CN106450432A - High-voltage lithium-ion battery with Si/C composite anode - Google Patents
High-voltage lithium-ion battery with Si/C composite anode Download PDFInfo
- Publication number
- CN106450432A CN106450432A CN201610962873.XA CN201610962873A CN106450432A CN 106450432 A CN106450432 A CN 106450432A CN 201610962873 A CN201610962873 A CN 201610962873A CN 106450432 A CN106450432 A CN 106450432A
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- China
- Prior art keywords
- silicon
- lithium
- lithium ion
- ion batteries
- carbon composite
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- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 37
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 36
- 239000002131 composite material Substances 0.000 title abstract 2
- 239000000654 additive Substances 0.000 claims abstract description 20
- 230000000996 additive effect Effects 0.000 claims abstract description 20
- 239000013543 active substance Substances 0.000 claims abstract description 8
- 239000000919 ceramic Substances 0.000 claims abstract description 8
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 8
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 7
- 229910021437 lithium-transition metal oxide Inorganic materials 0.000 claims abstract description 5
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical class O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 15
- 239000002153 silicon-carbon composite material Substances 0.000 claims description 15
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 14
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 claims description 14
- 239000008151 electrolyte solution Substances 0.000 claims description 14
- 229910052744 lithium Inorganic materials 0.000 claims description 14
- 239000000463 material Substances 0.000 claims description 12
- 230000004888 barrier function Effects 0.000 claims description 10
- -1 Cyanurate compound Chemical class 0.000 claims description 9
- 239000002253 acid Substances 0.000 claims description 7
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 6
- 229910052710 silicon Inorganic materials 0.000 claims description 6
- QGHDLJAZIIFENW-UHFFFAOYSA-N 4-[1,1,1,3,3,3-hexafluoro-2-(4-hydroxy-3-prop-2-enylphenyl)propan-2-yl]-2-prop-2-enylphenol Chemical group C1=C(CC=C)C(O)=CC=C1C(C(F)(F)F)(C(F)(F)F)C1=CC=C(O)C(CC=C)=C1 QGHDLJAZIIFENW-UHFFFAOYSA-N 0.000 claims description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 5
- 229910019142 PO4 Inorganic materials 0.000 claims description 5
- 150000001875 compounds Chemical class 0.000 claims description 5
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 5
- 239000010452 phosphate Substances 0.000 claims description 5
- IFDLFCDWOFLKEB-UHFFFAOYSA-N 2-methylbutylbenzene Chemical compound CCC(C)CC1=CC=CC=C1 IFDLFCDWOFLKEB-UHFFFAOYSA-N 0.000 claims description 4
- 150000002148 esters Chemical class 0.000 claims description 4
- VEWLDLAARDMXSB-UHFFFAOYSA-N ethenyl sulfate;hydron Chemical compound OS(=O)(=O)OC=C VEWLDLAARDMXSB-UHFFFAOYSA-N 0.000 claims description 4
- OBNCKNCVKJNDBV-UHFFFAOYSA-N ethyl butyrate Chemical compound CCCC(=O)OCC OBNCKNCVKJNDBV-UHFFFAOYSA-N 0.000 claims description 4
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 4
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 claims description 4
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 claims description 3
- 239000002033 PVDF binder Substances 0.000 claims description 3
- 229910052782 aluminium Inorganic materials 0.000 claims description 3
- JKJWYKGYGWOAHT-UHFFFAOYSA-N bis(prop-2-enyl) carbonate Chemical compound C=CCOC(=O)OCC=C JKJWYKGYGWOAHT-UHFFFAOYSA-N 0.000 claims description 3
- 238000005868 electrolysis reaction Methods 0.000 claims description 3
- GAEKPEKOJKCEMS-UHFFFAOYSA-N gamma-valerolactone Chemical compound CC1CCC(=O)O1 GAEKPEKOJKCEMS-UHFFFAOYSA-N 0.000 claims description 3
- 239000010439 graphite Substances 0.000 claims description 3
- 229910002804 graphite Inorganic materials 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- MHYFEEDKONKGEB-UHFFFAOYSA-N oxathiane 2,2-dioxide Chemical compound O=S1(=O)CCCCO1 MHYFEEDKONKGEB-UHFFFAOYSA-N 0.000 claims description 3
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 3
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 2
- ANLVEXKNRYNLDH-UHFFFAOYSA-N 1,3-dioxonan-2-one Chemical compound O=C1OCCCCCCO1 ANLVEXKNRYNLDH-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
