CN114171791A - Electrolyte and lithium ion battery - Google Patents
Electrolyte and lithium ion battery Download PDFInfo
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- CN114171791A CN114171791A CN202010945128.0A CN202010945128A CN114171791A CN 114171791 A CN114171791 A CN 114171791A CN 202010945128 A CN202010945128 A CN 202010945128A CN 114171791 A CN114171791 A CN 114171791A
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 120
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 19
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 19
- ROORDVPLFPIABK-UHFFFAOYSA-N diphenyl carbonate Chemical compound C=1C=CC=CC=1OC(=O)OC1=CC=CC=C1 ROORDVPLFPIABK-UHFFFAOYSA-N 0.000 claims abstract description 27
- FALRKNHUBBKYCC-UHFFFAOYSA-N 2-(chloromethyl)pyridine-3-carbonitrile Chemical compound ClCC1=NC=CC=C1C#N FALRKNHUBBKYCC-UHFFFAOYSA-N 0.000 claims abstract description 25
- 239000000654 additive Substances 0.000 claims abstract description 25
- 229940014800 succinic anhydride Drugs 0.000 claims abstract description 25
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 24
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 24
- 239000003960 organic solvent Substances 0.000 claims abstract description 24
- 230000000996 additive effect Effects 0.000 claims abstract description 13
- CBTAIOOTRCAMBD-UHFFFAOYSA-N 2-ethoxy-2,4,4,6,6-pentafluoro-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound CCOP1(F)=NP(F)(F)=NP(F)(F)=N1 CBTAIOOTRCAMBD-UHFFFAOYSA-N 0.000 claims abstract description 11
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims abstract description 11
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 19
- 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 18
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 6
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 6
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 5
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 4
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 4
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 claims description 4
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 4
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 claims description 4
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 4
- IIPYXGDZVMZOAP-UHFFFAOYSA-N lithium nitrate Chemical compound [Li+].[O-][N+]([O-])=O IIPYXGDZVMZOAP-UHFFFAOYSA-N 0.000 claims description 4
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical compound COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 claims description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 4
- HHVIBTZHLRERCL-UHFFFAOYSA-N sulfonyldimethane Chemical compound CS(C)(=O)=O HHVIBTZHLRERCL-UHFFFAOYSA-N 0.000 claims description 4
- 239000008151 electrolyte solution Substances 0.000 claims description 3
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 claims description 2
- HNAGHMKIPMKKBB-UHFFFAOYSA-N 1-benzylpyrrolidine-3-carboxamide Chemical compound C1C(C(=O)N)CCN1CC1=CC=CC=C1 HNAGHMKIPMKKBB-UHFFFAOYSA-N 0.000 claims description 2
- 101100537779 Homo sapiens TPM2 gene Proteins 0.000 claims description 2
- JGFBQFKZKSSODQ-UHFFFAOYSA-N Isothiocyanatocyclopropane Chemical compound S=C=NC1CC1 JGFBQFKZKSSODQ-UHFFFAOYSA-N 0.000 claims description 2
- 229910010941 LiFSI Inorganic materials 0.000 claims description 2
- 229910001290 LiPF6 Inorganic materials 0.000 claims description 2
- 229910012265 LiPO2F2 Inorganic materials 0.000 claims description 2
- 102100036471 Tropomyosin beta chain Human genes 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
- OBNCKNCVKJNDBV-UHFFFAOYSA-N butanoic acid ethyl ester Natural products CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 claims description 2
- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 claims description 2
- 150000007942 carboxylates Chemical class 0.000 claims description 2
- NKDDWNXOKDWJAK-UHFFFAOYSA-N dimethoxymethane Chemical compound COCOC NKDDWNXOKDWJAK-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
- WBJINCZRORDGAQ-UHFFFAOYSA-N formic acid ethyl ester Natural products CCOC=O WBJINCZRORDGAQ-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
- 229910001537 lithium tetrachloroaluminate Inorganic materials 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- 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 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
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 2
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 claims description 2
- 229940090181 propyl acetate Drugs 0.000 claims description 2
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 claims description 2
- 150000003457 sulfones Chemical class 0.000 claims description 2
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 claims description 2
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 claims description 2
- NONFLFDSOSZQHR-UHFFFAOYSA-N 3-(trimethylsilyl)propionic acid Chemical compound C[Si](C)(C)CCC(O)=O NONFLFDSOSZQHR-UHFFFAOYSA-N 0.000 claims 1
