CN116864807A - Lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte and lithium ion battery - Google Patents
Lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte and lithium ion battery Download PDFInfo
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- CN116864807A CN116864807A CN202310958864.3A CN202310958864A CN116864807A CN 116864807 A CN116864807 A CN 116864807A CN 202310958864 A CN202310958864 A CN 202310958864A CN 116864807 A CN116864807 A CN 116864807A
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- electrolyte
- lithium
- ion battery
- lithium ion
- carbonate
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- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 35
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 33
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 31
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 31
- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 14
- 239000003792 electrolyte Substances 0.000 claims abstract description 56
- 239000000654 additive Substances 0.000 claims abstract description 41
- 230000000996 additive effect Effects 0.000 claims abstract description 35
- 239000002904 solvent Substances 0.000 claims abstract description 33
- 229920001774 Perfluoroether Polymers 0.000 claims abstract description 14
- 239000007774 positive electrode material Substances 0.000 claims abstract description 12
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 11
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 11
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 11
- QMJWCTXTDYGKKZ-UHFFFAOYSA-N cyanomethanesulfonic acid Chemical compound OS(=O)(=O)CC#N QMJWCTXTDYGKKZ-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000007773 negative electrode material Substances 0.000 claims abstract description 7
- 125000004093 cyano group Chemical group *C#N 0.000 claims abstract description 5
- -1 (trimethyl) silane phosphane borate Chemical compound 0.000 claims description 14
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 14
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 11
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 claims description 11
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 8
- 150000001875 compounds Chemical class 0.000 claims description 8
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims description 8
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 7
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 claims description 7
- VTHRQKSLPFJQHN-UHFFFAOYSA-N 3-[2-(2-cyanoethoxy)ethoxy]propanenitrile Chemical compound N#CCCOCCOCCC#N VTHRQKSLPFJQHN-UHFFFAOYSA-N 0.000 claims description 7
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 7
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 7
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 6
- 239000002210 silicon-based material Substances 0.000 claims description 6
- 150000001733 carboxylic acid esters Chemical class 0.000 claims description 5
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 claims description 5
- GWAOOGWHPITOEY-UHFFFAOYSA-N 1,5,2,4-dioxadithiane 2,2,4,4-tetraoxide Chemical compound O=S1(=O)CS(=O)(=O)OCO1 GWAOOGWHPITOEY-UHFFFAOYSA-N 0.000 claims description 4
- 239000007983 Tris buffer Substances 0.000 claims description 4
- 239000002253 acid Substances 0.000 claims description 4
- 150000001335 aliphatic alkanes Chemical class 0.000 claims description 4
- 150000001336 alkenes Chemical class 0.000 claims description 4
- 150000001345 alkine derivatives Chemical class 0.000 claims description 4
- 150000004945 aromatic hydrocarbons Chemical class 0.000 claims description 4
- 150000005676 cyclic carbonates Chemical group 0.000 claims description 4
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 4
- 239000012948 isocyanate Substances 0.000 claims description 4
- 150000002513 isocyanates Chemical class 0.000 claims description 4
- YKYONYBAUNKHLG-UHFFFAOYSA-N propyl acetate Chemical compound CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 4
- FNOVKDUPBMGNFH-UHFFFAOYSA-N B(O)(O)O.C[SiH](C)C Chemical compound B(O)(O)O.C[SiH](C)C FNOVKDUPBMGNFH-UHFFFAOYSA-N 0.000 claims description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 3
- ZJPPTKRSFKBZMD-UHFFFAOYSA-N [Li].FS(=N)F Chemical compound [Li].FS(=N)F ZJPPTKRSFKBZMD-UHFFFAOYSA-N 0.000 claims description 3
- 229910021383 artificial graphite Inorganic materials 0.000 claims description 3
- 238000010030 laminating Methods 0.000 claims description 3
- 238000000926 separation method Methods 0.000 claims description 3
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 3
- 238000004804 winding Methods 0.000 claims description 3
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 2
- 239000011149 active material Substances 0.000 claims description 2
- 150000005678 chain carbonates Chemical class 0.000 claims description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 2
