CN114552001A - Electrolyte for improving high-temperature shelving performance of ternary lithium ion battery and application - Google Patents
Electrolyte for improving high-temperature shelving performance of ternary lithium ion battery and application Download PDFInfo
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- CN114552001A CN114552001A CN202011329342.XA CN202011329342A CN114552001A CN 114552001 A CN114552001 A CN 114552001A CN 202011329342 A CN202011329342 A CN 202011329342A CN 114552001 A CN114552001 A CN 114552001A
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- Prior art keywords
- electrolyte
- carbonate
- temperature
- lithium salt
- additive
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 71
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 30
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 29
- 229910003002 lithium salt Inorganic materials 0.000 claims description 46
- 159000000002 lithium salts Chemical class 0.000 claims description 46
- 239000000654 additive Substances 0.000 claims description 38
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 claims description 35
- 239000000203 mixture Substances 0.000 claims description 29
- 229910001290 LiPF6 Inorganic materials 0.000 claims description 28
- 229910010941 LiFSI Inorganic materials 0.000 claims description 27
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 22
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 19
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 17
- 230000000996 additive effect Effects 0.000 claims description 15
- 239000002904 solvent Substances 0.000 claims description 14
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 12
- -1 methylene cyclamate Chemical compound 0.000 claims description 12
- 229920001220 nitrocellulos Polymers 0.000 claims description 8
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 6
- IIPYXGDZVMZOAP-UHFFFAOYSA-N lithium nitrate Chemical compound [Li+].[O-][N+]([O-])=O IIPYXGDZVMZOAP-UHFFFAOYSA-N 0.000 claims description 6
- FGIUAXJPYTZDNR-UHFFFAOYSA-N potassium nitrate Chemical compound [K+].[O-][N+]([O-])=O FGIUAXJPYTZDNR-UHFFFAOYSA-N 0.000 claims description 6
- SQGYOTSLMSWVJD-UHFFFAOYSA-N silver(1+) nitrate Chemical compound [Ag+].[O-]N(=O)=O SQGYOTSLMSWVJD-UHFFFAOYSA-N 0.000 claims description 6
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 5
- 239000000020 Nitrocellulose Substances 0.000 claims description 4
- DKPFZGUDAPQIHT-UHFFFAOYSA-N butyl acetate Chemical compound CCCCOC(C)=O DKPFZGUDAPQIHT-UHFFFAOYSA-N 0.000 claims description 4
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Inorganic materials [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 claims description 4
- MHYFEEDKONKGEB-UHFFFAOYSA-N oxathiane 2,2-dioxide Chemical compound O=S1(=O)CCCCO1 MHYFEEDKONKGEB-UHFFFAOYSA-N 0.000 claims description 4
- 229910019142 PO4 Inorganic materials 0.000 claims description 3
- 229940109275 cyclamate Drugs 0.000 claims description 3
- BDUPRNVPXOHWIL-UHFFFAOYSA-N dimethyl sulfite Chemical compound COS(=O)OC BDUPRNVPXOHWIL-UHFFFAOYSA-N 0.000 claims description 3
- 239000010452 phosphate Substances 0.000 claims description 3
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 3
- 235000010333 potassium nitrate Nutrition 0.000 claims description 3
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Inorganic materials [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 claims description 3
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 2
- OQXNUCOGMMHHNA-UHFFFAOYSA-N 4-methyl-1,3,2-dioxathiolane 2,2-dioxide Chemical compound CC1COS(=O)(=O)O1 OQXNUCOGMMHHNA-UHFFFAOYSA-N 0.000 claims description 2
- SJHAYVFVKRXMKG-UHFFFAOYSA-N 4-methyl-1,3,2-dioxathiolane 2-oxide Chemical compound CC1COS(=O)O1 SJHAYVFVKRXMKG-UHFFFAOYSA-N 0.000 claims description 2
- 229910013188 LiBOB Inorganic materials 0.000 claims description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 2
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 claims description 2
- ACBQROXDOHKANW-UHFFFAOYSA-N bis(4-nitrophenyl) carbonate Chemical compound C1=CC([N+](=O)[O-])=CC=C1OC(=O)OC1=CC=C([N+]([O-])=O)C=C1 ACBQROXDOHKANW-UHFFFAOYSA-N 0.000 claims description 2
- NVJBFARDFTXOTO-UHFFFAOYSA-N diethyl sulfite Chemical compound CCOS(=O)OCC NVJBFARDFTXOTO-UHFFFAOYSA-N 0.000 claims description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 2
- 239000003759 ester based solvent Substances 0.000 claims description 2
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims description 2
- GJRQTCIYDGXPES-UHFFFAOYSA-N iso-butyl acetate Natural products CC(C)COC(C)=O GJRQTCIYDGXPES-UHFFFAOYSA-N 0.000 claims description 2
- FGKJLKRYENPLQH-UHFFFAOYSA-M isocaproate Chemical compound CC(C)CCC([O-])=O FGKJLKRYENPLQH-UHFFFAOYSA-M 0.000 claims description 2
- OQAGVSWESNCJJT-UHFFFAOYSA-N isovaleric acid methyl ester Natural products COC(=O)CC(C)C OQAGVSWESNCJJT-UHFFFAOYSA-N 0.000 claims description 2
