CN110957527A - Non-aqueous electrolyte and secondary battery - Google Patents
Non-aqueous electrolyte and secondary battery Download PDFInfo
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- CN110957527A CN110957527A CN201811130326.0A CN201811130326A CN110957527A CN 110957527 A CN110957527 A CN 110957527A CN 201811130326 A CN201811130326 A CN 201811130326A CN 110957527 A CN110957527 A CN 110957527A
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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 relates to a non-aqueous electrolyte, which comprises a solvent, a lithium salt and an additive, wherein the additive comprises an additive A, an additive B and an additive C, the additive A is one or more of saturated dinitrile compounds, the additive B is one or more of trinitrile compounds and/or one or more of unsaturated dinitrile compounds, and the additive C is one or more of sulfur-containing compounds with the carbon atom number less than 4. The non-aqueous electrolyte of the present invention can suppress decomposition of the electrolyte at high voltage by using three additives in combination, which improves cycle performance and high-temperature storage performance of the battery. The secondary battery of the present invention can exhibit excellent cycle performance and high-temperature storage performance at high voltage.
Description
Technical Field
The invention belongs to the technical field of materials, and particularly relates to a non-aqueous electrolyte and a secondary battery.
Background
In recent years, the popularization of portable electronic devices such as mobile phones, tablet computers, and notebook computers has promoted the development of high energy density secondary batteries. Among many secondary batteries, a lithium ion secondary battery that realizes energy conversion by insertion and extraction of lithium ions has a higher energy density than a lead-acid battery and a nickel-metal hydride battery, and has been developed rapidly since the world, and its application fields include digital products, electric tools, electric vehicles, communication base stations, power grid energy storage, and the like.
The secondary battery mainly includes a positive electrode, a negative electrode, a separator, and an electrolyte. The electrolyte serves as a medium for charge and discharge reactions and has an important influence on the performance of the secondary battery.
By using LiCoO2Or LiNi0.5Co0.2Mn0.3O2In the case of a positive electrode active material, in order to obtain a higher battery capacity, the charge cut-off voltage is sometimes set to 4.4V or more, and under such a high voltage environment, the oxidation of the positive electrode material increases, and the electrolytic solution is easily oxidized and decomposed on the positive electrode side; at the same time, the transition metal ions are eluted, reduced and deposited on the negative electrode side, and the migration of lithium ions is inhibited. Therefore, protection of the positive electrode surface of the battery at high voltage is particularly important.
In a lithium ion secondary battery using a carbon or silicon material as a negative electrode active material, the negative electrode active material is likely to react with an electrolyte solution during charge and discharge to decompose the electrolyte solution, and the electrolyte solution is generally formed into a solid electrolyte interface film (SEI) on the surface of the negative electrode by an additive, whereby the decomposition reaction of solvent molecules in the electrolyte solution can be suppressed. By adding Vinylene Carbonate (VC) into the electrolyte, the function of forming a film on the surface of a carbon and silicon cathode can be achieved, however, when the battery is in a high-temperature environment, the surface film formed by the VC is easy to decompose, the protection function is weakened, and gas generation and internal resistance of the battery can be increased.
Patent document US8808918B2 discloses that the high-temperature cycle performance of a battery is improved by adding a dinitrile compound to an electrolyte.
Patent document CN104766995B discloses that the cycle performance and high-temperature storage performance of a high-voltage battery are improved by adding a polynitrile-based compound and a compound containing a sulfur-oxygen-containing double bond to an electrolytic solution.
The inventor finds that in the high-voltage battery, the scheme needs to be further optimized to meet the practical application requirement.
Disclosure of Invention
The technical problem to be solved by the invention is to provide a non-aqueous electrolyte which is applied to a lithium ion battery and can improve the cycle performance and the high-temperature storage performance of the high-voltage lithium ion battery.
In order to achieve the purpose, the invention adopts the technical scheme that:
the invention aims to provide a non-aqueous electrolyte which comprises a solvent, a lithium salt and an additive, wherein the additive comprises an additive A, an additive B and an additive C, the additive A is one or more of saturated dinitrile compounds, the additive B is one or more of trinitrile compounds and/or unsaturated dinitrile compounds, and the additive C is one or more of sulfur-containing compounds with the carbon number less than 4.
The additive A is preferably added in an amount of 0.1 to 5%, more preferably 1 to 5%, and still more preferably 2 to 3% based on the total mass of the nonaqueous electrolytic solution.