- 150000002148 esters Chemical class 0.000 claims description 2
- 229910052731 fluorine Inorganic materials 0.000 claims description 2
- 125000001153 fluoro group Chemical group F* 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- 125000001424 substituent group Chemical group 0.000 claims description 2
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims 2
- 239000003759 ester based solvent Substances 0.000 claims 2
- 238000002161 passivation Methods 0.000 abstract description 11
- 230000000694 effects Effects 0.000 abstract description 7
- 229910001429 cobalt ion Inorganic materials 0.000 abstract description 4
- XLJKHNWPARRRJB-UHFFFAOYSA-N cobalt(2+) Chemical compound [Co+2] XLJKHNWPARRRJB-UHFFFAOYSA-N 0.000 abstract description 4
- 230000002829 reductive effect Effects 0.000 abstract description 4
- 230000009471 action Effects 0.000 abstract description 3
- 125000004433 nitrogen atom Chemical group N* 0.000 abstract description 3
- 239000000126 substance Substances 0.000 abstract description 3
- 125000000542 sulfonic acid group Chemical group 0.000 abstract description 3
- 239000000203 mixture Substances 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 5
- 230000014759 maintenance of location Effects 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- 239000004698 Polyethylene Substances 0.000 description 2
- FLAFBICRVKZSCF-UHFFFAOYSA-N [Li].[Co]=O.[Li] Chemical compound [Li].[Co]=O.[Li] FLAFBICRVKZSCF-UHFFFAOYSA-N 0.000 description 2
- 239000006230 acetylene black Substances 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 239000001768 carboxy methyl cellulose Substances 0.000 description 2
- 239000006258 conductive agent Substances 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 230000007812 deficiency Effects 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 238000011056 performance test Methods 0.000 description 2
- 229920000573 polyethylene Polymers 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 206010063385 Intellectualisation Diseases 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000003660 carbonate based solvent Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 150000007942 carboxylates Chemical class 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 239000010406 cathode material Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 238000005056 compaction Methods 0.000 description 1
- 229940125904 compound 1 Drugs 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 239000008151 electrolyte solution Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000003631 expected effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 150000002596 lactones Chemical class 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000009517 secondary packaging Methods 0.000 description 1
- 238000007086 side reaction Methods 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 229910001428 transition metal ion Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-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
-
- 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
- H01M10/0569—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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
-
- 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
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0034—Fluorinated solvents
-
- 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 belongs to the technical field of lithium ion batteries, and discloses a lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte and a lithium ion battery. The non-aqueous electrolyte of the lithium cobaltate high-voltage lithium ion battery comprises a non-aqueous organic solvent, electrolyte lithium salt and an additive, wherein the additive comprises a conventional additive and a cyanomethyl sulfonate additive with a structure shown in a formula (I); the solvent comprises a fluoroether solvent with a structure shown in a formula (II). The cyanomethyl sulfonate additive in the electrolyte can be oxidized and decomposed at the interface of the positive electrode to form a passivation film, so that the passivation film has a certain protection effect on the positive electrode material, meanwhile, nitrogen atoms on cyano groups can be chelated with free cobalt ions under the action of lone electron pairs, sulfonic acid groups can be reduced at the interface of the negative electrode to generate a passivation film with dense quality, and active sites on the negative electrode material are prevented from being contacted with the electrolyte; in addition, the fluoroether substance with the structure of the formula (II) is used as a solvent, so that the electrochemical window of the electrolyte can be better widened.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to a lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte and a lithium ion battery.
