CN117477020A - Lithium ion gel electrolyte, lithium ion battery and preparation method of lithium ion gel electrolyte - Google Patents
Lithium ion gel electrolyte, lithium ion battery and preparation method of lithium ion gel electrolyte Download PDFInfo
- Publication number
- CN117477020A CN117477020A CN202311429366.6A CN202311429366A CN117477020A CN 117477020 A CN117477020 A CN 117477020A CN 202311429366 A CN202311429366 A CN 202311429366A CN 117477020 A CN117477020 A CN 117477020A
- Authority
- CN
- China
- Prior art keywords
- lithium
- lithium ion
- electrolyte
- gel state
- ion gel
- Prior art date
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 49
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 49
- 239000011245 gel electrolyte Substances 0.000 title claims abstract description 19
- 238000002360 preparation method Methods 0.000 title abstract description 6
- 239000003792 electrolyte Substances 0.000 claims abstract description 32
- 239000000654 additive Substances 0.000 claims abstract description 24
- 239000000178 monomer Substances 0.000 claims abstract description 24
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 23
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 22
- KOMNUTZXSVSERR-UHFFFAOYSA-N 1,3,5-tris(prop-2-enyl)-1,3,5-triazinane-2,4,6-trione Chemical compound C=CCN1C(=O)N(CC=C)C(=O)N(CC=C)C1=O KOMNUTZXSVSERR-UHFFFAOYSA-N 0.000 claims abstract description 19
- 230000000996 additive effect Effects 0.000 claims abstract description 17
- 229920000642 polymer Polymers 0.000 claims abstract description 17
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 claims abstract description 13
- 239000003960 organic solvent Substances 0.000 claims abstract description 11
- 239000003999 initiator Substances 0.000 claims abstract description 9
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 9
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 9
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 19
- 229910052759 nickel Inorganic materials 0.000 claims description 14
- 238000000034 method Methods 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 9
- 238000002156 mixing Methods 0.000 claims description 8
- 239000002243 precursor Substances 0.000 claims description 8
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 6
- 239000002253 acid Substances 0.000 claims description 6
- CQEYYJKEWSMYFG-UHFFFAOYSA-N butyl acrylate Chemical compound CCCCOC(=O)C=C CQEYYJKEWSMYFG-UHFFFAOYSA-N 0.000 claims description 6
- -1 lithium hexafluorophosphate Chemical compound 0.000 claims description 6
- OZAIFHULBGXAKX-UHFFFAOYSA-N 2-(2-cyanopropan-2-yldiazenyl)-2-methylpropanenitrile Chemical compound N#CC(C)(C)N=NC(C)(C)C#N OZAIFHULBGXAKX-UHFFFAOYSA-N 0.000 claims description 5
- 239000011230 binding agent Substances 0.000 claims description 5
- 239000006258 conductive agent Substances 0.000 claims description 5
- 239000000463 material Substances 0.000 claims description 5
- 239000007774 positive electrode material Substances 0.000 claims description 5
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 4
- 239000011149 active material Substances 0.000 claims description 4
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 4
- 238000006116 polymerization reaction Methods 0.000 claims description 4
- 238000003756 stirring Methods 0.000 claims description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 3
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 3
- 239000006260 foam Substances 0.000 claims description 3
- 239000003112 inhibitor Substances 0.000 claims description 3
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 3
- 238000007789 sealing Methods 0.000 claims description 3
- 125000005463 sulfonylimide group Chemical group 0.000 claims description 3
- BQCIDUSAKPWEOX-UHFFFAOYSA-N 1,1-Difluoroethene Chemical compound FC(F)=C BQCIDUSAKPWEOX-UHFFFAOYSA-N 0.000 claims description 2
- MYWOJODOMFBVCB-UHFFFAOYSA-N 1,2,6-trimethylphenanthrene Chemical compound CC1=CC=C2C3=CC(C)=CC=C3C=CC2=C1C MYWOJODOMFBVCB-UHFFFAOYSA-N 0.000 claims description 2
- WXBWKMLIVXELSF-UHFFFAOYSA-N 2,2,2-trifluoro-n,n-dimethylacetamide Chemical compound CN(C)C(=O)C(F)(F)F WXBWKMLIVXELSF-UHFFFAOYSA-N 0.000 claims description 2