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 2
- JGFBQFKZKSSODQ-UHFFFAOYSA-N Isothiocyanatocyclopropane Chemical compound S=C=NC1CC1 JGFBQFKZKSSODQ-UHFFFAOYSA-N 0.000 claims description 2
- RJUFJBKOKNCXHH-UHFFFAOYSA-N Methyl propionate Chemical compound CCC(=O)OC RJUFJBKOKNCXHH-UHFFFAOYSA-N 0.000 claims description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-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
- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 claims description 2
- 229910052791 calcium Inorganic materials 0.000 claims description 2
- 229910052799 carbon Inorganic materials 0.000 claims description 2
- 239000011248 coating agent Substances 0.000 claims description 2
- 238000000576 coating method Methods 0.000 claims description 2
- 230000009977 dual effect Effects 0.000 claims description 2
- 229940093499 ethyl acetate Drugs 0.000 claims description 2
- 150000002466 imines Chemical class 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
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 2
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- 229910052749 magnesium Inorganic materials 0.000 claims description 2
- 229940017219 methyl propionate Drugs 0.000 claims description 2
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 2
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 claims description 2
- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 claims description 2
- 239000005543 nano-size silicon particle Substances 0.000 claims description 2
- 229940090181 propyl acetate Drugs 0.000 claims description 2
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 2
- 229910052719 titanium Inorganic materials 0.000 claims description 2
- 125000004417 unsaturated alkyl group Chemical group 0.000 claims description 2
- QVTVDJWJGGEOGX-UHFFFAOYSA-N urea;cyanide Chemical compound N#[C-].NC(N)=O QVTVDJWJGGEOGX-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
- 229910052725 zinc Inorganic materials 0.000 claims description 2
- 229910052726 zirconium Inorganic materials 0.000 claims description 2
- 239000007864 aqueous solution Substances 0.000 claims 2
- 239000007788 liquid Substances 0.000 claims 2
- VKEQBMCRQDSRET-UHFFFAOYSA-N Methylone Chemical compound CNC(C)C(=O)C1=CC=C2OCOC2=C1 VKEQBMCRQDSRET-UHFFFAOYSA-N 0.000 claims 1
- XTXRWKRVRITETP-UHFFFAOYSA-N Vinyl acetate Chemical compound CC(=O)OC=C XTXRWKRVRITETP-UHFFFAOYSA-N 0.000 claims 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims 1
- ABDBNWQRPYOPDF-UHFFFAOYSA-N carbonofluoridic acid Chemical compound OC(F)=O ABDBNWQRPYOPDF-UHFFFAOYSA-N 0.000 claims 1
- 229910052593 corundum Inorganic materials 0.000 claims 1
- 229910052731 fluorine Inorganic materials 0.000 claims 1
- 239000011737 fluorine Substances 0.000 claims 1
- 150000002825 nitriles Chemical class 0.000 claims 1
- 229910001845 yogo sapphire Inorganic materials 0.000 claims 1
- PAPBSGBWRJIAAV-UHFFFAOYSA-N ε-Caprolactone Chemical compound O=C1CCCCCO1 PAPBSGBWRJIAAV-UHFFFAOYSA-N 0.000 claims 1
- 239000003792 electrolyte Substances 0.000 abstract description 14
- 238000003860 storage Methods 0.000 abstract description 14
- 238000000034 method Methods 0.000 abstract description 6
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 abstract description 3
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical class OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 abstract description 2
- 239000000126 substance Substances 0.000 abstract description 2
- 239000011255 nonaqueous electrolyte Substances 0.000 abstract 2
- 238000002360 preparation method Methods 0.000 description 12
- 230000004087 circulation Effects 0.000 description 11
- 230000000052 comparative effect Effects 0.000 description 11
- 125000004122 cyclic group Chemical group 0.000 description 10
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 description 5
- 229910017052 cobalt Inorganic materials 0.000 description 5
- 239000010941 cobalt Substances 0.000 description 5
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 5
- 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 description 4
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 4
- 239000010406 cathode material Substances 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 239000010703 silicon Substances 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 125000004433 nitrogen atom Chemical group N* 0.000 description 3