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 claims description 2
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 claims description 2
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 2
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 claims description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 2
- 238000000354 decomposition reaction Methods 0.000 abstract description 5
- 238000011084 recovery Methods 0.000 abstract description 5
- 238000007086 side reaction Methods 0.000 abstract description 5
- 230000005540 biological transmission Effects 0.000 abstract description 3
- 230000002427 irreversible effect Effects 0.000 abstract description 3
- 230000014759 maintenance of location Effects 0.000 abstract description 3
- 230000002441 reversible effect Effects 0.000 abstract description 3
- 238000004090 dissolution Methods 0.000 abstract description 2
- 230000002401 inhibitory effect Effects 0.000 abstract 1
- 239000007784 solid electrolyte Substances 0.000 abstract 1
- 238000012360 testing method Methods 0.000 description 18
- 230000000052 comparative effect Effects 0.000 description 14
- 238000010998 test method Methods 0.000 description 11
- 238000000034 method Methods 0.000 description 7
- 238000007599 discharging Methods 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
- 239000011230 binding agent Substances 0.000 description 5
- 239000000463 material Substances 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 230000032683 aging Effects 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 229910021385 hard carbon Inorganic materials 0.000 description 4
- 229910001228 Li[Ni1/3Co1/3Mn1/3]O2 (NCM 111) Inorganic materials 0.000 description 3
- 239000010405 anode material Substances 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 230000006872 improvement Effects 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 229910002651 NO3 Inorganic materials 0.000 description 2
- 239000013543 active substance Substances 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 description 2
- 238000004364 calculation method Methods 0.000 description 2
- 239000011889 copper foil Substances 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 239000007773 negative electrode material Substances 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910002339 La(NO3)3 Inorganic materials 0.000 description 1
- 229910013553 LiNO Inorganic materials 0.000 description 1
- 229910021314 NaFeO 2 Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical group [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium nitrate Inorganic materials [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000010416 ion conductor Substances 0.000 description 1
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(III) nitrate Inorganic materials [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Inorganic materials [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 238000004886 process control Methods 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 235000010344 sodium nitrate Nutrition 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- BHZCMUVGYXEBMY-UHFFFAOYSA-N trilithium;azanide Chemical compound [Li+].[Li+].[Li+].[NH2-] BHZCMUVGYXEBMY-UHFFFAOYSA-N 0.000 description 1
- ONDPHDOFVYQSGI-UHFFFAOYSA-N zinc nitrate Inorganic materials [Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ONDPHDOFVYQSGI-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- 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
- H01M10/05—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
-
- 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
- H01M10/0568—Liquid materials characterised by the solutes
-
- 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
- H01M10/0569—Liquid materials characterised by the solvents
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
-
- 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
- H01M2300/0088—Composites
- H01M2300/0091—Composites in the form of mixtures
-
- 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 an electrolyte for improving the high-temperature shelving performance of a ternary lithium ion battery, which has higher decomposition resistance temperature, more compact SEI (solid electrolyte interface) film formed on the surface of an electrode, good high-temperature resistance, difficult decomposition and dissolution, and higher Li (lithium ion electrolyte interface) content+The transmission rate. Thereby inhibiting the electrode/electrolyte interface side reaction of the ternary lithium ion battery at high temperature and high pressure, and reducing the reversible/irreversible Li+The consumption of (2) and the stability of the interface are improved. The ternary lithium ion battery has high capacity retention rate during high-temperature storage in improved electrolyteAnd recovery rate.