- 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 2
- GTELLNMUWNJXMQ-UHFFFAOYSA-N 2-ethyl-2-(hydroxymethyl)propane-1,3-diol;prop-2-enoic acid Chemical class OC(=O)C=C.OC(=O)C=C.OC(=O)C=C.CCC(CO)(CO)CO GTELLNMUWNJXMQ-UHFFFAOYSA-N 0.000 claims description 2
- ZAYGISOXMIXWHX-UHFFFAOYSA-N 2-methylpropoxycarbonyloxy 2-methylpropyl carbonate Chemical compound CC(C)COC(=O)OOC(=O)OCC(C)C ZAYGISOXMIXWHX-UHFFFAOYSA-N 0.000 claims description 2
- CFVWNXQPGQOHRJ-UHFFFAOYSA-N 2-methylpropyl prop-2-enoate Chemical compound CC(C)COC(=O)C=C CFVWNXQPGQOHRJ-UHFFFAOYSA-N 0.000 claims description 2
- XOJWAAUYNWGQAU-UHFFFAOYSA-N 4-(2-methylprop-2-enoyloxy)butyl 2-methylprop-2-enoate Chemical compound CC(=C)C(=O)OCCCCOC(=O)C(C)=C XOJWAAUYNWGQAU-UHFFFAOYSA-N 0.000 claims description 2
- OMPJBNCRMGITSC-UHFFFAOYSA-N Benzoylperoxide Chemical compound C=1C=CC=CC=1C(=O)OOC(=O)C1=CC=CC=C1 OMPJBNCRMGITSC-UHFFFAOYSA-N 0.000 claims description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 2
- DAKWPKUUDNSNPN-UHFFFAOYSA-N Trimethylolpropane triacrylate Chemical compound C=CC(=O)OCC(CC)(COC(=O)C=C)COC(=O)C=C DAKWPKUUDNSNPN-UHFFFAOYSA-N 0.000 claims description 2
- OKKRPWIIYQTPQF-UHFFFAOYSA-N Trimethylolpropane trimethacrylate Chemical compound CC(=C)C(=O)OCC(CC)(COC(=O)C(C)=C)COC(=O)C(C)=C OKKRPWIIYQTPQF-UHFFFAOYSA-N 0.000 claims description 2
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 claims description 2
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 claims description 2
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical compound [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 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
- 235000019400 benzoyl peroxide Nutrition 0.000 claims description 2
- BLCKNMAZFRMCJJ-UHFFFAOYSA-N cyclohexyl cyclohexyloxycarbonyloxy carbonate Chemical compound C1CCCCC1OC(=O)OOC(=O)OC1CCCCC1 BLCKNMAZFRMCJJ-UHFFFAOYSA-N 0.000 claims description 2
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 claims description 2
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 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
- 239000010439 graphite Substances 0.000 claims description 2
- 229910002804 graphite Inorganic materials 0.000 claims description 2
- 229910021385 hard carbon Inorganic materials 0.000 claims description 2
- 150000002596 lactones Chemical class 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
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 claims description 2
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 claims description 2
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 claims description 2
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 2
- 229940090181 propyl acetate Drugs 0.000 claims description 2
- 229910021384 soft carbon Inorganic materials 0.000 claims description 2
- ISXSCDLOGDJUNJ-UHFFFAOYSA-N tert-butyl prop-2-enoate Chemical compound CC(C)(C)OC(=O)C=C ISXSCDLOGDJUNJ-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
- 229940096522 trimethylolpropane triacrylate Drugs 0.000 claims 1
- 230000002195 synergetic effect Effects 0.000 abstract description 4
- 238000004146 energy storage Methods 0.000 abstract description 3
- 230000000052 comparative effect Effects 0.000 description 22
- 238000003860 storage Methods 0.000 description 13
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical group OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 description 8
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 239000002904 solvent Substances 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 239000003431 cross linking reagent Substances 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- 229910052723 transition metal Inorganic materials 0.000 description 3
- 239000002000 Electrolyte additive Substances 0.000 description 2
- 238000007792 addition Methods 0.000 description 2
- 125000004093 cyano group Chemical group *C#N 0.000 description 2
