CN116706243A - Low-temperature non-combustible electrolyte for lithium battery and application thereof - Google Patents
Low-temperature non-combustible electrolyte for lithium battery and application thereof Download PDFInfo
- Publication number
- CN116706243A CN116706243A CN202310845285.8A CN202310845285A CN116706243A CN 116706243 A CN116706243 A CN 116706243A CN 202310845285 A CN202310845285 A CN 202310845285A CN 116706243 A CN116706243 A CN 116706243A
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- China
- Prior art keywords
- solvent
- lithium
- electrolyte
- low
- combustible
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- Pending
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 72
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 43
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 40
- 239000002904 solvent Substances 0.000 claims abstract description 56
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 19
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910001416 lithium ion Inorganic materials 0.000 claims abstract description 14
- 239000000654 additive Substances 0.000 claims abstract description 13
- 230000000996 additive effect Effects 0.000 claims abstract description 13
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 10
- 239000010439 graphite Substances 0.000 claims abstract description 10
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 8
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 8
- 239000003960 organic solvent Substances 0.000 claims abstract description 5
- 229910013716 LiNi Inorganic materials 0.000 claims description 9
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 8
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 claims description 7
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-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
- -1 lithium hexafluorophosphate Chemical compound 0.000 claims description 6
- 229910019142 PO4 Inorganic materials 0.000 claims description 5
- 239000007983 Tris buffer Substances 0.000 claims description 5
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 claims description 5
- 239000010452 phosphate Substances 0.000 claims description 5
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 5
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 5
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-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
- LOZAIRWAADCOHQ-UHFFFAOYSA-N triphosphazene Chemical compound PNP=NP LOZAIRWAADCOHQ-UHFFFAOYSA-N 0.000 claims description 4
- ZPFAVCIQZKRBGF-UHFFFAOYSA-N 1,3,2-dioxathiolane 2,2-dioxide Chemical compound O=S1(=O)OCCO1 ZPFAVCIQZKRBGF-UHFFFAOYSA-N 0.000 claims description 3
- DSMUTQTWFHVVGQ-UHFFFAOYSA-N 4,5-difluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1F DSMUTQTWFHVVGQ-UHFFFAOYSA-N 0.000 claims description 3
- 229910010707 LiFePO 4 Inorganic materials 0.000 claims description 3
- 229910002995 LiNi0.8Co0.15Al0.05O2 Inorganic materials 0.000 claims description 3
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 3
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 2
- YEVQZPWSVWZAOB-UHFFFAOYSA-N 2-(bromomethyl)-1-iodo-4-(trifluoromethyl)benzene Chemical compound FC(F)(F)C1=CC=C(I)C(CBr)=C1 YEVQZPWSVWZAOB-UHFFFAOYSA-N 0.000 claims description 2
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 2
- DKPFZGUDAPQIHT-UHFFFAOYSA-N Butyl acetate Natural products CCCCOC(C)=O DKPFZGUDAPQIHT-UHFFFAOYSA-N 0.000 claims description 2
- 229910012851 LiCoO 2 Inorganic materials 0.000 claims description 2
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 2
- YSMRWXYRXBRSND-UHFFFAOYSA-N TOTP Chemical compound CC1=CC=CC=C1OP(=O)(OC=1C(=CC=CC=1)C)OC1=CC=CC=C1C YSMRWXYRXBRSND-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
- 125000001301 ethoxy group Chemical group [H]C([H])([H])C([H])([H])O* 0.000 claims description 2
- GZKHDVAKKLTJPO-UHFFFAOYSA-N ethyl 2,2-difluoroacetate Chemical compound CCOC(=O)C(F)F GZKHDVAKKLTJPO-UHFFFAOYSA-N 0.000 claims description 2
- IRSJDVYTJUCXRV-UHFFFAOYSA-N ethyl 2-bromo-2,2-difluoroacetate Chemical compound CCOC(=O)C(F)(F)Br IRSJDVYTJUCXRV-UHFFFAOYSA-N 0.000 claims description 2
- GVCAWQUJCHZRCB-UHFFFAOYSA-N ethyl 2-chloro-2,2-difluoroacetate Chemical compound CCOC(=O)C(F)(F)Cl GVCAWQUJCHZRCB-UHFFFAOYSA-N 0.000 claims description 2