Description
Technical Field
The invention relates to the field of lithium ion batteries, in particular to electrolyte for a ternary lithium ion battery.
Background
The trend of new energy automobiles replacing traditional fuel automobiles cannot be changed, and lithium ion batteries serving as main motive sources of new energy automobiles are hot spots of global current research. Lithium ion batteries used in electric vehicles are generally expected to have a useful life of over ten years. LiNi1/3Co1/3Mn1/3O2 is used as the lithium ion battery anode material, has a single alpha-NaFeO 2 type layered rock salt structure, is very stable, basically does not change the unit cell parameters after long-term circulation, has a stable lattice structure, and is a very ideal lithium ion battery anode material for charge-discharge circulation under high magnification and high current. The lithium ion battery taking the nickel-cobalt-manganese ternary material as the anode material has good safety performance and rate capability, and is popular in the field of electric vehicles. The battery is often subjected to extreme environments such as low temperature, high humidity and the like in the use process, for example, the temperature in the automobile can reach more than 50 ℃ when the automobile is started or runs and is placed in a burning sun, and the high-temperature environment is a severe test on the performance and the service life of the battery. On the other hand, in the power battery pack, different temperature environments of the single batteries and different self-discharge degrees of the single batteries affect the consistency of battery discharge capacity and battery voltage, and consequently affect the energy exertion and the use process control of the power battery pack in the field of batteries. In order to better exert the advantages of environmental protection, large energy density and the like of the lithium ion battery, the performance degradation of the lithium ion battery in the storage process is reduced, and the service life is prolonged. The influence factors of the battery performance attenuation under the high-temperature condition and the corresponding influence mechanism need to be deeply researched, an improvement scheme is provided, technical support is provided for the wide application of the lithium ion battery, and the gradual improvement of the battery performance is ensured. The decomposition of the electrolyte at high temperature and the side reaction of the electrode/electrolyte interface are key factors influencing the high-temperature storage performance of the battery, and the improvement of the high-temperature shelf performance of the battery by improving the components of the electrolyte is a more effective method.
Disclosure of Invention
The invention aims to provide an electrolyte for improving the high-temperature shelf performance of a ternary lithium ion battery, wherein LiFSI in the electrolyte can reduce the pyrolysis of the electrolyte and optimize an SEI film component; the content of soluble components in the SEI film can be reduced by optimizing the content of the ethylene carbonate, and the compactness of the SEI film is improved; nitrate ions in the electrolyte can form a fast ion conductor Li3N film on the surface of the electrode, so that the electrode/electrolyte interface side reaction under high temperature and high pressure of the battery can be inhibited; the sulfur-containing additive in the electrolyte can form an SEI film which is not easy to decompose at high temperature on the surface of the electrode, so that the stability of the electrode/electrolyte interface is improved. The ternary lithium ion battery has good full-charge high-temperature storage performance in the improved electrolyte.
In order to achieve the purpose, the invention adopts the following specific scheme:
the electrolyte for improving the high-temperature shelving performance of the ternary battery comprises the following components:
1. one or more lithium salts;
the concentration of the lithium salt is 0.8-3 mol/L, preferably 1-2 mol/L.
The lithium salt includes one or more of: LiPF6, LiBF4, LiClO4, LiAsF6, LiBOB, LiODFB, LiFSI, LiTFSI. The mixture of LiPF6 and LiFSI is preferred, and the molar ratio of the LiPF6 and the LiFSI is 4/1-1/4.
2. One or more ester solvents:
the solvent comprises one or more of the following: ethylene carbonate, propylene carbonate, diethyl carbonate, ethyl methyl carbonate, dimethyl carbonate, methyl acetate, ethyl acetate, n-butyl acetate, isobutyl acetate. Of these, a mixture of ethylene carbonate and diethyl carbonate is preferred. Ethylene carbonate: the volume ratio of diethyl carbonate is 1/3-4/1, wherein 1/1 is preferred.