The additive B is preferably added in an amount of 0.1 to 4%, more preferably 1 to 4%, and still more preferably 2 to 4% of the total mass of the nonaqueous electrolytic solution.
The additive C is preferably added in an amount of 0.1 to 5%, more preferably 1 to 5%, based on the total mass of the nonaqueous electrolytic solution.
Preferably, the saturated dinitrile compound is one or more of succinonitrile, glutaronitrile, adiponitrile, suberonitrile, sebaconitrile and glycol (dipropionitrile) ether.
Preferably, the trinitrile compound is one or more of 1,2, 3-propanetrinitrile, 1,3, 5-pentatrinitrile and 1,3, 6-hexanetricarbonitrile.
Preferably, the unsaturated dinitrile compound is 1, 4-dicyano-2-butene.
Preferably, the sulfur-containing compound with the carbon number less than 4 is one or more of 1,3- (1-propylene) sultone, vinyl sulfate, vinyl sulfite and allyl sulfate.
Preferably, the lithium salt is one or more of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium hexafluoroarsenate, anhydrous lithium perchlorate, lithium bis (trifluoromethylsulfonyl) imide, lithium trifluoromethylsulfonate, lithium dioxalate borate, lithium monooxalatedifluoroborate and lithium difluorosulfonimide. Further preferably, the lithium salt is lithium hexafluorophosphate.
Preferably, the concentration of the lithium salt is 0.9-1.5 mol/L.
Preferably, the solvent is one or more of ethylene carbonate, propylene carbonate, gamma-butyrolactone, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl propyl carbonate, methyl propionate, ethyl propionate, propyl propionate, methyl acetate, ethyl acetate, propyl acetate, methyl butyrate, ethyl butyrate, propyl butyrate, sulfolane, diethylene glycol dimethyl ether and triethylene glycol dimethyl ether.
Another object of the present invention is to provide a secondary battery comprising an electrolytic solution, a separator, a positive electrode and a negative electrode capable of absorbing and desorbing lithium ions, wherein the electrolytic solution is the above-mentioned nonaqueous electrolytic solution.
Preferably, the active material of the positive electrode is LiCoO2、LiNixCoyMn1-x-yO2、LiNixCoyAl1-x-yO2The active material of the negative electrode is graphite and/or silicon material.
The saturated dinitrile compound, the trinitrile compound/unsaturated dinitrile compound and the sulfur-containing compound with the carbon atom number less than 4 can form a protective film (CEI) on the surface of the positive electrode, and the three additives have synergistic effect to perfect the protection of the positive electrode in a high-voltage battery. In addition, the sulfur-containing compound can also form a protective film (SEI) on the surface of the negative electrode. However, when the number of carbon atoms in the sulfur-containing compound is not less than 4, adverse effects such as increase in internal resistance of the battery, lithium deposition on the surface of the negative electrode, and deterioration in cycle performance are caused.
Due to the application of the technical scheme, compared with the prior art, the invention has the following advantages:
the non-aqueous electrolyte of the present invention can suppress decomposition of the electrolyte at high voltage by using three additives in combination, which improves cycle performance and high-temperature storage performance of the battery.
The secondary battery of the present invention can exhibit excellent cycle performance and high-temperature storage performance at high voltage.
Detailed Description
The present application will be described in detail with reference to examples, but the present application is not limited to these examples. In this specification, "%" represents mass% unless otherwise specified.
Example 1:
[ production of Positive electrode ]
Weighing LiCoO according to the mass ratio of 90:5:52And adding a proper amount of NMP into the conductive carbon black and the PVDF, and fully stirring to obtain the anode slurry. And coating the anode slurry on an aluminum foil, drying, rolling and cutting to obtain the anode.
[ production of negative electrode ]
Weighing graphite, styrene butadiene rubber and carboxymethyl cellulose according to the mass ratio of 95:3:2, adding a proper amount of deionized water, and fully stirring to obtain the cathode slurry. And coating the negative electrode slurry on a copper foil, drying, rolling and cutting to obtain the negative electrode.