- 238000011065 in-situ storage Methods 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 239000011572 manganese Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 150000002825 nitriles Chemical class 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- XAMCLRBWHRRBCN-UHFFFAOYSA-N 5-prop-2-enoyloxypentyl prop-2-enoate Chemical compound C=CC(=O)OCCCCCOC(=O)C=C XAMCLRBWHRRBCN-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 229910013716 LiNi Inorganic materials 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-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
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 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
- 230000000536 complexating effect Effects 0.000 description 1
- 238000010668 complexation reaction Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000010494 dissociation reaction Methods 0.000 description 1
- 230000005593 dissociations Effects 0.000 description 1
- 239000011267 electrode slurry Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 150000003949 imides Chemical class 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 238000010406 interfacial reaction Methods 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 239000002808 molecular sieve Substances 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 125000002560 nitrile group Chemical group 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000004537 pulping Methods 0.000 description 1
- 238000004080 punching Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000005096 rolling process Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 150000003624 transition metals Chemical class 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
- H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
- C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
- C08F220/10—Esters
- C08F220/12—Esters of monohydric alcohols or phenols
- C08F220/16—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms
- C08F220/18—Esters of monohydric alcohols or phenols of phenols or of alcohols containing two or more carbon atoms with acrylic or methacrylic acids
- C08F220/1804—C4-(meth)acrylate, e.g. butyl (meth)acrylate, isobutyl (meth)acrylate or tert-butyl (meth)acrylate
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
- C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
- C08F220/42—Nitriles
- C08F220/44—Acrylonitrile
- C08F220/48—Acrylonitrile with nitrogen-containing monomers
-
- 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
- H01M10/058—Construction or manufacture
-
- 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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0082—Organic polymers
-
- 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)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- General Chemical & Material Sciences (AREA)
- Electrochemistry (AREA)
- Manufacturing & Machinery (AREA)
- Health & Medical Sciences (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- General Physics & Mathematics (AREA)
- Dispersion Chemistry (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- Materials Engineering (AREA)
- Physics & Mathematics (AREA)
- Secondary Cells (AREA)
Abstract
The invention discloses a lithium ion gel electrolyte, a lithium ion battery and a preparation method thereof, wherein the lithium ion gel electrolyte comprises a polymer monomer, an organic solvent, lithium salt, an additive and an initiator, the polymer monomer at least comprises 1,3, 5-triallyl isocyanurate and acrylonitrile, and the additive at least comprises FEC;1,3, 5-triallyl isocyanurate accounts for 0.1-2% of the total mass of the lithium ion gel state electrolyte, and acrylonitrile accounts for 2.5-7.5% of the total mass of the lithium ion gel state electrolyte. According to the invention, through the synergistic effect of various monomers and additives of the gel electrolyte, the stability of the electrode/electrolyte interface and the high-temperature stability of the lithium battery are realized, and the use safety and the high-temperature energy storage capacity of the battery can be improved on the premise of optimizing the electrochemical stability of the electrolyte/electrode interface.
Description
Technical Field
The invention belongs to the technical field of lithium batteries, relates to a gel state battery, and in particular relates to a lithium ion gel state electrolyte, a lithium ion battery and a preparation method thereof.