3. One or more NO-containing compounds3 -Additive:
the mass fraction of the additive is 0.1-5%, preferably 0.2-1%.
The additives includeOne or more of: LiNO3,Cu(NO3)2，NaNO3，Mg(NO3)2， Ca(NO3)2，Fe(NO3)3，Zn(NO3)2，AgNO3，KNO3，NH4NO3,Ce(NO3)3,La(NO3)3ZrO (NO3)2, nitrocellulose ((C6H7N3O11) N), bis (4-nitrophenyl) carbonate.
4. One or more S-containing additives:
the mass fraction of the additive is 0.2-5%, preferably 0.5-2%.
The S-containing additive comprises one or more of: 1, 3-Propane Sultone (PS), propenyl-1, 3-sultone (PST), 1, 4-Butane Sultone (BS), methylene cyclamate, propylene sulfite, vinyl sulfate, dimethyl sulfite, diethyl sulfite, 4-methyl ethylene sulfate (PCS), 4-propyl ethylene sulfate, propylene sulfate. Among them, preferred is propenyl-1, 3-sultone (PST).
5. The electrolyte is also added with a third additive: one or more of vinylene carbonate, ethylene carbonate, lithium difluorophosphate and tripropynyl phosphate, and the concentration of the additive is preferably 0.1 to 5%, and preferably 1 to 3%.
The electrolyte is applied to the ternary lithium ion battery, the charged placing temperature is 50-80 ℃, and the charged placing temperature is preferably 55-65 ℃.
The invention has the beneficial effects that:
the electrolyte has higher decomposition temperature resistance, a compact SEI film formed on the surface of an electrode, good high-temperature resistance, difficult decomposition and dissolution and higher Li & lt + & gt transmission rate. Therefore, the side reaction of the electrode/electrolyte interface of the ternary lithium ion battery at high temperature and high pressure can be inhibited, the consumption of reversible/irreversible Li < + > is reduced, and the interface stability is improved. The ternary lithium ion battery has good high-temperature storage performance and rate capability in the improved electrolyte.
Drawings
Table 1: examples 1-2 and comparative examples 1-6 are the discharge capacity and capacity retention and recovery of the ternary lithium ion battery before and after it was left to stand at high temperature of 55 ℃.
Detailed Description
Example 1
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6 to LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.0 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate, nitrocellulose and propenyl-1, 3-sultone respectively, and the mass fractions of the additives are respectively 2%, 0.5% and 1% of the total mass of the lithium salt and the ester solvent; obtaining the electrolyte.
The anode of the ternary lithium ion battery is prepared as follows: LiNi1/3Co1/3Mn1/3O2The mass ratio of the conductive carbon black to the PVDF (polyvinylidene fluoride) is 94: 4: 2 dissolving in N-methyl pyrrolidone, mixing, coating on both sides of aluminum foil, and coating with positive active substance content of 5mg/cm2And cutting the dried material into rectangular electrode plates with the length of 200mm and the width of 146mm for later use by a slicing machine. The negative electrode of the cell was prepared as follows: the mass ratio of the graphite, the hard carbon, the conductive carbon black and the binder is 60:30:8:2, the graphite, the hard carbon, the conductive carbon black and the binder are dissolved in a proper amount of water, the mixture is uniformly mixed and coated on the two sides of the copper foil, and the loading of the negative active material is 2.8mg/cm2And cutting the dried material into rectangular electrode slices with the length of 200mm and the width of 146mm by a slicing machine for later use. SC12 is used as a diaphragm, a plurality of soft package batteries are assembled in a drying room, 25g of electrolyte is added, and then the assembled batteries are subjected to high-temperature formation, high-temperature aging, normal-temperature aging, secondary capacity grading and other testing steps, so that a complete SEI film is formed on the surface of an electrode.