- 229910010943 LiFOP Inorganic materials 0.000 claims 1
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 abstract description 6
- 239000003063 flame retardant Substances 0.000 abstract description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 34
- 229910013872 LiPF Inorganic materials 0.000 description 17
- 101150058243 Lipf gene Proteins 0.000 description 17
- 229910052786 argon Inorganic materials 0.000 description 17
- 239000011259 mixed solution Substances 0.000 description 17
- 230000000052 comparative effect Effects 0.000 description 13
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- 239000010405 anode material Substances 0.000 description 5
- 239000013538 functional additive Substances 0.000 description 5
- 239000000463 material Substances 0.000 description 5
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 4
- 238000003917 TEM image Methods 0.000 description 4
- -1 lithium hexafluorophosphate Chemical compound 0.000 description 4
- 239000010406 cathode material Substances 0.000 description 3
- 239000007774 positive electrode material Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- QJMMCGKXBZVAEI-UHFFFAOYSA-N tris(trimethylsilyl) phosphate Chemical compound C[Si](C)(C)OP(=O)(O[Si](C)(C)C)O[Si](C)(C)C QJMMCGKXBZVAEI-UHFFFAOYSA-N 0.000 description 3
- 229910012258 LiPO Inorganic materials 0.000 description 2
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
- 238000003421 catalytic decomposition reaction Methods 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 229910052744 lithium Inorganic materials 0.000 description 2
- 230000014759 maintenance of location Effects 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- 229920001774 Perfluoroether Polymers 0.000 description 1
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000003660 carbonate based solvent Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 150000002170 ethers Chemical class 0.000 description 1
- 125000004494 ethyl ester group Chemical group 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 125000002560 nitrile group Chemical group 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- MRDKYAYDMCRFIT-UHFFFAOYSA-N oxalic acid;phosphoric acid Chemical compound OP(O)(O)=O.OC(=O)C(O)=O MRDKYAYDMCRFIT-UHFFFAOYSA-N 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 238000004627 transmission electron microscopy Methods 0.000 description 1
Images
Classifications
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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
- H01M10/05—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
- H01M10/42—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
- H01M2200/00—Safety devices for primary or secondary batteries
-
- 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
-
- 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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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
Abstract
The application discloses an electrolyte and a battery suitable for an NCM system. The electrolyte comprises an organic solvent, electrolyte lithium salt and an additive, wherein the additive comprises vinyl sulfate accounting for 0.1-10% of the total mass of the electrolyte, succinic anhydride accounting for 0.1-5% of the total mass of the electrolyte, ethoxy (pentafluoro) cyclotriphosphazene accounting for 0.1-15% of the total mass of the electrolyte and diphenyl carbonate accounting for 0.01-5% of the total mass of the electrolyte. The electrolyte and the battery provided by the invention not only have excellent electrochemical properties at normal temperature and high temperature, but also have obviously improved overcharge and flame retardant properties; therefore, the lithium ion battery has wide application prospect in the future batteries of high-energy density systems.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to an electrolyte and a lithium ion secondary battery.
Background
The lithium ion battery anode material such as the NCM ternary material has the advantages of high specific capacity, good cycle performance, good safety, small environmental pollution and the like, is gradually paid attention to by people, and is expected to become one of the mainstream anode materials of the lithium ion battery in the future. To meet the demand for high energy density, NCM ternary cathode materials are also evolving in two directions: 1) the nickel content is high, and higher Ni content can bring higher capacity; 2) the high voltage, the improvement of voltage can promote the capacity of material on the one hand, on the other hand also can promote the voltage platform of material. However, the stability of the positive electrode material/electrolyte interface is reduced with the increase of the charging voltage, so that the side reaction is increased, and the cycle performance of the lithium ion battery is seriously influenced.
