 | Electrolyte, secondary battery, and electronic device |
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| CN113675400A (en) * | 2020-05-15 | 2021-11-19 | 比亚迪股份有限公司 | Positive electrode, preparation method thereof and lithium ion battery |
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| CN117855608A (en) * | 2024-03-07 | 2024-04-09 | 宁德新能源科技有限公司 | Electrolyte, secondary battery, and electronic device |
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Application publication date: 20200417 |