Background
The lithium ion battery is widely applied to 3C digital products due to the advantages of high working voltage, high energy density, long service life, wide working temperature range, environmental friendliness and the like. Today, light weight and high energy density are increasingly becoming a trend in battery development, especially for 3C digital products. For example, with the intellectualization and diversification of mobile phones, people have been increasingly using mobile phones, so that mobile phones are required to have more electric quantity, lighter weight, and rapid charging performance.
In order to increase the energy density of a lithium ion battery, a common measure is to increase the charge cut-off voltage of a positive electrode material, such as the commercial lithium cobalt oxide lithium ion battery voltage from 4.2V to 4.35V to 4.4V to 4.45V to 4.48V to 4.55V. However, the positive electrode material has certain defects under high voltage, for example, the high voltage positive electrode active material has strong oxidizing property in a lithium deficiency state, and the electrolyte is easily oxidized and decomposed to generate a large amount of gas and heat; in addition, the high-voltage positive electrode active material is unstable in a lithium deficiency state, and side reactions, such as oxygen release, transition metal ion dissolution and the like, are easy to occur.
On the other hand, the quality of the interface morphology of the negative electrode seriously affects the quick charge performance of the battery, so that the additive is required to be capable of reducing to form a passivation film on the negative electrode, and has better performance and better dynamics.
Therefore, development of a novel film-forming additive is required, which can form a passivation film on the positive electrode and the negative electrode, protect the positive electrode material and the negative electrode material, reduce interface resistance of the positive electrode and the negative electrode, and inhibit oxidation and reduction of the solvent.
Disclosure of Invention
In view of the defects and requirements of the prior art, the invention provides a lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte, wherein a cyanomethyl sulfonate additive with a structure shown in a formula (I) in the electrolyte can be oxidized and decomposed at an anode interface to form a passivation film, a certain protection effect is provided for an anode material, and simultaneously nitrogen atoms on cyano groups can be chelated with free cobalt ions under the action of lone electron pairs, sulfonic acid groups can be reduced at a cathode interface to generate a dense passivation film, so that active sites on the cathode material are prevented from being contacted with the electrolyte; in addition, the fluoroether substance with the structure of the formula (II) is used as a solvent, so that the electrochemical window of the electrolyte can be better widened.
In order to achieve the purpose, the nonaqueous electrolyte of the lithium cobaltate high-voltage lithium ion battery comprises a nonaqueous organic solvent, electrolyte lithium salt and an additive, wherein the additive comprises a conventional additive and a cyanomethyl sulfonate additive with a structure shown in a formula (I); the nonaqueous organic solvent comprises a fluoroether solvent having the structure of formula (II),
wherein R is 1 And R is 2 Are each independently selected from aromatic hydrocarbons or derivatives thereof, alkanes and fluoroalkanes, alkenes and fluoroalkenes, alkynes and fluoroalkenes, cyano groups, and the like, and R 1 And R is 2 At least one substituent of (a) contains a fluorine atom; r is R 3 Selected from the group consisting of aromatic hydrocarbons or derivatives thereof, alkanes, alkenes, and alkynes.
Preferably, in some embodiments of the present invention, the isocyanate-based additive having the structure of formula (i) is selected from one or more of compounds (1) - (3):
further preferably, in some embodiments of the present invention, the isocyanate-based additive having the structure of formula (i) is added in an amount of 0.5% to 5%, for example, 0.7% to 1.3% of the total mass of the electrolyte.
Preferably, in some embodiments of the present invention, the fluorocarboxylic acid ester solvent having the structure of formula (ii) is selected from one or more of compounds (4) - (6):
further preferably, in some embodiments of the present invention, the fluorinated carboxylic ester solvent having the structure of formula (ii) is added in an amount of 5.0% to 20.0% based on the total mass of the electrolyte.