The performance of high nickel and high voltage lithium ion batteries is primarily determined by the structure and properties of the active materials and electrolyte. Among them, the matching of the electrolyte is very important. With the continuous emergence and application of high-voltage cathode materials in recent years, a conventional carbonate and lithium hexafluorophosphate system can be decomposed in a high-voltage system battery, so that the battery performances such as cycle performance, high-temperature performance and the like are reduced; a small amount of functional additive is added into the carbonate-based electrolyte to ensure that the functional additive is subjected to oxidation/reduction decomposition reaction in preference to solvent molecules, and an effective protective film is formed on the surface of an electrode, so that the subsequent decomposition of the carbonate-based solvent can be inhibited. The film formed by the additive with excellent performance can even inhibit the dissolution of metal ions of the anode material and the deposition on the cathode, thereby obviously improving the interface stability of the electrode/electrolyte and the cycle performance of the battery.
US patent US 2008/0311481Al (Samsung SDI co., Ltd) discloses ether/aryl compounds containing two nitrile groups, which improve the ballooning of the battery under high voltage and high temperature conditions, improve high temperature storage performance, and the battery performance thereof is to be further improved.
Chinese patent CN104659417B discloses that the high voltage electrolyte contains fluoro carbonate compound and fluoro ether compound, lithium oxalyldifluoroborate and lithium hexafluorophosphate; although the system can play a certain role at high voltage, FEC is easily decomposed to produce VC and hydrofluoric acid under high temperature, and the hydrofluoric acid corrodes an SEI film formed on the surface of an electrode, so that the electrical performance of the battery is deteriorated.
In view of the above, it is desirable to provide a functional electrolyte solution to solve the above problems, so that the high specific energy system battery can be popularized and applied.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: an electrolyte solution suitable for a high-voltage, high-specific energy system lithium ion secondary battery is provided.
In order to solve the technical problems, the invention adopts the following technical scheme:
the invention provides an electrolyte, which comprises an organic solvent, electrolyte lithium salt and an additive; wherein the additive comprises vinyl sulfate (DTD) accounting for 0.1-10% of the total mass of the electrolyte, Succinic Anhydride (SA) accounting for 0.1-5% of the total mass of the electrolyte, ethoxy (pentafluoro) cyclotriphosphazene (FPN) accounting for 0.1-15% of the total mass of the electrolyte, and diphenyl carbonate (DPC) accounting for 0.01-5% of the total mass of the electrolyte.
Preferably, the vinyl sulfate accounts for 0.5-3% of the total mass of the electrolyte; the succinic anhydride accounts for 0.5-2% of the total mass of the electrolyte; the ethoxy (pentafluoro) cyclotriphosphazene accounts for 5-15% of the total mass of the electrolyte; the diphenyl carbonate accounts for 0.1-3% of the total mass of the electrolyte.
Further preferably, the additive is composed of vinyl sulfate, succinic anhydride, ethoxy (pentafluoro) cyclotriphosphazene and diphenyl carbonate, and the vinyl sulfate accounts for 0.5-1.5% of the total mass of the electrolyte; the succinic anhydride accounts for 0.5-2% of the total mass of the electrolyte; the ethoxy (pentafluoro) cyclotriphosphazene accounts for 5-15% of the total mass of the electrolyte; the diphenyl carbonate accounts for 0.3-3% of the total mass of the electrolyte.
Preferably, the additive also comprises other additives, and the other additives are vinylene carbonate and LiPO2F2One or more of LiFOP, TMSP and TMSB.
More preferably, the other additives account for 0.1-5% of the total mass of the electrolyte.
More preferably, the other additives account for 0.5-3% of the total mass of the electrolyte.
Preferably, the organic solvent is one or more of carbonate, carboxylate, ether and sulfone.