[ preparation of electrolyte ]
Ethylene Carbonate (EC), diethyl carbonate (DEC) and Ethyl Propionate (EP) were mixed in a mass ratio of 30:40:30 to obtain a mixed solvent, and lithium hexafluorophosphate was dissolved therein at a concentration of 1 mol/l. Adding succinonitrile (ADN) accounting for 1% of the mass fraction of the electrolyte, 1% of 1,3, 6-Hexanetricarbonitrile (HTN) and 1% of 1,3- (1-propylene) sultone (PRS), and fully dissolving to obtain the electrolyte.
[ production of Battery ]
The positive electrode, the negative electrode and the electrolyte are used, a PE diaphragm with the thickness of 20 micrometers is selected, and a winding process is adopted to manufacture the soft package battery with the model number of 053048.
[ Battery Performance test ]
The voltage range of the battery charging and discharging test is 3.0-4.45V. After the cells were formed at a rate of 0.1C at 25 ℃, they were pre-cycled at a rate of 0.2C for 3 weeks. And then carrying out high-temperature storage performance test and normal-temperature cycle performance test.
High temperature storage performance test the cells were first charged at 25 ℃ to 4.45V at a constant current of 0.5C, charged at constant voltage until the current dropped to 0.05C, and then placed in an oven at 60 ℃ for 7 days. The thickness of the battery before and after storage was tested. Thickness change rate ═ 100% of [ (thickness after storage-thickness before storage)/thickness before storage ]. The cell was then discharged to 3.0V at 25 ℃ at 0.5C. The remaining capacity rate of the battery was tested. The remaining capacity rate (discharge capacity after storage/charge capacity before storage) is 100%.
The normal temperature cycle performance test is to cycle the battery at 25 ℃ for 500 weeks at 0.5C to calculate the capacity retention rate. Capacity retention rate (500-cycle discharge capacity/first-cycle discharge capacity) × 100%.
Examples 2 to 13, comparative examples 1 to 9:
a battery was fabricated in the same manner as in example 1, except that the additive was changed. The battery performance test was performed in the same manner as in example 1.
The components and mass fractions of the additives of examples 1 to 13 and comparative examples 1 to 9, and the results of the battery performance test are shown in Table 1.
Wherein succinonitrile is abbreviated as SN, sebaconitrile is abbreviated as SBN, ethylene glycol (dipropionitrile) ether is abbreviated as DENE, 1, 4-dicyano-2-butene is abbreviated as DCB, 1,3, 6-hexanetricarbonitrile is abbreviated as HTN, 1,3- (1-propene) sultone is abbreviated as PRS, vinyl sulfate is abbreviated as ESA, vinylene carbonate is abbreviated as VC, 1, 3-propanesultone is abbreviated as PS, and 1, 4-butanesultone is abbreviated as BS.
TABLE 1
The test data for the cells prepared from the additive-containing nonaqueous electrolyte solutions of the examples and comparative examples in table 1 show that the conventional additive VC + PS combination has poor high-temperature storage and normal-temperature cycle performance in high-voltage cells, mainly because VC is easily oxidized at high voltage and VC + PS cannot exert a good performance improvement effect in high-voltage cells; the battery performance is also poor when a saturated dinitrile compound, a trinitrile compound, a sulfur-containing compound with the carbon number less than 4 are used alone or in combination. When a combination of a saturated dinitrile compound, a trinitrile compound and/or a saturated dinitrile compound, a sulfur-containing compound having a carbon number of less than 4 is used, the high-temperature shelf performance and the cycle performance of the battery are remarkably improved. When the sulfur compound has 4 carbon atoms (comparative examples 7 and 9), its effect of improving the above-mentioned battery performance is reduced.
The above embodiments are merely illustrative of the technical concept and features of the present invention, and the purpose thereof is to enable those skilled in the art to understand the content of the present invention and implement the invention, and not to limit the scope of the invention, and all equivalent changes or modifications made according to the spirit of the present invention should be covered by the scope of the present invention.
Claims (10)
1. A non-aqueous electrolyte comprising a solvent, a lithium salt and an additive, characterized in that: the additive comprises an additive A, an additive B and an additive C, wherein the additive A is one or more of saturated dinitrile compounds, the additive B is one or more of trinitrile compounds and/or one or more of unsaturated dinitrile compounds, and the additive C is one or more of sulfur-containing compounds with the carbon atom number less than 4.
2. The nonaqueous electrolytic solution of claim 1, wherein: the additive A is added in an amount of 0.1 to 5 percent of the total mass of the non-aqueous electrolyte; the additive B is added in an amount of 0.1 to 4 percent of the total mass of the nonaqueous electrolyte; the additive C is added in an amount of 0.1 to 5 percent of the total mass of the nonaqueous electrolyte.