Further, in some embodiments of the present invention, the conventional additive is selected from one or more of fluoroethylene carbonate (FEC), succinonitrile (SN), adiponitrile (ADN), 1,3, 6-Hexanetrinitrile (HTCN), 1, 2-bis (cyanoethoxy) ethane (DENE), 1, 3-Propane Sultone (PS), 1, 3-propenesulfonic acid lactone (PST), vinyl Ethylene Carbonate (VEC), vinyl sulfate (DTD), tris (trimethyl) silane borate (TMSB), tris (trimethyl) silane phosphane borate (TMSP), and Methylene Methane Disulfonate (MMDS).
Further, in some embodiments of the present invention, the conventional additive is added in an amount of 5.0% to 30.0% of the total mass of the electrolyte.
Preferably, in some embodiments of the present invention, when the conventional additive is included, the fluoroethylene carbonate is added in an amount of 1.0% to 30.0% of the total mass of the electrolyte; the addition amount of the sulfur-series additives such as the 1, 3-propane sultone, the 1, 3-propylene sultone and the like accounts for 0.1 to 10.0 percent of the total mass of the electrolyte; the addition amount of nitrile additives such as succinonitrile, adiponitrile, 1,3, 6-hexanetrinitrile, 1, 2-bis (cyanoethoxy) ethane and the like accounts for 1.0-10.0% of the total mass of the electrolyte; the addition amount of one of other special additives such as tri (trimethyl) silane borate/tri (trimethyl) silane phosphane borate and the like accounts for 0.1-2.0% of the total mass of the electrolyte.
Further, in some embodiments of the present invention, the conventional additives are fluoroethylene carbonate (FEC), 1, 3-Propane Sultone (PS), adiponitrile (ADN), 1, 2-bis (cyanoethoxy) ethane (DENE), and vinyl sulfate (DTD); preferably, the addition amount of the fluoroethylene carbonate accounts for 5.0-9.0% of the total mass of the electrolyte, the addition amount of the 1, 3-propane sultone accounts for 2.5-3.5% of the total mass of the electrolyte, the addition amount of the adiponitrile accounts for 1.5-2.5% of the total mass of the electrolyte, the addition amount of the 1, 2-bis (cyanoethoxy) ethane accounts for 0.7-1.3% of the total mass of the electrolyte, and the addition amount of the vinyl sulfate accounts for 0.7-1.3% of the total mass of the electrolyte.
Further, in some embodiments of the present invention, the electrolyte lithium salt is selected from one or more of lithium hexafluorophosphate, lithium difluorosulfonimide, lithium tetrafluoroborate, and lithium difluorophosphate, and preferably, the addition amount of the electrolyte lithium salt is 12.5% to 30.0% of the total mass of the electrolyte.
Preferably, in some embodiments of the present invention, the electrolyte lithium salt is a mixed lithium salt of lithium hexafluorophosphate, lithium difluorophosphate, and lithium difluorosulfonimide, and the addition amount of the lithium hexafluorophosphate is 10.5% to 17.0% of the total mass of the electrolyte, the addition amount of the lithium difluorophosphate is 0.5% to 1.5% of the total mass of the electrolyte, and the addition amount of the lithium difluorosulfonimide is 3.0% to 7.0% of the total mass of the electrolyte.
Further, in some embodiments of the present invention, the non-aqueous organic solvent is selected from the group consisting of carbonate solvents, carboxylate solvents, fluorocarbonate solvents, fluorocarboxylate solvents, fluoroether solvents.
Further, in some embodiments of the invention, the carbonate-based solvent is selected from the group consisting of cyclic carbonates, chain carbonates; wherein the cyclic carbonate solvent is selected from one or more of ethylene carbonate and propylene carbonate; the chain carbonic ester is selected from one or more of dimethyl carbonate, diethyl carbonate and ethylmethyl carbonate; the carboxylic ester solvent is selected from one or more of ethyl acetate, n-propyl acetate, ethyl propionate and propyl propionate; the fluoroether solvent is selected from compounds (4) - (6).