Further preferably, the organic solvent is one or more of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propylene carbonate, methyl formate, ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate, ethyl butyrate, dimethoxymethane, 1, 2-dimethoxyethane, tetrahydrofuran, 1, 3-dioxolane, dimethyl sulfoxide, sulfolane and dimethyl sulfone.
Preferably, the electrolyte lithium salt is LiPF6、LiBF4、LiClO4、LiCH3SO3、LiSCN、LiNO3、LiO3SCF2CF3、LiAsF6、LiAlCl4One or more of LiTFSI, LiFSI; the concentration of the electrolyte lithium salt is 0.7-3 mol/L.
The invention also provides a lithium ion battery which comprises the electrolyte in any one of the above-mentioned aspects.
Preferably, the lithium ion battery further comprises a positive electrode material, the positive electrode material is an NCM material, and the voltage of the lithium ion battery is more than or equal to 4.4V.
According to the invention, four additives of different types are used in combination in the electrolyte to generate a synergistic effect, so that the catalytic decomposition of the conventional carbonate solvent in a high-voltage state is inhibited, and the gas generation of the battery and the dissolution of metal ions are inhibited; through the optimized combination of the additives, the high-temperature, low-temperature and normal-temperature performances of the high-voltage lithium ion battery are considered; and the addition of the ethoxy (pentafluoro) cyclotriphosphazene and the diphenyl carbonate greatly improves the flame retardant and overcharge performances of the battery.
Due to the application of the technical scheme, compared with the prior art, the invention has the following advantages:
the electrolyte provided by the invention ensures that the high-voltage NCM system lithium ion battery not only has stable cycle performance at normal temperature, but also can inhibit the lithium ion battery from ballooning, cycle attenuation and thickness increase under the high-temperature condition; and can promote simultaneously overcharge and fire behaviour, and then improve the security that the battery used.
The electrolyte and the battery provided by the invention not only have excellent electrochemical properties at normal temperature and high temperature, but also have obviously improved overcharge and flame retardant properties; therefore, the lithium ion battery has wide application prospect in the future batteries of high-energy density systems.
Drawings
Fig. 1 is a 25 c normal temperature cycle performance curve of the batteries of the respective examples and comparative examples.
Fig. 2 is a 45 c high temperature cycle performance curve of the batteries of the respective examples and comparative examples.
FIG. 3 is a TEM image of a disassembled positive electrode plate of a cell of comparative example 1 after formation and capacity grading.
FIG. 4 is a TEM image of the disassembled positive pole piece after the battery of example 5 is subjected to chemical composition and grading.
FIG. 5 is a TEM image of a disassembled positive electrode plate of the battery of example 12 after chemical composition and grading.
Detailed Description
The invention is further described with reference to the following figures and examples. However, the present invention is not limited to the following examples. The implementation conditions adopted in the embodiments can be further adjusted according to different requirements of specific use, and the implementation conditions not mentioned are conventional conditions in the industry. The technical features of the embodiments of the present invention may be combined with each other as long as they do not conflict with each other.
Comparative examples and examples, the additives involved are as follows: vinyl sulfate (DTD), Succinic Anhydride (SA), ethoxy (pentafluoro) cyclotriphosphazene (FPN), diphenyl carbonate (DPC), lithium tetrafluoro oxalate phosphate (LiFOP), tris (trimethylsilyl) phosphate (TMSP), lithium difluorophosphate (LiPO)2F2) And Vinylene Carbonate (VC).
Comparative example 1
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6And (4) preparing the electrolyte without adding other functional additives.
Comparative example 2
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1 wt% of DTD was added to the electrolyte to prepare an electrolyte.
Comparative example 3
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1 wt% of SA was added to the electrolyte to prepare an electrolyte.
Comparative example 4
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 3 wt% of FPN was added to the electrolyte to prepare an electrolyte.
Comparative example 5
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 0.5 wt% of DPC was added to the electrolyte to prepare an electrolyte.