- FTKASJMIPSSXBP-UHFFFAOYSA-N ethyl 2-nitroacetate Chemical compound CCOC(=O)C[N+]([O-])=O FTKASJMIPSSXBP-UHFFFAOYSA-N 0.000 claims description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 2
- FUZZWVXGSFPDMH-UHFFFAOYSA-N hexanoic acid Chemical compound CCCCCC(O)=O FUZZWVXGSFPDMH-UHFFFAOYSA-N 0.000 claims description 2
- DEUISMFZZMAAOJ-UHFFFAOYSA-N lithium dihydrogen borate oxalic acid Chemical compound B([O-])(O)O.C(C(=O)O)(=O)O.C(C(=O)O)(=O)O.[Li+] DEUISMFZZMAAOJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate 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
- 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
- 125000000951 phenoxy group Chemical group [H]C1=C([H])C([H])=C(O*)C([H])=C1[H] 0.000 claims description 2
- 239000007774 positive electrode material Substances 0.000 claims description 2
- 229940090181 propyl acetate Drugs 0.000 claims description 2
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 claims description 2
- SFENPMLASUEABX-UHFFFAOYSA-N trihexyl phosphate Chemical compound CCCCCCOP(=O)(OCCCCCC)OCCCCCC SFENPMLASUEABX-UHFFFAOYSA-N 0.000 claims description 2
- QJAVUVZBMMXBRO-UHFFFAOYSA-N tripentyl phosphate Chemical compound CCCCCOP(=O)(OCCCCC)OCCCCC QJAVUVZBMMXBRO-UHFFFAOYSA-N 0.000 claims description 2
- XZZNDPSIHUTMOC-UHFFFAOYSA-N triphenyl phosphate Chemical compound C=1C=CC=CC=1OP(OC=1C=CC=CC=1)(=O)OC1=CC=CC=C1 XZZNDPSIHUTMOC-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
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 claims 1
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 claims 1
- 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 1
- 229910052799 carbon Inorganic materials 0.000 abstract description 5
- 238000004807 desolvation Methods 0.000 abstract description 4
- 230000004888 barrier function Effects 0.000 abstract 1
- 229910052710 silicon Inorganic materials 0.000 abstract 1
- 239000010703 silicon Substances 0.000 abstract 1
- 230000000052 comparative effect Effects 0.000 description 12
- 238000012360 testing method Methods 0.000 description 9
- 238000011056 performance test Methods 0.000 description 8
- 238000003756 stirring Methods 0.000 description 8
- 229910052782 aluminium Inorganic materials 0.000 description 7
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 7
- 239000001768 carboxy methyl cellulose Substances 0.000 description 6
- 239000011888 foil Substances 0.000 description 6
- 239000002033 PVDF binder Substances 0.000 description 5
- 239000007788 liquid Substances 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 4
- 239000012300 argon atmosphere Substances 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 4
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- 239000013538 functional additive Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 239000001301 oxygen Substances 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 4
- 238000007789 sealing Methods 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 3
- 229910010710 LiFePO Inorganic materials 0.000 description 3
- SYRDSFGUUQPYOB-UHFFFAOYSA-N [Li+].[Li+].[Li+].[O-]B([O-])[O-].FC(=O)C(F)=O Chemical compound [Li+].[Li+].[Li+].[O-]B([O-])[O-].FC(=O)C(F)=O SYRDSFGUUQPYOB-UHFFFAOYSA-N 0.000 description 3
- 239000006230 acetylene black Substances 0.000 description 3
- 229910021383 artificial graphite Inorganic materials 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 3
- 239000011230 binding agent Substances 0.000 description 3
- 239000011889 copper foil Substances 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 229920003048 styrene butadiene rubber Polymers 0.000 description 3
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 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 2
- 239000011149 active material Substances 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 238000009835 boiling Methods 0.000 description 2
- 150000005678 chain carbonates Chemical class 0.000 description 2
- 230000001351 cycling effect Effects 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 238000007710 freezing Methods 0.000 description 2
- 230000008014 freezing Effects 0.000 description 2
- 239000003365 glass fiber Substances 0.000 description 2