Further, in some embodiments of the present invention, the nonaqueous organic solvent comprises ethylene carbonate, propylene carbonate, ethyl propionate, propyl propionate, and fluoroether solvents; preferably, the mass ratio of the ethylene carbonate, the propylene carbonate, the ethyl propionate, the propyl propionate and the fluoroether solvent in the nonaqueous organic solvent is 8-13:15-25:15-25:35-45:8-13, e.g. 10:20:20:40:10.
on the other hand, the invention also provides a lithium cobaltate high-voltage lithium ion battery, which comprises an electric core formed by laminating or winding a positive plate, a separation film and a negative plate, and the lithium cobaltate high-voltage lithium ion battery electrolyte, wherein the positive active material of the positive plate is lithium cobaltate active material, and the compaction density of the positive plate is 4.2-4.6 g/cm 3 。
Further, in some embodiments of the present invention, the negative electrode active material of the negative electrode sheet is artificial graphite and a silicon-based material, wherein the silicon-based material is selected from one or more of silicon oxide, elemental silicon material, and the compacted density of the negative electrode sheet is 1.6 to 1.8g/cm 3 。
Further, in some embodiments of the invention, the lithium ion battery has a charge cutoff voltage of 4.45V or more.
Compared with the prior art, the invention has the main advantages that: the cyanomethyl sulfonate additive with the structure shown in the formula (I) can be oxidized and decomposed at the interface of a positive electrode to form a passivation film, has a certain protection effect on the positive electrode material, and simultaneously nitrogen atoms on cyano groups can be chelated with free cobalt ions under the action of lone electron pairs, and sulfonic acid groups can be reduced at the interface of a negative electrode to generate a dense passivation film, so that active sites on the negative electrode material are prevented from being contacted with electrolyte. The method comprises the steps of carrying out a first treatment on the surface of the The fluoroether substance with the structure of formula (II) is used as a solvent, so that the electrochemical window of the electrolyte can be better widened.
Detailed Description
The present invention will be described in further detail with reference to the following examples in order to make the objects, technical solutions and advantages of the present invention more apparent. Additional aspects and advantages of the invention will be set forth in part in the description which follows, and in part will be obvious from the description, or may be learned by practice of the invention. It is to be understood that the following description is intended to be illustrative of the invention and not restrictive.
The terms "comprising," "including," "containing," or any other variation thereof, as used herein, are intended to cover a non-exclusive inclusion. For example, a composition, step, method, article, or apparatus that comprises a list of elements is not necessarily limited to only those elements but may include other elements not expressly listed or inherent to such composition, step, method, article, or apparatus.
When an equivalent, concentration, or other value or parameter is expressed as a range, preferred range, or a range bounded by a list of upper preferable values and lower preferable values, this is to be understood as specifically disclosing all ranges formed from any pair of any upper range limit or preferred value and any lower range limit or preferred value, regardless of whether ranges are separately disclosed. For example, when ranges of "1 to 5" are disclosed, the described ranges should be construed to include ranges of "1 to 4", "1 to 3", "1 to 2 and 4 to 5", "1 to 3 and 5", and the like. When a numerical range is described herein, unless otherwise indicated, the range is intended to include its endpoints and all integers and fractions within the range.
The singular forms include plural referents unless the context clearly dictates otherwise. "optional" or "any" means that the subsequently described event or event may or may not occur, and that the description includes both cases where the event occurs and cases where the event does not.
The indefinite articles "a" and "an" preceding an element or component of the invention are not limited to the requirement (i.e. the number of occurrences) of the element or component. Thus, the use of "a" or "an" should be interpreted as including one or at least one, and the singular reference of an element or component includes the plural reference unless the amount clearly dictates otherwise.