- OZJPLYNZGCXSJM-UHFFFAOYSA-N 5-valerolactone Chemical compound O=C1CCCCO1 OZJPLYNZGCXSJM-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 125000004429 atom Chemical group 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 238000003490 calendering Methods 0.000 description 2
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- 230000000694 effects Effects 0.000 description 2
- 206010016766 flatulence Diseases 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 239000007773 negative electrode material Substances 0.000 description 2
- 238000011056 performance test Methods 0.000 description 2
- OFHWSHGIZXHMJP-UHFFFAOYSA-N 1,3,5-tripropyl-1,3,5-triazinane-2,4,6-trione Chemical compound CCCN1C(=O)N(CCC)C(=O)N(CCC)C1=O OFHWSHGIZXHMJP-UHFFFAOYSA-N 0.000 description 1
- WKFDWSVVMAKCDI-UHFFFAOYSA-N C(C=1C(C(=O)OCC)=CC=CC1)(=O)OCC.[C] Chemical compound C(C=1C(C(=O)OCC)=CC=CC1)(=O)OCC.[C] WKFDWSVVMAKCDI-UHFFFAOYSA-N 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910013172 LiNixCoy Inorganic materials 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 241000255964 Pieridae Species 0.000 description 1
- PFYQFCKUASLJLL-UHFFFAOYSA-N [Co].[Ni].[Li] Chemical compound [Co].[Ni].[Li] PFYQFCKUASLJLL-UHFFFAOYSA-N 0.000 description 1
- 125000002252 acyl group Chemical group 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 239000005030 aluminium foil Substances 0.000 description 1
- 239000006183 anode active material Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical compound C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
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- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 230000010261 cell growth Effects 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 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
- 238000013461 design Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000006253 efflorescence Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 238000005538 encapsulation Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- DIMZOVQGUDDSHG-UHFFFAOYSA-N ethene;sulfuric acid Chemical group C=C.OS(O)(=O)=O DIMZOVQGUDDSHG-UHFFFAOYSA-N 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- JBFHTYHTHYHCDJ-UHFFFAOYSA-N gamma-caprolactone Chemical compound CCC1CCC(=O)O1 JBFHTYHTHYHCDJ-UHFFFAOYSA-N 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical compound [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 description 1
- WDGKXRCNMKPDSD-UHFFFAOYSA-N lithium;trifluoromethanesulfonic acid Chemical compound [Li].OS(=O)(=O)C(F)(F)F WDGKXRCNMKPDSD-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 239000007774 positive electrode material Substances 0.000 description 1
- 206010037844 rash Diseases 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 238000004513 sizing Methods 0.000 description 1
- 239000002002 slurry Substances 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
- 125000002023 trifluoromethyl group Chemical group FC(F)(F)* 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 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
- H01M10/052—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
- H01M10/0567—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
- H01M10/42—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
- H01M2300/0025—Organic electrolyte
-
- 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)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The invention discloses a high-voltage lithium-ion battery with a Si/C composite anode. The high-voltage lithium-ion battery comprises a cathode, an anode as well as a separator and a non-aqueous electrolyte placed between the cathode and the anode, wherein the active substance of the cathode is lithium transition metal oxide; the active substance of the anode is a Si-based substance; the separator is a ceramic separator; the non-aqueous electrolyte comprises a non-aqueous organic solvent, lithium salt and an additive, the additive comprises FEC (fluoroethylene carbonate) and isocyanurate compounds in the mass ratio being (6-36):1. Compared with the prior art, the lithium-ion battery using the electrolyte has excellent normal-temperature cycle performance, high-temperature cycle performance and high-temperature storage life, and the gas output in the high-temperature storage process can be remarkably reduced.
Description
Technical field
The present invention relates to lithium ion battery preparing technical field, and in particular to a kind of silicon-carbon composite cathode high-voltage lithium ion
Battery.