- 238000002347 injection Methods 0.000 description 2
- 239000007924 injection Substances 0.000 description 2
- 239000012046 mixed solvent Substances 0.000 description 2
- 238000004806 packaging method and process Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 238000004080 punching Methods 0.000 description 2
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 2
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 238000007614 solvation Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- DEBZEVJNWCNATM-UHFFFAOYSA-N 2,2,4,4,6,6-hexamethyl-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound CP1(C)=NP(C)(C)=NP(C)(C)=N1 DEBZEVJNWCNATM-UHFFFAOYSA-N 0.000 description 1
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$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 description 1
- WTFUTSCZYYCBAY-SXBRIOAWSA-N 6-[(E)-C-[[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]methyl]-N-hydroxycarbonimidoyl]-3H-1,3-benzoxazol-2-one Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)C/C(=N/O)/C1=CC2=C(NC(O2)=O)C=C1 WTFUTSCZYYCBAY-SXBRIOAWSA-N 0.000 description 1
- 229910012820 LiCoO Inorganic materials 0.000 description 1
- 229910015872 LiNi0.8Co0.1Mn0.1O2 Inorganic materials 0.000 description 1
- 239000002174 Styrene-butadiene Substances 0.000 description 1
- 230000005856 abnormality Effects 0.000 description 1
- 239000013543 active substance Substances 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- PMGNOQUKCGLETL-UHFFFAOYSA-N carbonic acid 1,2-difluoroethene Chemical compound C(O)(O)=O.FC=CF PMGNOQUKCGLETL-UHFFFAOYSA-N 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000008151 electrolyte solution Substances 0.000 description 1
- 229940021013 electrolyte solution Drugs 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 description 1
- 230000001747 exhibiting effect Effects 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 238000009830 intercalation Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000011812 mixed powder Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000004570 mortar (masonry) Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 239000002985 plastic film Substances 0.000 description 1
- 229920006255 plastic film Polymers 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000009517 secondary packaging Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
- 238000004804 winding Methods 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
- H01M10/0569—Liquid materials characterised by the solvents
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—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
- H01M10/058—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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
- H01M2300/0028—Organic electrolyte characterised by the solvent
- H01M2300/0037—Mixture of solvents
- H01M2300/004—Three 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
Landscapes
- 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)
- Secondary Cells (AREA)
Abstract
The invention provides a low-temperature non-combustible electrolyte of a lithium battery, which comprises an organic solvent, lithium salt and an additive, and is characterized in that the organic solvent comprises a solvent A, a solvent B and a solvent C, wherein the solvent A is a solvent with higher dielectric constant, moderate donor number and lower solidifying point, the solvent B is a solvent with intrinsic non-combustible property, the solvent C is a chain solvent with higher affinity with lithium ions and low solidifying point and low viscosity, and the additive is a film forming additive. The lithium battery low-temperature non-combustible electrolyte provided by the invention has good electrochemical compatibility with a graphite/silicon carbon/metallic lithium negative electrode, high low-temperature conductivity, low lithium ion desolvation energy barrier and flame retardance, can greatly improve the low-temperature applicability of the lithium ion battery, and fundamentally solves the potential safety hazard of the battery.
Description
Technical Field
The invention relates to a lithium battery electrolyte, in particular to a lithium battery low-temperature non-combustible electrolyte and application thereof.