3. The nonaqueous electrolytic solution of claim 1 or 2, wherein: the saturated dinitrile compound is one or more of succinonitrile, glutaronitrile, adiponitrile, suberonitrile, sebaconitrile and glycol (dipropionitrile) ether.
4. The nonaqueous electrolytic solution of claim 1 or 2, wherein: the trinitrile compound is one or more of 1,2, 3-propanetrinitrile, 1,3, 5-pentanitrile and 1,3, 6-hexanetricarbonitrile.
5. The nonaqueous electrolytic solution of claim 1 or 2, wherein: the unsaturated dinitrile compound is 1, 4-dicyano-2-butene.
6. The nonaqueous electrolytic solution of claim 1 or 2, wherein: the sulfur-containing compound with the carbon atom number less than 4 is one or more of 1,3- (1-propylene) sultone, vinyl sulfate, vinyl sulfite and allyl sulfate.
7. The nonaqueous electrolytic solution of claim 1, wherein: the lithium salt is one or more of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium hexafluoroarsenate, anhydrous lithium perchlorate, lithium bis (trifluoromethylsulfonyl) imide, lithium trifluoromethylsulfonate, lithium dioxalate borate, lithium monooxalatedifluoroborate and lithium difluorosulfimide, and the concentration of the lithium salt is 0.9-1.5 mol/L.
8. The nonaqueous electrolytic solution of claim 1, wherein: the solvent is one or more of ethylene carbonate, propylene carbonate, gamma-butyrolactone, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl propyl carbonate, methyl propionate, ethyl propionate, propyl propionate, methyl acetate, ethyl acetate, propyl acetate, methyl butyrate, ethyl butyrate, propyl butyrate, sulfolane, diethylene glycol dimethyl ether and triethylene glycol dimethyl ether.
9. A secondary battery comprising an electrolyte, a separator, a positive electrode and a negative electrode capable of absorbing and desorbing lithium ions, characterized in that: the electrolyte is the nonaqueous electrolyte solution of any one of claims 1 to 8.
10. The secondary battery according to claim 9, characterized in that: the active material of the positive electrode is LiCoO2、LiNixCoyMn1-x-yO2、LiNixCoyAl1-x-yO2The active material of the negative electrode is graphite and/or silicon material.
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Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105552439A (en) * | 2015-12-16 | 2016-05-04 | 东莞市杉杉电池材料有限公司 | Electrolyte of rapid-charging lithium ion battery |
| US20160294007A1 (en) * | 2015-03-31 | 2016-10-06 | Ningde Contemporary Amperex Technology Limited | Electrolyte additive and use thereof in lithium-ion battery |
| CN106099187A (en) * | 2016-07-13 | 2016-11-09 | 东莞市凯欣电池材料有限公司 | A kind of wide homogeneous non-aqueous electrolytic solution of warm area |
| CN106159330A (en) * | 2016-10-08 | 2016-11-23 | 东莞市凯欣电池材料有限公司 | A kind of PC base high-voltage electrolyte and a kind of lithium ion battery |
| CN108598488A (en) * | 2018-06-08 | 2018-09-28 | 东莞市杉杉电池材料有限公司 | A kind of lithium ion battery with high energy density and its electrolyte |
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20160294007A1 (en) * | 2015-03-31 | 2016-10-06 | Ningde Contemporary Amperex Technology Limited | Electrolyte additive and use thereof in lithium-ion battery |
| CN105552439A (en) * | 2015-12-16 | 2016-05-04 | 东莞市杉杉电池材料有限公司 | Electrolyte of rapid-charging lithium ion battery |
| CN106099187A (en) * | 2016-07-13 | 2016-11-09 | 东莞市凯欣电池材料有限公司 | A kind of wide homogeneous non-aqueous electrolytic solution of warm area |
| CN106159330A (en) * | 2016-10-08 | 2016-11-23 | 东莞市凯欣电池材料有限公司 | A kind of PC base high-voltage electrolyte and a kind of lithium ion battery |
| CN108598488A (en) * | 2018-06-08 | 2018-09-28 | 东莞市杉杉电池材料有限公司 | A kind of lithium ion battery with high energy density and its electrolyte |
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