Example 1
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 0.1 wt% of DTD, 0.1 wt% of SA, 1 wt% of FPN and 1 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 2
In an argon-filled glove box (H)2Content of O<10ppm), the organic solvent carbonic acid is addedThe ethyl ester, the ethylene carbonate and the methyl ethyl carbonate are uniformly mixed according to the mass ratio of 2:3:5, and 1.1mol/L electrolyte lithium salt LiPF is added into the mixed solution6Then, 0.5 wt% of DTD, 0.1 wt% of SA, 0.5 wt% of FPN and 0.5 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 3
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 0.1 wt% of DTD, 0.5 wt% of SA, 10 wt% of FPN and 0.1 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 4
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 0.5 wt% of DTD, 0.5 wt% of SA, 3 wt% of FPN and 0.5 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 5
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1 wt% of DTD, 1 wt% of SA, 5 wt% of FPN and 0.5 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 6
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 0.5 wt% of DTD, 0.5 wt% of SA, 15 wt% of FPN and 0.3 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 7
Under the condition of argon fillingIn the glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.15mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1 wt% of DTD, 2 wt% of SA, 10 wt% of FPN and 3 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 8
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1.5 wt% of DTD, 2 wt% of SA, 10 wt% of FPN and 0.5 wt% of DPC were added to the electrolyte to prepare an electrolyte.
Example 9
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1.5 wt% of DTD, 2 wt% of SA, 10 wt% of FPN, 0.5 wt% of DPC and 0.5 wt% of LiFOP were added to the electrolyte to prepare an electrolyte.
Example 10
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1.5 wt% of DTD, 1 wt% of SA, 5 wt% of FPN, 0.5 wt% of DPC and 1 wt% of LiFOP were added to the electrolyte to prepare an electrolyte.
Example 11
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1.5 wt% of DTD, 1 wt% of SA, 5 wt% of FPN, 0.5 wt% of DPC, and,1 wt% of LiFOP and 1 wt% of TMSP to prepare an electrolyte.
Example 12
In an argon-filled glove box (H)2Content of O<10ppm), uniformly mixing organic solvents of diethyl carbonate, ethylene carbonate and methyl ethyl carbonate in a mass ratio of 2:3:5, and adding 1.1mol/L electrolyte lithium salt LiPF into the mixed solution6Then, 1.5 wt% of DTD, 1 wt% of SA, 5 wt% of FPN, 0.5 wt% of DPC, 1 wt% of LiPO were added to the electrolyte2F2TMSP of 0.5 wt% and VC of 0.5 wt% to prepare an electrolyte.
The electrolyte prepared in the above comparative example and example was injected into a battery and tested, wherein the battery in the comparative example and example was a 2500mAh pouch battery using a 4.4V NCM622 (high voltage nickel cobalt manganese ternary battery)/artificial graphite system. The normal-temperature cycle performance and the high-temperature cycle performance at 45 ℃ are tested by adopting a Shenzhen Xinwei battery tester; transmission Electron Microscopy (TEM) images were tested on a JEOL JEM2010(200kV) TEM instrument, with a scale of 100nm, 200 nm.
The 1C cycle performance of the cell was tested at 25 deg.C normal temperature and 45 deg.C high temperature over a voltage range of 2.75-4.4V. Table 1 shows data of the normal temperature cycle capacity retention rate, the 45 ℃ high temperature cycle capacity retention rate, and the expansion rate before and after the 45 ℃ high temperature cycle of the batteries prepared by the electrolytes of all comparative examples and examples, and the cycle number is 1000 weeks.
TABLE 1
The batteries obtained from the electrolytes of the comparative examples and the examples were subjected to overcharge and flame retardant effect tests, and the results are shown in table 2.