Background
The lithium battery becomes the most advanced chemical power system at present due to the advantages of high output voltage, high energy density, long cycle life, zero self discharge and the like, occupies the main markets of portable electronic product power supplies and electric automobile power supplies, and gradually permeates into the field of electric power energy storage. However, there are still two challenges to be addressed by lithium batteries. The first is that intrinsic safety is not high, mainly because lithium battery electrolytes use low flash point, low boiling point chain carbonate solvents, resulting in serious deterioration of safety. Meanwhile, in order to further pursue high energy density, high-capacity electrode materials (a high-nickel ternary positive electrode, a high-voltage lithium cobaltate positive electrode, a silicon carbon negative electrode, a lithium negative electrode and the like) are adopted in the battery, and the materials are poor in thermal stability, so that potential safety hazards of the battery are further increased. Second, the low temperature performance is poor, mainly due to the use of Ethylene Carbonate (EC) in the electrolyte. Although EC contributes to the formation of an SEI film on the surface of a negative electrode, its freezing point is as high as 36.4 ℃, the viscosity of an electrolyte at low temperature is remarkably increased, and the conductivity is rapidly reduced, resulting in the failure of normal operation of a battery.
Propylene Carbonate (PC), trimethyl phosphate (TMP) and other solvents have the characteristics of higher dielectric constant, low cost, low solidifying point and the like, but are completely incompatible with the conventional battery cathodes (graphite cathodes and silicon carbon cathodes), and have serious co-intercalation phenomenon during discharge. Although studies have been conducted to confirm that the electrochemical compatibility of PC with the above-described anode can be effectively improved by the design of a high concentration electrolyte or a high molar ratio electrolyte, the problems of high viscosity and high cost and the like at the same time make it difficult to apply such electrolytes on a large scale.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a low-temperature non-combustible electrolyte for a lithium battery and application thereof.
The invention provides the following technical scheme:
the invention provides a low-temperature non-combustible electrolyte of a lithium battery, which comprises an organic solvent, lithium salt and an additive, wherein the solvent A is a solvent with higher dielectric constant, moderate donor number and lower solidifying point, the solvent B is a solvent with intrinsic non-combustible property, the solvent C is a chain solvent with higher affinity with lithium ions and low solidifying point and low viscosity, and the additive is a film forming additive.
The solvent A with high dielectric constant has good lithium salt solubility, can provide high conductivity at normal temperature/low temperature for electrolyte, and meanwhile, the moderate donor number also enables the combination energy between lithium ions and the solvent A to be lower, thereby being beneficial to improving the dynamic performance of the lithium ions at low temperature; the solvent B has the characteristic of intrinsic incombustibility, and can effectively improve the safety of electrolyte and batteries; the solvent C has the property of low freezing point and low viscosity, so that the viscosity and the conductivity of the electrolyte can be effectively improved, the desolvation speed of lithium ions can be effectively improved after the solvent C is introduced, the interface property of the negative electrode is optimized, the diffusion kinetics of the lithium ions is improved, and the cycling stability of the negative electrode is effectively improved. The obtained A-B-C ternary electrolyte has good ionic conductivity in a wider liquid range, can effectively improve the intrinsic safety of the battery, and also endows the battery with the capability of discharging at extremely low temperature (below-40 ℃).
Further, the content of the solvent A accounts for 10-30% of the total mass of the electrolyte, the content of the solvent B accounts for 20-50% of the total mass of the electrolyte, the content of the solvent C accounts for 10-50% of the total mass of the electrolyte, the content of the lithium salt accounts for 5-20% of the total mass of the electrolyte, and the content of the additive accounts for 0.1-5% of the total mass of the electrolyte.
Further, the solvent A is one or more of propylene carbonate, trimethyl phosphate, N-dimethylformamide and ethylene glycol dimethyl ether.
Further, the solvent B is one or more of ethoxy pentafluoroethylene triphosphazene, phenoxy pentafluoroethylene triphosphazene, hexamethyl cyclotriphosphazene, tributyl phosphate, tripentyl phosphate, trihexyl phosphate, trioctyl phosphate, triphenyl phosphate, tricresyl phosphate and tris (2, 2-trifluoroethyl) phosphate.
Further, the solvent C is one or more of diethyl carbonate, methyl ethyl carbonate, 2-trifluoroethyl methyl carbonate, methyl formate, methyl acetate, ethyl acetate, propyl acetate, butyl acetate, ethyl difluoroacetate, ethyl difluorochloroacetate, ethyl difluorobromoacetate and ethyl 2-nitroacetate.