The method for testing the high-temperature shelving performance of the battery comprises the following steps:
under the environment temperature of 1.25 +/-2 ℃, charging to 4.2V at a constant current and a constant voltage of 1C, and stopping current at 0.05C;
standing for 1h at the ambient temperature of 2.25 +/-2 ℃;
discharging at 1C constant current to 2.8V (recording discharge capacity C1) at the ambient temperature of 3.25 +/-2 ℃;
standing for 1h at the ambient temperature of 4.25 +/-2 ℃;
under the environment temperature of 5.25 +/-2 ℃, charging to 4.2V at a constant current and a constant voltage of 1C, and stopping current at 0.05C;
standing for 7d at the ambient temperature of 6.55 +/-2 ℃;
standing for 24h at the ambient temperature of 7.25 +/-2 ℃;
discharging at 1C constant current to 2.8V (recording discharge capacity C2) at the ambient temperature of 8.25 +/-2 ℃;
standing for 1h at the ambient temperature of 9.25 +/-2 ℃;
under the environment temperature of 10.25 +/-2 ℃, charging to 4.2V at a constant current and a constant voltage of 1C, and stopping current at 0.05C;
standing for 1h at the ambient temperature of 11.25 +/-2 ℃;
discharging at constant current of 1C to 2.8V (recording discharge capacity C3) at ambient temperature of 12.25 +/-2 ℃;
the remaining capacity calculating method comprises the following steps: (C2/C1) × 100%; the recovery capacity calculation method comprises the following steps: (C3/C1) 100%.
The test results are shown in table 1.
Example 2
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6 to LiFSI is 1:3, and the concentration of lithium salt in the electrolyte is 1.5 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are respectively lithium difluorophosphate, nitrocellulose and propenyl-1, 3-sultone, and the mass fractions of the additives are respectively 2%, 0.5% and 1% of the total mass of the lithium salt and the ester solvent; obtaining the electrolyte.
The test method was the same as in example 1;
the test results are shown in table 1.
Example 3
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6 to LiFSI is 4:1, and the concentration of lithium salt in the electrolyte is 2 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate and LiNO respectively31, 3-propane sultone, the mass fractions of which are respectively 1%, 0.2% and 2% of the total mass of the lithium salt and the ester solvent; obtaining the electrolyte.
The test method was the same as in example 1;
the test results are shown in table 1.
Example 4
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6 to LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.0 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate, lithium difluorophosphate, copper nitrate and methylene cyclamate, and the mass fractions of the additives are 1 percent, 1 percent and 1 percent of the total mass of the lithium salt and the ester solvent respectively; obtaining the electrolyte.
The test method was the same as in example 1;
the test results are shown in table 1.
Example 5
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6 to LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.0 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are tripropynyl phosphate and La (NO)3)3Dimethyl sulfite, which accounts for 1 percent, 0.5 percent and 2 percent of the total mass of the lithium salt and the ester solvent respectively; obtaining the electrolyte.
The test method was the same as in example 1;
the test results are shown in table 1.
Example 6
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar concentration ratio is 1:1, and the concentration of lithium salt in the electrolyte is 1.2 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are ethylene carbonate, lithium difluorophosphate, KNO3, 1, 4-butane sultone respectively, and the mass fractions are respectively 1%, 1%, 1% and 2% of the total mass of the lithium salt and the ester solvent;
the test method was the same as in example 1;
the test results are shown in table 1.
Comparative example 1
High temperature electrolytes are available from the Guangzhou Tiancio under the model TC-EFF 05;
the anode of the ternary lithium ion battery is prepared as follows: the mass ratio of LiNi1/3Co1/3Mn1/3O2 to the conductive carbon black to the binder is 94: 4: 2 dissolving in N-methyl pyrrolidone, mixing, and coating on both sides of aluminum foil, wherein the content of positive active substance is 5mg/cm2And cutting the dried material into rectangular electrode plates with the length of 200mm and the width of 146mm for later use by a slicing machine. The negative electrode of the cell was prepared as follows: the mass ratio of the graphite, the hard carbon, the conductive carbon black and the binder is 60:30:8:2, the graphite, the hard carbon, the conductive carbon black and the binder are dissolved in a proper amount of water, the mixture is uniformly mixed and coated on the two sides of the copper foil, and the loading of the negative active material is 2.8mg/cm2And cutting the dried material into rectangular electrode plates with the length of 200mm and the width of 146mm for later use by a slicing machine. And (2) assembling a plurality of soft package batteries in a drying room by taking Celgard 2500 as a diaphragm, adding 25g of electrolyte, and then carrying out high-temperature formation, high-temperature aging, normal-temperature aging, secondary capacity grading and other testing steps on the assembled batteries so as to form a complete SEI film on the surface of an electrode.