TABLE 2
As can be seen from the data in tables 1 and 2, and fig. 1 and 2, the electrolyte in the embodiment produces a synergistic effect with the addition of 4 different functional additives and the selective addition of other functional additives, and improves the normal temperature cycle performance, the high temperature cycle performance, the thickness expansion in the high temperature cycle, and the like of the 4.4V high voltage ternary NCM622 battery. By combining the analysis of the attached figures 3, 4 and 5, a layer of stable solid electrolyte interface film is formed on the surfaces of the anode and cathode materials of the battery due to the combination optimization of the additives, so that the direct contact between the materials and the electrolyte is prevented, the catalytic decomposition of the anode materials to the electrolyte solvent under the conditions of high voltage and high temperature is avoided, and the normal temperature and high temperature performance of the battery is further improved. The overcharge and flame retardant properties of the high-voltage NCM622 battery are greatly improved by adding the overcharge additive DPC and the flame retardant additive FPN.
According to the test results, the electrochemical performance of the 4.4V NCM622 lithium ion battery can be greatly improved by the electrolyte formula, and particularly, the formula in the example 12 is particularly excellent in various performance performances.
The present invention has been described in detail in order to enable those skilled in the art to understand the invention and to practice it, and it is not intended to limit the scope of the invention, and all equivalent changes and modifications made according to the spirit of the present invention should be covered by the present invention.
Claims (10)
1. An electrolytic solution comprising an organic solvent, an electrolytic lithium salt and an additive, characterized in that: the additive comprises vinyl sulfate accounting for 0.1-10% of the total mass of the electrolyte, succinic anhydride accounting for 0.1-5% of the total mass of the electrolyte, ethoxy (pentafluoro) cyclotriphosphazene accounting for 0.1-15% of the total mass of the electrolyte and diphenyl carbonate accounting for 0.01-5% of the total mass of the electrolyte.
2. The electrolyte of claim 1, wherein: the vinyl sulfate accounts for 0.5-3% of the total mass of the electrolyte; the succinic anhydride accounts for 0.5-2% of the total mass of the electrolyte; the ethoxy (pentafluoro) cyclotriphosphazene accounts for 5-15% of the total mass of the electrolyte; the diphenyl carbonate accounts for 0.1-3% of the total mass of the electrolyte.
3. The electrolyte of claim 2, wherein: the additive consists of vinyl sulfate, succinic anhydride, ethoxy (pentafluoro) cyclotriphosphazene and diphenyl carbonate, and the vinyl sulfate accounts for 0.5-1.5% of the total mass of the electrolyte; the succinic anhydride accounts for 0.5-2% of the total mass of the electrolyte; the ethoxy (pentafluoro) cyclotriphosphazene accounts for 5-15% of the total mass of the electrolyte; the diphenyl carbonate accounts for 0.3-3% of the total mass of the electrolyte.
4. The electrolyte of claim 1 or 2, wherein: the additive also comprises other additives, and the other additives are vinylene carbonate and LiPO2F2One or more of LiFOP, TMSP and TMSB.
5. The electrolyte of claim 4, wherein: the other additives account for 0.1-5% of the total mass of the electrolyte.
6. The electrolyte of claim 5, wherein: the other additives account for 0.5-3% of the total mass of the electrolyte.
7. The electrolyte of claim 1, wherein: the organic solvent is one or more of carbonate, carboxylate, ether and sulfone.
8. The electrolyte of claim 7, wherein: the organic solvent is one or more of ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, propylene carbonate, methyl formate, ethyl formate, methyl acetate, ethyl acetate, propyl acetate, ethyl propionate, methyl butyrate, ethyl butyrate, dimethoxymethane, 1, 2-dimethoxyethane, tetrahydrofuran, 1, 3-dioxolane, dimethyl sulfoxide, sulfolane and dimethyl sulfone.
9. The electrolyte of claim 1, wherein: the electrolyte lithium salt is LiPF6、LiBF4、LiClO4、LiCH3SO3、LiSCN、LiNO3、LiO3SCF2CF3、LiAsF6、LiAlCl4One or more of LiTFSI, LiFSI; the concentration of the electrolyte lithium salt is 0.7-3 mol/L.
10. A lithium ion battery, characterized by: comprising the electrolyte of any one of claims 1 to 9.
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