Further, the lithium salt is one or more of lithium hexafluorophosphate, lithium dioxalate borate, lithium bistrifluoromethane sulfonyl imide, lithium perchlorate, lithium difluorooxalate borate, lithium nitrate and lithium triflate.
Further, the additive is one or more of fluoroethylene carbonate, 1, 2-difluoroethylene carbonate, ethylene sulfate, 4-methyl ethylene sulfate, 4-ethyl ethylene sulfate, 1, 3-dioxol-2-one, lithium difluorophosphate, lithium tetrafluoroborate, lithium bisoxalato borate and lithium difluorooxalato borate.
The invention also provides a low-temperature high-safety lithium battery, which comprises a positive electrode, a negative electrode and the non-combustible electrolyte.
Further, the positive electrode active material is LiFePO 4 、LiCoO 2 、LiNi 0.8 Co 0.15 Al 0.05 O 2 、LiNi 0.5～ 0.9 Co 0.05～0.2 Mn 0.05～0.3 O 2 One or more of the following; the negative electrode is one or more of graphite, a silicon-carbon negative electrode and lithium metal.
The invention has the following beneficial effects:
1. according to the invention, through the optimal collocation of three functional solvents, an electrolyte system with a wider liquid range and superior ion conductivity is realized;
2. the lithium battery electrolyte prepared by the invention can effectively improve the intrinsic safety of the battery and also endow the battery with the capability of discharging at low temperature (less than-40 ℃)
3. The lithium battery electrolyte designed by the invention has simple components, stability and adjustability and low cost, and can be popularized and applied on a large scale.
Drawings
In order to more clearly illustrate the embodiments of the invention or the technical solutions in the prior art, the drawings that are required in the embodiments or the description of the prior art will be briefly described, it being obvious that the drawings in the following description are only some embodiments of the invention, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a graph showing the initial charge-discharge curve (current density 25mA g) of a graphite half cell using the electrolytes of examples 1 to 3 according to the present invention -1 )；
FIG. 2 is a graph showing the results of the cycle performance test of the batteries of the electrolytes of example 1 and example 3 in the present invention;
FIG. 3 is a graph showing the results of the conductivity tests of the electrolytes of example 1, example 3 and comparative example 1 according to the present invention at different temperatures;
FIG. 4 is a graph of the results of an ignition test of glass fiber separators impregnated with comparative example 1 and example 4;
FIG. 5 is a view showing Li LiNi of the electrolyte of example 4 used in the present invention 0.8 Mn 0.1 Co 0.1 O 2 A cycle performance test result diagram of the lithium battery;
FIG. 6 is a Li LiFePO using the electrolyte of example 5 in the present invention 4 A cycle performance test result diagram of the lithium battery;
FIG. 7 shows 4Ah graphite LiNi using the electrolyte of example 3 in the present invention 0.8 Mn 0.1 Co 0.1 O 2 A graph of the cycle performance test results of the pouch cell at a current density of 0.5C/1C (1c=4a);
FIG. 8 is a graph of 4Ah graphite LiNi using the electrolytes of comparative example 1 and example 3 in the present invention 0.8 Mn 0.1 Co 0.1 O 2 A low-temperature test result diagram of the soft package battery;
fig. 9 is a graph of a needling test of a pouch cell using the electrolytes of comparative example 1 and example 3 in the present invention;
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
Example 1
In an argon atmosphere glove box with the oxygen content and the moisture content being lower than 0.1ppm, dissolving lithium bistrifluoromethane sulfonyl imide in a mass ratio of 1:3:0 trimethyl phosphate/tris (2, 2-trifluoroethyl) phosphate/diethyl carbonate, wherein the mass of lithium bistrifluoromethane sulfonyl imide is 0.94g, the total mass of the solvent is 6g, and 0.05g of functional additive vinyl sulfate is added to obtain 5mL of electrolyte of example 1, magnetically stirring is carried out for 1 hour, and the electrolyte is placed in a glove box in a sealing manner and protected from light for standby.
Example 2
Unlike example 1, the mass ratio of trimethyl phosphate/tris (2, 2-trifluoroethyl) phosphate/diethyl carbonate mixed solvent was 1:2:1.