Background
The high-nickel ternary anode is used for replacing the traditional lithium iron phosphate anode, so that the energy density of the lithium battery is improved to 300Wh Kg -1 The effective way is as above. However, the strong side reactions of the high voltage positive electrode and the conventional electrolyte can cause a large electrode/electrolyte interface impedance, affecting the practical use of the battery. In order to improve the cycle stability of the battery, FEC has been widely used as an additive for a high energy density lithium battery because it has a property of decomposing into a film on the electrode surface and suppressing interfacial side reactions.
On the other hand, the structural instability of the high-nickel ternary positive electrode determines that transition metal elements (nickel, cobalt and manganese) in the structure of the high-nickel ternary positive electrode can be dissolved in electrolyte in the charging and discharging process, and the transition metal elements are transferred from the positive electrode to the surface of the negative electrode along with the charging and discharging process, so that the intermediate layer of the solid electrolyte is seriously damaged. To solve this problem, the in-situ polymer of the polymer monomer, the electrolyte and the initiator is adopted to replace the traditional electrolyte, so that the electrolyte can be converted into a non-flowing gel state from a liquid state, thereby inhibiting the transfer of metal elements and maintaining the excellent interface wettability and the ion conductivity of the electrolyte. By using a gel electrolyte and FEC additives, the cycling stability of the high nickel ternary gel state cell is significantly improved compared to the liquid state cell.
However, the gel state battery needs to have excellent high temperature storage properties, which is determined by its use environment as a power battery and the actual situation that the gel in situ curing requires high temperature. However, FEC additives and conventional LiPF 6 Lithium salts, which exist at severely high temperatures as gel electrolyte componentsInstability, in the high temperature storage process, is easy to decompose to generate hydrofluoric acid, thereby corroding the positive electrode material and causing the reduction of battery performance.
In order to improve the high-temperature energy storage capacity of the high-nickel ternary lithium battery containing the FEC additive, the 1,3, 5-triallyl isocyanurate is widely used as an electrolyte additive because of the characteristics of low cost, low melting point and environmental friendliness, and the isocyanurate structure has the effects of water removal and acid control, wherein nitrogen atoms in the six-membered ring structure can carry out complexation reaction with positive transition metal, so that side reactions of the high-nickel ternary positive electrode in the process of charging and discharging and electrolyte are inhibited. For example, publication number CN106450432a proposes a method of using 1,3, 5-triallyl isocyanurate and FEC as additives simultaneously, effectively improving the high-temperature storage property and cycle stability of the battery. The publication No. CN106654242A uses 1,3, 5-triallyl isocyanurate, dinitrile compounds and FEC as electrolyte additives to respectively protect the anode and the cathode, so that the contact stability of the high-nickel ternary anode and the silicon cathode under high-pressure and high-temperature conditions and the electrolyte is improved.
However, 1,3, 5-triallyl isocyanurate is susceptible to polymerization reaction on the surface of a negative electrode when used as an additive due to the presence of a chemically unstable double bond in the structure thereof, and nitrile additives have the defect of unstable contact with the negative electrode, resulting in a large interface resistance of the negative electrode. In addition, the high viscosity of nitriles and isocyanuric acid affects lithium ion conduction of the electrolyte and affects the ionic conductivity of the electrolyte.
Disclosure of Invention
In view of the above, the present invention provides a lithium ion gel electrolyte, a lithium ion battery, and a method of preparing the same. The gel state battery consists of a negative electrode, a gel state electrolyte and a high-nickel ternary positive electrode, and the preparation process of the gel state battery is compatible with the existing liquid state battery. Wherein, due to the existence of gel electrolyte, the battery has excellent electrochemical stability of anode and cathode interfaces and high-temperature storage performance.
In order to achieve the above purpose, the present invention adopts the following technical scheme:
the invention firstly provides a lithium ion gel electrolyte, which comprises a polymer monomer, an organic solvent, lithium salt, an additive and an initiator, wherein the polymer monomer at least comprises 1,3, 5-triallyl isocyanurate and acrylonitrile, and the additive at least comprises FEC;1,3, 5-triallyl isocyanurate accounts for 0.1-2% of the total mass of the lithium ion gel state electrolyte, and acrylonitrile accounts for 2.5-7.5% of the total mass of the lithium ion gel state electrolyte.