Example 1
Preparation of electrolyte: in a glove box filled with argon, ethylene carbonate, propylene carbonate, ethyl propionate, propyl propionate and a compound (4) are mixed according to the mass ratio of EC: PC: EP: PP: compound (4) =10: 20:20:40:10, slowly adding lithium hexafluorophosphate accounting for 14.0 percent of the total mass of the electrolyte and lithium difluorophosphate accounting for 1.0 percent of the total mass of the electrolyte into the mixed solution, adding lithium difluorosulfimide accounting for 5.0 percent of the total mass of the electrolyte, and finally adding a cyanomethyl sulfonate additive (compound 1) accounting for 1.0 percent of the total mass of the electrolyte, and stirring uniformly to obtain the lithium ion battery electrolyte of the embodiment 1.
Preparation of a lithium ion battery:
the positive electrode active material lithium cobaltate, the conductive agent acetylene black and the binder polyvinylidene fluoride (PVDF) are mixed according to the mass ratio of 95:3: and 2, fully stirring and uniformly mixing the mixture in an N-methyl pyrrolidone solvent system, coating the mixture on an aluminum foil, drying and cold pressing the aluminum foil, and obtaining the positive plate.
The negative electrode active material artificial graphite, silicon oxide, conductive agent acetylene black, binder Styrene Butadiene Rubber (SBR) and thickener sodium carboxymethyl cellulose (CMC) are mixed according to the mass ratio of 88:8:2.5:0.5: and 1, fully stirring and uniformly mixing the materials in a deionized water solvent system, coating the materials on a copper foil, drying and cold pressing the materials, and thus obtaining the negative plate.
Polyethylene (PE) is used as a base film, and a nano alumina coating is coated on the base film to be used as a separation film.
And (3) sequentially laminating the positive plate, the isolating film and the negative plate, winding in the same direction to obtain a bare cell, placing the bare cell in an outer package, injecting prepared electrolyte, and performing procedures such as packaging, placing at 45 ℃, high-temperature clamp formation, secondary packaging, capacity division and the like to obtain the high-voltage lithium cobalt oxide lithium ion battery.
Examples 2 to 7
Examples 2 to 7 and comparative examples 1 to 7 were the same as example 1 except that the composition ratios of the respective components of the electrolytic solutions were added as shown in Table 1.
TABLE 1 composition ratios of respective components of electrolytes of examples 1 to 7 and comparative examples 1 to 7
Effect testing
1) And (3) testing normal temperature cycle performance: at 25 ℃, the battery after capacity division is charged to 4.48V according to constant current and constant voltage of 0.7C, the cut-off current is 0.02C, then the battery is discharged to 3.0V according to constant current of 0.7C, and the cycle capacity retention rate of 500 weeks is calculated after 500 cycles of charge/discharge. The calculation formula is as follows:
500 th cycle capacity retention (%) = (500 th cycle discharge capacity/first cycle discharge capacity) ×100%.
2) And (3) testing the residual rate of the constant-temperature storage capacity at 85 ℃): firstly, the battery is circularly charged and discharged for 1 time (4.48V-3.0V) at the normal temperature under the temperature of 0.5C, and the discharge capacity C before the battery is stored is recorded 0 Then charging the battery to a full state of 4.48V at constant current and constant voltage, then placing the battery into an incubator at 85 ℃ for storage for 4 hours, and taking out the battery after the storage is completed; after the battery is cooled for 24 hours at room temperature, the battery is discharged to 3.0V at constant current of 0.5C again, and the discharge capacity C of the battery after storage is recorded 1 And calculating the capacity remaining rate of the battery after being stored for 4 hours at the constant temperature of 85 ℃, wherein the calculation formula is as follows:
capacity remaining rate=c after constant temperature storage at 85 ℃ for 4 hours 1 /C 0 *100％。
3) 45 ℃ cycle performance test: at 45 ℃, the battery after capacity division is charged to 4.48V according to constant current and constant voltage of 0.7C, the cut-off current is 0.02C, then the battery is discharged to 3.0V according to constant current of 0.7C, and the cycle capacity retention rate of 300 weeks is calculated after 300 cycles of charging/discharging. The calculation formula is as follows:
300 th cycle capacity retention (%) = (300 th cycle discharge capacity/first cycle discharge capacity) ×100%.