Example 3
Unlike example 1, the mass ratio of trimethyl phosphate/tris (2, 2-trifluoroethyl) phosphate/diethyl carbonate mixed solvent was 1:1:1.
Example 4
In an argon atmosphere glove box with the oxygen content and the water content being lower than 0.1ppm, dissolving lithium difluoro oxalato borate in a mass ratio of 1:1:1, wherein the lithium difluorooxalate borate has the mass of 0.72g and the total mass of the solvent is 7.5g, and 0.12g of the functional additive 1, 2-difluoroethylene carbonate and 0.05g of the functional additive ethylene sulfate are added to obtain 5mL of the electrolyte of the example 4, magnetically stirring for 1 hour, sealing and placing in a glove box for standby in a dark place.
Example 5
In an argon atmosphere glove box with oxygen content and moisture content lower than 0.1ppm, dissolving lithium perchlorate in a mass ratio of 1:1:1, wherein the mass of lithium difluorooxalate borate is 0.72g, the total mass of the solvent is 6g, and 0.12g of functional additive 1, 2-difluoro ethylene carbonate is added to obtain 5mL of electrolyte of example 9, magnetically stirring is carried out for 1 hour, and the electrolyte is placed in a glove box in a sealing manner for standby in a dark place.
Comparative example 1
Preparing common commercial lithium battery electrolyte: in an argon atmosphere glove box with oxygen content and moisture content lower than 0.1ppm, dissolving lithium hexafluorophosphate in a mass ratio of 1:1, wherein the mass of lithium hexafluorophosphate is 0.76g and the total mass of the solvent is 6g, to obtain 5mL of electrolyte of comparative example 2, magnetically stirring for 1 hour, sealing and placing in a glove box for standby in a dark place.
And (3) carrying out electrochemical performance test on the electrolyte prepared by the method:
the process of manufacturing the button cell and the soft package cell is as follows:
button cell: the positive pole piece is made of LiFePO 4 Powder (or LiCoO) 2 、LiNi 0.8 Co 0.15 Al 0.05 O 2 、LiNi 0.5～ 0.9 Co 0.05～0.2 Mn 0.05～0.3 O 2 ) The active material comprises acetylene black conductive carbon (AB) and PVDF binder, wherein the AB is PVDF=90:5:5. LiFePO is prepared 4 Grinding the powder and AB in a mortar according to a certain proportion for 20min, mixing the uniformly mixed powder with PVDF (5% NMP solution), placing the mixture on a miniature ball mill, stirring for 20min to obtain uniform slurry, uniformly coating the slurry on aluminum foil, drying the aluminum foil in an oven at 80 ℃ in vacuum for 10h, extruding a positive pole piece with a diameter of 12mm by using a punch, and weighing the positive pole piece for later use;
the negative electrode plate consists of artificial graphite (or silicon carbon), super P conductive carbon, styrene Butadiene Rubber (SBR) and sodium carboxymethyl cellulose (CMC) binder, wherein the active material is Super P SBR, CMC=85:6:4.5:4.5. Uniformly mixing artificial graphite powder and Super P conductive carbon in proportion for 20min, mixing the uniformly mixed artificial graphite and Super P conductive carbon with SBR (49.5% aqueous solution) and CMC (2% aqueous solution), placing the mixture on a miniature ball mill, stirring for 15min to obtain uniform slurry, uniformly coating the slurry on copper foil, vacuum drying the copper foil in an oven at 80 ℃ for 5h, punching a negative electrode plate with the diameter of 12mm by using a punching machine, and weighing the negative electrode plate for later use.