The method for testing the high-temperature shelving performance of the battery comprises the following steps:
under the environment temperature of 1.25 +/-2 ℃, charging to 4.2V at a constant current and a constant voltage of 1C, and stopping current at 0.05C;
standing for 1h at the ambient temperature of 2.25 +/-2 ℃;
discharging at 1C constant current to 2.8V (recording discharge capacity C1) at the ambient temperature of 3.25 +/-2 ℃;
standing for 1h at the ambient temperature of 4.25 +/-2 ℃;
under the environment temperature of 5.25 +/-2 ℃, charging to 4.2V at a constant current and a constant voltage of 1C, and stopping current at 0.05C;
standing for 7d at the ambient temperature of 6.55 +/-2 ℃;
standing for 24h at the ambient temperature of 7.25 +/-2 ℃;
discharging at 1C constant current to 2.8V (recording discharge capacity C2) at the ambient temperature of 8.25 +/-2 ℃;
standing for 1h at the ambient temperature of 9.25 +/-2 ℃;
under the environment temperature of 10.25 +/-2 ℃, charging to 4.2V at a constant current and a constant voltage of 1C, and stopping current at 0.05C;
standing for 1h at the ambient temperature of 11.25 +/-2 ℃;
discharging at constant current of 1C to 2.8V (recording discharge capacity C3) at ambient temperature of 12.25 +/-2 ℃;
the remaining capacity calculating method comprises the following steps: (C2/C1) × 100%; the recovery capacity calculation method comprises the following steps: (C3/C1) 100%.
The test results are shown in table 1.
Comparative example 2
The electrolyte lithium salt is LiPF6, and the concentration of the lithium salt in the electrolyte is 1.0 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate, nitrocotton and propenyl-1, 3-sultone respectively, and the mass fractions of the additives are respectively 2%, 0.5% and 1% of the total mass of the lithium salt and the ester solvent; obtaining the electrolyte.
The test method is the same as that of comparative example 1;
the test results are shown in table 1.
Comparative example 3
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6 to LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.0 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate and propenyl-1, 3-sultone respectively, and the mass fractions of the additives are respectively 2% and 1% of the total mass of the lithium salt and the ester solvent; thus obtaining the electrolyte.
The test method is the same as that of comparative example 1;
the test results are shown in table 1.
Comparative example 4
The electrolyte lithium salt is a mixture of LiPF6/LiFSI (lithium hexafluorophosphate/lithium bis (fluorosulfonyl) imide), the molar ratio of LiPF6/LiFSI is 1:3, and the concentration of lithium salt in the electrolyte is 1.2 mol/L; the solvent is the mixture of ethylene carbonate and ethyl methyl carbonate, and the volume ratio is 1: 1; the additives are nitrocotton and propenyl-1, 3-sultone respectively, and the mass fractions of the additives are 0.5 percent and 1 percent of the total mass of the lithium salt and the ester solvent respectively; obtaining the electrolyte.
The test method is the same as that of comparative example 1;
the test results are shown in table 1.
Comparative example 5
The electrolyte lithium salt is a mixture of LiPF6/LiFSI, the molar ratio of LiPF6/LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.5 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate and nitrocotton respectively, and the mass fractions of the vinylene carbonate and the nitrocotton are respectively 2% and 1% of the total mass of the lithium salt and the ester solvent; obtaining the electrolyte.
The test method is the same as that of comparative example 1;
the test results are shown in table 1.
Comparative example 6
The electrolyte lithium salt is a mixture of LiPF6/LiFSI, the molar ratio of LiPF6/LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.2 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additives are vinylene carbonate, lithium nitrate and 1, 4-butane sultone respectively, and the mass fractions of the additives are 0.5 percent, 0.1 percent and 0.2 percent of the total mass of the lithium salt and the ester solvent respectively; obtaining the electrolyte.
The test method is the same as that of comparative example 1;
the test results are shown in table 1.