As a preferred embodiment of the present invention, the polymer monomer further comprises one or more of ethoxylated trimethylolpropane triacrylate, pentaerythritol tetraacrylate, trimethylolpropane triacrylate, trimethylolpropane trimethacrylate, butyl acrylate, t-butyl acrylate, isobutyl acrylate, 1, 4-butylene glycol dimethacrylate, and vinylidene fluoride.
As a preferable mode of the present invention, the organic solvent includes two or more of ethyl propionate, propyl acetate, ethyl acetate, methyl acetate, dimethyl carbonate, diethyl carbonate, propyl propionate, ethylene carbonate, propylene carbonate, methyl ethyl carbonate, and dipropyl carbonate.
As a preferred embodiment of the present invention, the lithium salt includes one or more of lithium hexafluorophosphate, lithium perchlorate, lithium difluorooxalato borate, lithium trifluoromethane sulfonate, lithium bistrifluoromethyl sulfonyl imide, and lithium bistrifluorosulfonyl imide.
As a preferable scheme of the invention, the FEC accounts for 5-20% of the total mass of the lithium ion gel electrolyte, and the additive further comprises one or more of lithium difluorophosphate, lithium bisoxalato borate, vinyl sulfate, 1, 3-propenesulfonic acid lactone and N, N-dimethyl trifluoroacetamide.
As a preferred embodiment of the present invention, the initiator comprises one or more of azobisisobutyronitrile, azobisisoheptonitrile, dibenzoyl peroxide, diisobutyl peroxydicarbonate, dicyclohexyl peroxydicarbonate.
The invention also provides a gel state lithium ion battery, which comprises the lithium ion gel state electrolyte, a negative electrode, a positive electrode and a diaphragm.
As a preferred embodiment of the present invention, the positive electrode includes a positive electrode active material, a conductive agent, a binder, and a current collector; the positive electrode active material comprises one or more of lithium iron phosphate, lithium manganese iron phosphate, lithium nickelate, lithium manganate, lithium cobaltate, nickel cobalt manganese ternary material and nickel cobalt aluminum ternary material.
As a preferred aspect of the present invention, the negative electrode includes a negative electrode sheet including a lithium-containing metal and a current collector; or a negative electrode sheet containing an active material, a conductive agent, a binder, and a current collector; wherein the active material comprises one or more of graphite, hard carbon, soft carbon, silicon oxygen and silicon carbon.
The invention finally provides a preparation method of the gel state lithium ion battery, which comprises the following steps:
1) Controlling the water content to be less than or equal to 10ppm, and uniformly mixing the organic solvent to obtain an organic solvent component;
2) Controlling the water content to be less than or equal to 10ppm, removing the polymerization inhibitor from the polymer monomer, and uniformly mixing to obtain a polymer monomer component;
3) Controlling the water content to be less than or equal to 10ppm, mixing the polymer monomer component obtained in the step 2), the organic solvent component obtained in the step 1), the additive and the lithium salt, adding an initiator, and stirring until the mixture is clear to obtain a precursor;
4) And (3) assembling the positive electrode shell, the positive electrode plate, the diaphragm, the lithium plate, the foam nickel and the negative electrode plate in sequence, injecting the precursor obtained in the step (3), and stamping and sealing to obtain the gel-state lithium ion battery.
Compared with the prior art, the invention has the following beneficial effects:
1) The invention realizes the electrode/electrolyte interface stability and high temperature stability of the lithium battery through the synergistic effect of various monomers and additives of the gel electrolyte.
2) Compared with the conventional gel state battery, the gel state lithium ion battery has the advantages of low price of each monomer component, no addition of an additional acid control additive and cost advantage.
3) The gel state lithium ion battery can improve the use safety and the high-temperature energy storage capacity of the battery on the premise of optimizing the electrochemical stability of an electrolyte/electrode interface.