Soft package battery: the positive pole piece is made of LiNi 0.8 Co 0.1 Mn 0.1 O 2 Active substance and guideThe electrical agent acetylene black and the binder polyvinylidene fluoride (PVDF) are prepared according to the mass ratio of 97:1.5:1.5 fully stirring and uniformly mixing the mixture in an N-methyl pyrrolidone solvent system, coating the mixture on an aluminum foil, drying the aluminum foil, and cold pressing the aluminum foil to obtain the aluminum foil. The negative electrode plate is prepared from graphite, a conductive agent acetylene black, a binder Styrene Butadiene Rubber (SBR) and a thickener sodium carboxymethyl cellulose (CMC) according to the mass ratio of 96:1:1.5:1.5, 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 to obtain the negative plate. And sequentially laminating the positive plate, the isolating film and the negative plate, winding in the same direction to obtain a bare cell, packaging by adopting an aluminum plastic film, and packaging, standing, forming, aging, secondary packaging, capacity division and other working procedures of the battery after liquid injection to obtain the soft package lithium battery. Wherein the surface density of the positive electrode and the negative electrode is 21.2mg cm respectively -2 36mg cm -2 The injection amount was 10g.
The results obtained were analyzed as follows:
FIG. 1 is a first cycle charge-discharge curve of batteries with different diethyl carbonate contents, wherein as the diethyl carbonate content is increased, the first coulombic efficiency and reversible specific capacity of the batteries are improved to a certain extent;
FIG. 2 is a graph showing the results of cycle performance testing of the cells of the electrolytes of examples 1 and 3, wherein the spontaneously formed low desolvation solvation structure substantially enhanced the rate capability and cycle performance of the cells after the introduction of the low coordination lithium ion reagent diethyl carbonate;
FIG. 3 is a graph showing the results of the conductivity tests of the electrolyte solutions of example 1, example 3 and comparative example 1 at different temperatures, and it can be seen that example 3 has a wide liquid range (0-60 ℃ C.) and excellent low-temperature conductivity.
FIG. 4 is an ignition test result of the glass fiber separator impregnated with comparative example 1 and example 4, and it is apparent that the separator of comparative example 1 is rapidly ignited, whereas the separator of example 4 is completely non-flammable, exhibiting a good flame retardant effect;
FIG. 5 is Li LiNi using the electrolyte of example 4 0.8 Mn 0.1 Co 0.1 O 2 The cycle performance test result of the lithium battery shows that the capacity retention rate is still more than 90% after 400 weeks of cycle;
FIG. 6 is Li LiFePO using the electrolyte of example 5 4 The cycle performance test result of the lithium battery shows that the electrolyte of the embodiment 5 and the lithium iron phosphate positive electrode show excellent compatibility;
FIG. 7 is a 4Ah graphite LiNi using the electrolyte of example 3 0.8 Mn 0.1 Co 0.1 O 2 The cycle performance test result of the soft-packed battery at the current density of 0.5C/1C (1 C=4A) shows that the 400-week cycle retention rate of the soft-packed battery is 94.1%, and the soft-packed battery has excellent electrochemical stability;
FIG. 8 is 4Ah graphite LiNi using the electrolytes of comparative example 1 and example 3 0.8 Mn 0.1 Co 0.1 O 2 The low temperature test result of the soft pack battery shows that the soft pack battery using the electrolyte of example 3 has a capacity retention rate of up to 79% at-40 ℃ and excellent low temperature performance.
Fig. 9 is a needling test of the pouch cells of the electrolytes of comparative example 1 and example 3, the pouch cell using the electrolyte of comparative example 1 was rapidly exploded by fire, and the cell using the electrolyte of example 3 was free from any abnormality, showing excellent safety.
In summary, the electrolyte provided by the invention designs a low-temperature non-combustible electrolyte of a lithium battery through the combination and collocation of three functional solvents, and solves the problems that the electrolyte of the lithium battery in the prior art has low safety due to the use of a chain carbonate solvent with a low flash point and a low boiling point, the low-temperature performance is poor, the viscosity of the electrolyte is obviously increased and the conductivity is rapidly reduced at a low temperature, so that the battery cannot work normally.