Table 2 battery performance test results for each of examples and comparative examples
From examples 1 to 5 and comparative examples 1 to 3 in Table 2, the electrochemical properties were as follows: the novel additive of the cyanomethyl sulfonate with the structure (I) can improve the electrochemical performance of a lithium cobaltate high-voltage battery, but the effect is not particularly good when the novel additive is singly used, and mainly consists of a single passivation film component formed by oxidizing a single additive at an anode interface, and only solvent ethylene carbonate is used for forming a film of a negative electrode. In addition, the addition amount of the novel cyanomethyl sulfonate additive with the structure (I) exceeds or is lower than the addition amount of the novel cyanomethyl sulfonate additive, and the expected effect of experiments cannot be achieved.
The electrochemical properties of examples 6-7 and comparative example 6 in table 2 show that the novel additive has better effect when being used in combination with other additives, and the novel additive mainly has the advantages that the novel additive can generate decomposition reaction at the interface of the positive electrode material to generate a passivation film, inhibit the dissolution of cobalt in the positive electrode material, prevent cobalt ions from migrating to the interface of the negative electrode material, catalyze the reductive decomposition of the solvent and have a certain effect on the positive and negative electrode protection.
Those skilled in the art will readily appreciate from the foregoing disclosure and teachings that various changes and modifications may be made to the foregoing embodiments and that any and all modifications, equivalents, and improvements may be made within the spirit and principles of the present invention. In addition, although specific terms are used in the present specification, these terms are for convenience of description only and do not limit the present invention in any way.
Claims (10)
1. The non-aqueous electrolyte of the lithium cobaltate high-voltage lithium ion battery comprises a non-aqueous organic solvent, electrolyte lithium salt and an additive, and is characterized in that the additive comprises a conventional additive and a cyanomethyl sulfonate additive with a structure shown in a formula (I); the nonaqueous organic solvent comprises a fluoroether solvent with a structure shown in a formula (II),
wherein R is 1 And R is 2 Are each independently selected from the group consisting of aromatic hydrocarbons or derivatives thereof, alkanes and fluoroalkanes, alkenes and fluoroalkenes, alkynes and fluoroalkenes, and cyano groups, and R 1 And R is 2 At least one substituent of (a) contains a fluorine atom; r is R 3 Selected from the group consisting of aromatic hydrocarbons or derivatives thereof, alkanes, alkenes, and alkynes.
2. The lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte according to claim 1, wherein the isocyanate-based additive having the structure of formula (i) is selected from one or more of compounds (1) to (3):
preferably, the isocyanate-based additive having the structure of formula (i) is added in an amount of 0.5% to 5%, for example 0.7% to 1.3% of the total mass of the electrolyte.
3. The lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte according to claim 1, wherein the fluorocarboxylic acid ester solvent having the structure of formula (ii) is selected from one or more of compounds (4) to (6):
preferably, the addition amount of the fluorinated carboxylic ester solvent with the structure of formula (II) accounts for 5.0-20.0% of the total mass of the electrolyte.
4. The lithium cobaltate high voltage lithium ion battery non-aqueous electrolyte according to claim 1, wherein the conventional additive is selected from one or more of fluoroethylene carbonate (FEC), succinonitrile (SN), adiponitrile (ADN), 1,3, 6-Hexanetrinitrile (HTCN), 1, 2-bis (cyanoethoxy) ethane (DENE), 1, 3-Propane Sultone (PS), 1, 3-Propenolactone (PST), vinylene carbonate (VEC), vinyl sulfate (DTD), tris (trimethyl) silane borate (TMSB), tris (trimethyl) silane phosphane borate (TMSP) and Methylene Methane Disulfonate (MMDS); preferably, the addition amount of the conventional additive accounts for 5.0-30.0% of the total mass of the electrolyte.