Drawings
FIG. 1 is an activated discharge capacity and coulombic efficiency of examples 1-4 and comparative examples 1-3.
FIG. 2 is a normal temperature EIS curve.
Detailed Description
In order to facilitate understanding of the technical means, the creation characteristics, the achievement of the objects and the effects achieved by the present invention, the present invention is further described below with reference to specific examples, but the following examples are only preferred examples of the present invention, not all of which are described in detail below. Based on the examples in the embodiments, those skilled in the art can obtain other examples without making any inventive effort, which fall within the scope of the invention. The experimental methods in the following examples are conventional methods unless otherwise specified, and materials, reagents, etc. used in the following examples are commercially available unless otherwise specified.
The invention provides a gel electrolyte containing an FEC additive, a 1,3, 5-triallyl isocyanurate cross-linking agent and an acrylonitrile monomer and a battery. In the gel electrolyte, the isocyanuric acid and the acrylonitrile exist as polymer groups, and the electrochemical stability of the gel electrolyte is obviously improved compared with that of an additive; 1,3, 5-triallyl isocyanurate is used as a cross-linking agent, and mainly plays roles in improving the mechanical strength of gel and controlling acid at high temperature; acrylonitrile is used as a monomer with high dielectric constant, and plays a role in complexing with an anode transition element and improving the solid-liquid capability; the FEC additive has the effect of forming a film on the negative electrode; the synergistic effect of the three effectively improves the interface stability and the high-temperature storage stability of the lithium ion battery matched with the high-nickel ternary positive electrode.
Example 1
The gel state battery used in this example was prepared by the following method: the water content in the glove box is controlled to be not more than 10ppm, ethylene carbonate, propylene carbonate, methyl ethyl carbonate and dimethyl carbonate are fully stirred and uniformly mixed according to the mass ratio of 30/5/45/20, and the solvent component can be obtained by purifying, removing impurities and removing water through a molecular sieve.
Under the same conditions, the polymerization inhibitor is removed from the 1,3, 5-triallyl isocyanurate, the acrylonitrile and the butyl acrylate by using neutral alumina, and the monomer components are obtained by mixing according to the mass ratio of 2/9/9.
Under the same conditions, mixing the monomer, the solvent, the FEC and the lithium hexafluorophosphate according to the mass ratio of 15/67.5/5/12.5, adding the azodiisobutyronitrile with the mass fraction of 0.5% of the monomer, and stirring until the mixture is clear, thus obtaining the precursor.
LiNi is added to 0.83 Co 0.11 Mn 0.06 O 2 Dispersing conductive agent carbon fiber and binder polyvinylidene fluoride in a proper amount of N-methyl pyrrolidone according to a mass ratio of 96:2:2, and fully and uniformly stirring according to a pulping process step. Uniformly coating the uniformly dispersed positive electrode slurry on an aluminum foil, and baking, rolling, slitting and punching to obtain the positive electrode plate.
And in a glove box, assembling the positive electrode shell, the positive electrode plate, the diaphragm, the lithium plate, the foam nickel and the negative electrode plate in sequence, injecting the precursor of the embodiment, wherein the injection amount of the precursor in each battery is 60 microliters, and stamping and sealing to obtain the lithium ion button cell. And placing the button cell in a 45 ℃ oven, standing at a high temperature for 48 hours to finish curing, and obtaining the lithium ion gel state cell with the capacity of 2.04mAh per cell.
Example 2
This comparative example differs from example 1 in that the ratio of 1,3, 5-triallyl isocyanurate, acrylonitrile, butyl acrylate is 4/13/13.
Example 3
This comparative example is different from example 1 in that the ratio of 1,3, 5-triallyl isocyanurate, acrylonitrile, butyl acrylate is 0.2/15/15.
Comparative example 1
This comparative example differs from example 1 in that the 1,3, 5-triallyl isocyanurate in the monomer is replaced by the mass of 1, 5-pentanediol diacrylate.