Comparative example 7
The electrolyte lithium salt is a mixture of LiPF6/LiFSI, the molar ratio of LiPF6/LiFSI is 1:1, and the concentration of lithium salt in the electrolyte is 1.2 mol/L; the solvent is the mixture of ethylene carbonate and diethyl carbonate, and the volume ratio is 1: 1; the additive is vinylene carbonate, and the mass fraction of the vinylene carbonate is 1 percent of the total mass of the lithium salt and the ester solvent; obtaining the electrolyte.
The test method is the same as that of comparative example 1;
the test results are shown in table 1.
TABLE 1
In conclusion, the invention discloses an electrolyte for improving the high-temperature shelf performance of a ternary lithium ion battery, which simultaneously contains PF6-FSI-S-containing and NO-containing 3-The additive forms a compact SEI film on the surface of the electrode, and the SEI film has good high-temperature resistance, is not easy to decompose and dissolve and has higher Li + transmission rate. Therefore, the side reaction of the electrode/electrolyte interface of the ternary lithium ion battery at high temperature and high pressure can be inhibited, the consumption of reversible/irreversible Li < + > is reduced, and the interface stability is improved. The ternary lithium ion battery has high capacity retention rate and recovery rate when stored in the improved electrolyte at high temperature.
Claims (6)
1. An electrolyte capable of improving the high-temperature shelving performance of a ternary lithium ion battery comprises the following components:
(1) one or more lithium salts; the concentration of the lithium salt is 0.8-3 mol/L, preferably 1.0-2 mol/L;
(2) one or more ester solvents;
(3) one or more kinds containing NO3-Additive: said NO is contained3-The mass of the additive is 0.1-5% of the total mass of the lithium salt and the ester solvent, preferably 0.2-1%;
(4) one or more S-containing additives: the mass of the additive is 0.2-5% of the total mass of the lithium salt and the ester solvent, and preferably 0.5-2%;
the S-containing additive comprises one or more of: 1, 3-Propane Sultone (PS), propenyl-1, 3-sultone (PST), 1, 4-Butane Sultone (BS), methylene cyclamate, propylene sulfite, vinyl sulfate, dimethyl sulfite, diethyl sulfite, 4-methyl ethylene sulfate (PCS), 4-propyl ethylene sulfate, propylene sulfate;
(5) the electrolyte is also added with a third additive; the third additive is: one or more than two of vinylene carbonate, ethylene carbonate, lithium difluorophosphate and tripropynyl phosphate, and the mass of the third additive is 0.1-5% of the total mass of lithium salt and ester solvent, preferably 1-3%.
2. The electrolyte of claim 1, wherein:
the lithium salt includes one or more of: LiPF6, LiBF4, LiClO4, LiAsF6, LiBOB, LiODFB, liffsi, LiTFSI;
the lithium salt is preferably a mixture of LiPF6 and LiFSI, and the molar ratio of the LiPF6 and the LiFSI is 4/1-1/4.
3. The electrolyte of claim 1, wherein:
ester solvent: preferred is a mixture of ethylene carbonate and diethyl carbonate; ethylene carbonate: the volume ratio of diethyl carbonate is 1/3-4/1, wherein 1/1 is preferred;
the solvent comprises one or more of the following: ethylene carbonate, propylene carbonate, diethyl carbonate, ethyl methyl carbonate, dimethyl carbonate, methyl acetate, ethyl acetate, n-butyl acetate, isobutyl acetate.
4. The electrolyte of claim 1, wherein:
the NO 3-containing additive comprises one or more of the following: LiNO3,Cu(NO3)2NaNO3, Mg (NO3)2, Ca (NO3)2, Fe (NO3)3, Zn (NO3)2, AgNO3, KNO3, NH4NO3, Ce (NO3)3, La (NO3)3, ZrO (NO3)2, nitrocellulose ((C6H7N3O11) N), bis (4-nitrophenyl) carbonate.
5. Use of the electrolyte of any of claims 1-4 in a ternary lithium ion battery.
6. Use of an electrolyte according to claim 5, characterized in that: the charged standing temperature is 50-80 ℃, and the preferred charged standing temperature is 55-65 ℃.
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