5. The lithium cobaltate high voltage lithium ion battery nonaqueous electrolyte according to claim 1, wherein the conventional additives are fluoroethylene carbonate (FEC), 1, 3-Propane Sultone (PS), adiponitrile (ADN), 1, 2-bis (cyanoethoxy) ethane (DENE) and vinyl sulfate (DTD); preferably, the addition amount of the fluoroethylene carbonate accounts for 5.0-9.0% of the total mass of the electrolyte, the addition amount of the 1, 3-propane sultone accounts for 2.5-3.5% of the total mass of the electrolyte, the addition amount of the adiponitrile accounts for 1.5-2.5% of the total mass of the electrolyte, the addition amount of the 1, 2-bis (cyanoethoxy) ethane accounts for 0.7-1.3% of the total mass of the electrolyte, and the addition amount of the vinyl sulfate accounts for 0.7-1.3% of the total mass of the electrolyte.
6. The lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte according to claim 1, wherein the electrolyte lithium salt is one or more selected from lithium hexafluorophosphate, lithium difluorosulfonimide, lithium tetrafluoroborate and lithium difluorophosphate; preferably, the addition amount of the electrolyte lithium salt accounts for 12.5-30.0% of the total mass of the electrolyte; preferably, the electrolyte lithium salt is a mixed lithium salt of lithium hexafluorophosphate, lithium difluorophosphate and lithium difluorosulfimide, wherein the addition of the lithium hexafluorophosphate accounts for 10.5-17.0% of the total mass of the electrolyte, the addition of the lithium difluorophosphate accounts for 0.5-1.5% of the total mass of the electrolyte, and the addition of the lithium difluorosulfimide accounts for 3.0-7.0% of the total mass of the electrolyte.
7. The lithium cobaltate high-voltage lithium ion battery nonaqueous electrolyte according to claim 1, wherein the nonaqueous organic solvent is selected from the group consisting of carbonate solvents, carboxylic acid ester solvents, fluorocarbonate solvents, fluorocarboxylic acid ester solvents, fluoroether solvents; preferably, the carbonate solvent is selected from cyclic carbonates and chain carbonates; wherein the cyclic carbonate solvent is selected from one or more of ethylene carbonate and propylene carbonate; the chain carbonic ester is selected from one or more of dimethyl carbonate, diethyl carbonate and ethylmethyl carbonate; the carboxylic ester solvent is selected from one or more of ethyl acetate, n-propyl acetate, ethyl propionate and propyl propionate; the fluoroether solvent is selected from compounds (4) - (6); preferably, the nonaqueous organic solvent comprises ethylene carbonate, propylene carbonate, ethyl propionate, propyl propionate and fluoroether solvents; preferably, the mass ratio of the ethylene carbonate, the propylene carbonate, the ethyl propionate, the propyl propionate and the fluoroether solvent in the nonaqueous organic solvent is 8-13:15-25:15-25:35-45:8-13, e.g. 10:20:20:40:10.
8. a lithium cobaltate high-voltage lithium ion battery, characterized in that the lithium cobaltate high-voltage lithium ion battery comprises an electric core formed by laminating or winding a positive plate, a separation film and a negative plate, and the lithium cobaltate high-voltage lithium ion battery electrolyte as claimed in any one of claims 1 to 7; preferably, the positive electrode active material of the positive electrode sheet is lithium cobaltate active material; preferably, the positive electrode sheet has a compacted density of 4.2 to 4.6g/cm 3 。
9. The lithium cobaltate high voltage lithium ion battery of claim 8 wherein the negative electrode active material of the negative electrode sheet is artificial graphite or a part and a silicon-based material, wherein the silicon-based material is selected from one or more of silicon oxide, elemental silicon material; preferably, the negative electrode sheet has a compacted density of 1.6 to 1.8g/cm 3 。
10. The lithium cobaltate high voltage lithium ion battery of claim 8 wherein the lithium ion battery has a charge cut-off voltage of 4.45V or more.
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