Background technology
Lithium ion battery is the battery of a new generation's most competitiveness, is referred to as " the environmental protection energy ", is to solve contemporary ring
Border pollution problem and the one preferred technique of energy problem.In recent years, in high-energy battery field lithium ion battery achieved with huge
Success, but consumer still expects that the higher battery of combination property emerges, and this depends on to new electrode material and electrolyte
The research and development of system.
The electronic digital such as smart mobile phone, panel computer product requires more and more higher to the energy density of battery at present so that
Commercial li-ion battery is difficult to meet and requires.The energy density of lifting battery can be by following two modes：
1. high power capacity and high-pressure solid positive and negative pole material are selected；
2. the running voltage of battery is improved.
Pure silicon-based anode theory gram volume may be up to 4200mAh/g, but the negative pole as lithium ion, due to bulk effect,
Cell expansion, efflorescence are extremely serious, and cycle performance is poor, and then, silicon carbon material is combined by people's consideration, forms silicon-carbon cathode material
Material, can largely improve the specific capacity of material, while the bulk effect of silica-base material can be reduced to a certain extent,
And the electrolyte for being matched with silicon-carbon cathode material is also arisen at the historic moment, become the focus of lithium battery electrolytes research.
Fluorinated ethylene carbonate can form uniform and stable SEI film on silicon-carbon cathode surface, due to silicon-carbon cathode material
Particularity, generally require in its electrolyte system than the more film for additive of graphite cathode system, it usually needs using big
The FEC additive of amount, due to FEC in hot environment easy decomposes, it is impossible to meet battery high-temperature use requirement etc., single
Solely fluorinated ethylene carbonate (FEC) is used, which has various disadvantages.
Ask to solve flatulence of the lithium ion battery containing fluorinated ethylene carbonate additive during high temperature storage
Topic, the Chinese patent of Application No. CN201110157665 is using in the electrolytic solution by adding organic dinitrile material (NC-
(CH2) n-CN, wherein n=2～4) and method.Although this method can improve the high temperature of lithium ion battery to a certain extent
Storage performance, but the method is subject to certain restrictions.For example when requiring cycle performance with high-temperature storage performance while further
During raising, both results occur contradiction.
105428712 A of Samsung SDI Co., Ltd CN is disclosed to be contained based on Si negative electrode active material lithium rechargeable battery
There is additive to include trifluoromethanesulfonic acid lithium and fluoroethylene carbonate, improve reciprocal characteristics and the cycle life of Si negative battery
Characteristic.But, this invention needs to lift the high-temperature behavior of Si negative battery further and meets high energy density cells in height
Application under the conditions of temperature.
In view of this, it is necessory to provide one kind improve silicon-based anode lithium ion battery under high voltages good stability, with
When take into account circulation and the electrolyte method of high-temperature behavior and its battery.
Content of the invention
For not enough present in background above technology, the invention provides a kind of silicon-carbon composite cathode high-voltage lithium ion
Battery.
To achieve these goals, the present invention is achieved through the following technical solutions：
A kind of silicon-carbon composite cathode high-voltage lithium ion batteries, including：Negative electrode, anode, it is placed between negative electrode and anode
Barrier film and nonaqueous electrolytic solution, it is characterised in that；
The active substance of negative electrode is lithium transition-metal oxide；
The active substance of anode is the material based on Si；
Barrier film is ceramic diaphragm；
The nonaqueous electrolytic solution includes：Non-aqueous organic solvent, lithium salts and additive, additive includes fluorinated ethylene carbonate
With different
Cyanurate compound, and the mass fraction ratio of fluorinated ethylene carbonate and chlorinated isocyanurates is 6～36:1；Described
Isocyanide urea
Acid esters includes with least one in the compound shown in structure Formulas I：
R in formula1R2R3It is independently selected from H or saturation/unsaturated alkyl that carbon number is 1～10.
The additive of nonaqueous electrolytic solution also include 1,3- propane sultone, 1,4- butane sultone, 1,3- propene sultone,
One or more in sulfuric acid vinyl ester, adiponitrile and succinonitrile, and above-mentioned each additive quality hundred in the electrolytic solution
Divide ratio respectively 0.1～10%.
Active substance-the lithium transition-metal oxide of negative electrode is LiNixCoyMnzL(1-x-y-z)O2, wherein L is Al, Sr,
One kind in Mg, Ti, Ca, Zr, Zn, Si and Fe, 0≤x≤1,0≤y≤1,0≤z≤1.