Comparative example 2
This comparative example is different from example 1 in that the ratio of 1,3, 5-triallyl isocyanurate, acrylonitrile, butyl acrylate is 1/0/9.
Comparative example 3
This comparative example differs from example 1 in that the FEC component was replaced by an equal mass solvent.
Comparative example 4
This comparative example differs from example 1 in that the monomer in the precursor is replaced by an equal mass of solvent and no initiator is added.
The lithium ion batteries of examples 1 to 3 and comparative examples 1 to 4 were tested and compared for performance differences using the following methods. And (3) normal temperature activation test:
the lithium ion batteries of examples 1 to 3 and comparative examples 1 to 4 were charged to 4.3V at 25 ℃ with a constant current and constant voltage of 0.1C, the off current was 0.05C, and then discharged to 3V with a constant current of 0.1C, and after repeating the charge and discharge three times, the discharge capacity and coulombic efficiency of the lithium ion batteries are shown in fig. 1.
Comparative examples 1 to 3 show that when the mass fraction of 1,3, 5-triallyl isocyanurate based on the gel is too high (2%), the gel ion conductivity is suppressed, resulting in a decrease in discharge capacity; when the mass fraction is 1.5% and 0.1%, the coulomb efficiency of the battery reaches 99.5% and above, the discharge capacity reaches 95% and above of the theoretical capacity, and the performance is excellent. As is clear from comparative example 1 and comparative examples 1 to 3, the presence of isocyanurate groups is an important cause for improving the coulombic efficiency of the battery, the presence of polar nitrile groups plays an important role in promoting the dissociation of lithium salt and the promotion of the ionic conductivity of gel, and FEC additives also help to inhibit interfacial reaction and promote the formation of stable SEI films, and the three have a synergistic effect in the gel system. Comparative examples 1,3 and 4 show that the crosslinked gel having isocyanurate groups and cyano groups can effectively improve the coulombic efficiency of lithium ion batteries without significantly sacrificing the ionic conductivity, which has positive significance for improving the cycle stability of the batteries.
High temperature storage test:
the lithium ion batteries of examples 1 and 3 and comparative examples 1 and 4 were charged to 4.3V at a constant current and constant voltage of 0.1C, were subjected to EIS test at normal temperature at a cutoff current of 0.05C, were then stored in a 60 ℃ incubator, and were subjected to EIS test again at normal temperature after 7 days, and EIS results before and after storage are shown in fig. 2.
In FIG. 2, after charging to 4.3V, (a) example 1, (b) example 3, (c) comparative example 1, (d) ordinary temperature EIS curve of comparative example 4; after storage, (e) example 1, (f) example 3, (g) comparative example 1, (h) ordinary temperature EIS curve of comparative example 4.
As can be seen from fig. 2, when a sufficient amount of isocyanurate groups are present in the gel, the corresponding semi-solid battery has better high-temperature storage, which is manifested in that the battery resistance does not significantly change before and after high-temperature storage. On the contrary, when the content of the 1,3, 5-triallyl isocyanurate is low or the common acrylic ester cross-linking agent is substituted, cyano and FEC can not independently inhibit the reaction of the high-nickel ternary positive electrode and electrolyte at high temperature and high pressure, so that the high-temperature storage property of the battery is poor, and the interfacial film impedance and the charge transfer impedance are obviously improved after the high-temperature storage. And under the condition that no acid control gel exists, hydrofluoric acid generated by high-temperature decomposition of electrolyte has serious corrosion to SEI films and positive electrode substances, and the high-temperature storage capacity of the battery is worst.
While the invention has been described with respect to preferred embodiments thereof, it will be understood by those skilled in the art that various modifications and additions may be made without departing from the scope of the invention. Equivalent embodiments of the present invention will be apparent to those skilled in the art having the benefit of the teachings disclosed herein, when considered in the light of the foregoing disclosure, and without departing from the spirit and scope of the invention; meanwhile, any equivalent changes, modifications and evolution of the above embodiments according to the essential technology of the present invention still fall within the scope of the technical solution of the present invention.