The low-melting-point high-dielectric-constant solvent A ensures good ionic conductivity of the electrolyte in a wider liquid range, and the moderate donor number also ensures that the combination energy between lithium ions and the solvent A is lower, thereby being beneficial to improving the dynamic performance of the lithium ions at low temperature and endowing the battery with the capability of discharging at extremely low temperature (< -40 ℃). The solvent C has the property of low solidifying point and low viscosity, so that the viscosity and the conductivity of the electrolyte can be effectively improved, meanwhile, a self-adaptive double-layer solvation structure with lower desolvation energy can be constructed based on the property of the solvent C and lithium ions, the interface property of the negative electrode is optimized, the diffusion kinetics of lithium ions is improved, and the cycling stability of the negative electrode is effectively improved.
The foregoing description of the preferred embodiments of the invention is not intended to be limiting, but rather is intended to cover all modifications, equivalents, alternatives, and improvements that fall within the spirit and scope of the invention.
Claims (9)
1. The low-temperature non-combustible electrolyte for the lithium battery comprises an organic solvent, lithium salt and an additive, and is characterized in that the organic solvent comprises a solvent A, a solvent B and a solvent C, wherein the solvent A is a solvent with higher dielectric constant, moderate donor number and lower solidifying point, the solvent B is a solvent with intrinsic non-combustible property, the solvent C is a chain solvent with higher affinity with lithium ions and low solidifying point and low viscosity, and the additive is a film forming additive.
2. The lithium battery low temperature non-combustible electrolyte of claim 1, wherein: the content of the solvent A accounts for 10-30% of the total mass of the electrolyte, the content of the solvent B accounts for 20-50% of the total mass of the electrolyte, the content of the solvent C accounts for 10-50% of the total mass of the electrolyte, the content of the lithium salt accounts for 5-20% of the total mass of the electrolyte, and the content of the additive accounts for 0.1-5% of the total mass of the electrolyte.
3. The lithium battery low temperature non-combustible electrolyte of claim 1, wherein: the solvent A is one or more of propylene carbonate, trimethyl phosphate, N-dimethylformamide and ethylene glycol dimethyl ether.
4. The lithium battery low temperature non-combustible electrolyte of claim 1, wherein: the solvent B is one or more of ethoxy pentafluoroethylene triphosphazene, phenoxy pentafluoroethylene triphosphazene, tributyl phosphate, tripentyl phosphate, trihexyl phosphate, trioctyl phosphate, triphenyl phosphate, tricresyl phosphate and tris (2, 2-trifluoroethyl) phosphate.
5. The lithium battery low temperature non-combustible electrolyte of claim 1, wherein: the solvent C is one or more of diethyl carbonate, methyl ethyl carbonate, 2-trifluoroethyl methyl carbonate, methyl formate, methyl acetate, ethyl acetate, propyl acetate, butyl acetate, ethyl difluoroacetate, ethyl difluorochloroacetate, ethyl difluorobromoacetate and ethyl 2-nitroacetate.
6. The lithium battery low temperature non-combustible electrolyte of claim 1, wherein: the lithium salt is one or more of lithium hexafluorophosphate, lithium dioxalate borate, lithium bis (trifluoromethanesulfonyl) imide, lithium bis (fluorosulfonyl) imide, lithium perchlorate, lithium difluorooxalato borate, lithium nitrate and lithium trifluoromethanesulfonate.
7. The lithium battery low temperature non-combustible electrolyte of claim 1, wherein: the additive is one or more of fluoroethylene carbonate, 1, 2-difluoroethylene carbonate, ethylene sulfate, 4-methyl ethylene sulfate, 4-ethyl ethylene sulfate, 1, 3-dioxol-2-one, lithium difluorophosphate, lithium tetrafluoroborate, lithium bisoxalato borate and lithium difluorooxalato borate.
8. The utility model provides a low temperature high security lithium cell which characterized in that: comprising a positive electrode, a negative electrode and the lithium battery low-temperature non-combustible electrolyte of any one of claims 1 to 7.
9. The low temperature high safety lithium battery according to claim 8, wherein: the positive electrode active material is LiFePO 4 、LiCoO 2 、LiNi 0.8 Co 0.15 Al 0.05 O 2 、LiNi 0.5～0.9 Co 0.05～0.2 Mn 0.05～0.3 O 2 One or more of the following; the negative electrode is one or more of graphite negative electrode, silicon-carbon negative electrode and lithium metal.
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