Claims (10)
1. A lithium ion gel state electrolyte, comprising a polymer monomer, an organic solvent, a lithium salt, an additive and an initiator, wherein the polymer monomer at least comprises 1,3, 5-triallyl isocyanurate and acrylonitrile, and the additive at least comprises FEC;1,3, 5-triallyl isocyanurate accounts for 0.1-2% of the total mass of the lithium ion gel state electrolyte, and acrylonitrile accounts for 2.5-7.5% of the total mass of the lithium ion gel state electrolyte.
2. The lithium ion gel state electrolyte of claim 1, wherein the polymer monomer further comprises one or more of ethoxylated trimethylol propane triacrylate, pentaerythritol tetraacrylate, trimethylol propane triacrylate, trimethylol propane trimethacrylate, butyl acrylate, t-butyl acrylate, isobutyl acrylate, 1, 4-butylene dimethacrylate, vinylidene fluoride.
3. The lithium ion gel electrolyte according to claim 1, wherein the organic solvent comprises two or more of ethyl propionate, propyl acetate, ethyl acetate, methyl acetate, dimethyl carbonate, diethyl carbonate, propyl propionate, ethylene carbonate, propylene carbonate, methyl ethyl carbonate, and dipropyl carbonate.
4. The lithium ion gel state electrolyte of claim 1, wherein the lithium salt comprises one or more of lithium hexafluorophosphate, lithium perchlorate, lithium difluorooxalato borate, lithium trifluoromethane sulfonate, lithium bistrifluoromethyl sulfonyl imide, lithium bisfluoro sulfonyl imide.
5. The lithium ion gel state electrolyte of claim 1, wherein FEC comprises 5-20% of the total mass of the lithium ion gel state electrolyte, and the additive further comprises one or more of lithium difluorophosphate, lithium bisoxalato borate, vinyl sulfate, 1, 3-propenesulfonic acid lactone, and N, N-dimethyl trifluoroacetamide.
6. The lithium ion gel electrolyte of claim 1, wherein the initiator comprises one or more of azobisisobutyronitrile, azobisisoheptonitrile, dibenzoyl peroxide, diisobutyl peroxydicarbonate, dicyclohexyl peroxydicarbonate.
7. A gel state lithium ion battery comprising the lithium ion gel state electrolyte of any one of claims 1-6, a negative electrode, a positive electrode and a separator.
8. The gel state lithium ion battery of claim 7, wherein the positive electrode comprises a positive electrode active material, a conductive agent, a binder, and a current collector; the positive electrode active material comprises one or more of lithium iron phosphate, lithium manganese iron phosphate, lithium nickelate, lithium manganate, lithium cobaltate, nickel cobalt manganese ternary material and nickel cobalt aluminum ternary material.
9. The gel state lithium ion battery of claim 7, wherein the negative electrode comprises a negative electrode sheet comprising lithium metal and a current collector; or a negative electrode sheet containing an active material, a conductive agent, a binder, and a current collector; wherein the active material comprises one or more of graphite, hard carbon, soft carbon, silicon oxygen and silicon carbon.
10. A method of preparing a gel state lithium ion battery according to claim 7, comprising the steps of:
1) Controlling the water content to be less than or equal to 10ppm, and uniformly mixing the organic solvent to obtain an organic solvent component;
2) Controlling the water content to be less than or equal to 10ppm, removing the polymerization inhibitor from the polymer monomer, and uniformly mixing to obtain a polymer monomer component;
3) Controlling the water content to be less than or equal to 10ppm, mixing the polymer monomer component obtained in the step 2), the organic solvent component obtained in the step 1), the additive and the lithium salt, adding an initiator, and stirring until the mixture is clear to obtain a precursor;
4) And (3) assembling the positive electrode shell, the positive electrode plate, the diaphragm, the lithium plate, the foam nickel and the negative electrode plate in sequence, injecting the precursor obtained in the step (3), and stamping and sealing to obtain the gel-state lithium ion battery.
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