The active substance of the negative electrode is preferably cobalt acid lithium or nickel cobalt lithium aluminate.
The active substance of the anode is preferably the silicon-carbon that nano-silicon or SiOx are composited with graphite.
The barrier film is coated with Al using one side2O3Ceramic diaphragm, or the ceramic diaphragm of dual coating PVDF.
It is 6%～26% percentage by weight that the content of the fluorinated ethylene carbonate presses the gross weight meter of nonaqueous electrolytic solution.
Compound shown in the formula 1, is 0.1%～2% by the gross weight meter of nonaqueous electrolytic solution.
The lithium salts is selected from lithium hexafluoro phosphate, lithium perchlorate, LiBF4, di-oxalate lithium borate, two (trifluoromethyl sulphurs
Acyl) one or more in imine lithium and imidodisulfuryl fluoride lithium salt.
In the nonaqueous electrolytic solution, lithium salts is preferably the lithium hexafluoro phosphate of concentration 1.15mol/L.
Described non-aqueous organic solvent is selected from ethylene carbonate, Allyl carbonate, butylene, dimethyl carbonate, carbon
Diethyl phthalate, Ethyl methyl carbonate, methyl propyl carbonate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate,
One kind in propyl propionate, methyl butyrate, ethyl n-butyrate., gamma-butyrolacton, gamma-valerolactone, δ-valerolactone, 6-caprolactone or two
More than kind.
In order to optimize cell output further, the electrolysis additive also containing PS, Isosorbide-5-Nitrae-
One or more in butane sultone, 1,3- propene sultone, sulfuric acid vinyl ester, adiponitrile and succinonitrile, and above-mentioned
Each additive mass percent in the electrolytic solution is respectively 0.1～10%.
It is an advantage of the current invention that：
(1) in additive 6%-26% fluorinated ethylene carbonate (FEC), formed in silicon-carbon cathode stable and with toughness
SEI film, bear battery during repeated charge silicon produce volumetric expansion, it is ensured that battery has preferable cyclicity
Energy.
(2) structural compounds shown in 0.1%～2% Formulas I in additive, can improve the high temperature circulation of lithium ion battery
Performance and high temperature storage life-span.Possible the reason for is：Isocyanurate compound contains three N atoms, often has N atom to have one
To lone pair electrons, can effectively with high-valency metal atom complexation, the interface impedance of positive pole can be significantly reduced, be conducive to lithium ion
In the migration at positive pole interface, and N atom significantly reduces positive electrode to electrolyte with the complexation of high-valency metal atom
Oxidation activity, so as to improve high temperature cyclic performance and the high temperature storage life-span of lithium ion battery.
(3) lithium-ion battery electrolytes of the present invention have so that silicon-carbon cathode lithium ion battery is still kept under high voltages
The beneficial effect of excellent normal-temperature circulating performance, high temperature cyclic performance and high-temperature storage characteristics.
Specific embodiment
Below by exemplary embodiment, the present invention will be further elaborated；But the scope of the present invention should not be limited to
In the scope of embodiment, any change without departing from present subject matter or change and can be understood by the person skilled in the art,
All within protection scope of the present invention.
Embodiment 1
1st, the preparation method of the present embodiment silicon-carbon composite cathode high-voltage lithium ion batteries, according to the Capacity design of battery,
Positive and negative pole material capacity determines coated face density.Positive active material is purchased from the leading 4.4V cobalt acid lithium material of Beijing University；Negative electrode active
Material is purchased from the silicon-carbon cathode (silicone content in silicon-carbon cathode material accounts for 1%～10%) of Shenzhen Bei Terui production.
Its positive pole preparation process, negative pole preparation process, electrolyte preparation process, barrier film preparation process and battery number of assembling steps
It is described as follows：
The positive pole preparation process is：By 96.8:2.0:1.2 mass ratio mixing high-voltage anode active material cobalt acid
Lithium, conductive carbon black and binding agent polyvinylidene fluoride, are dispersed in METHYLPYRROLIDONE, obtain anode sizing agent, by positive pole
Slurry is uniformly coated on the two sides of aluminium foil, through drying, calendering and be vacuum dried, and with supersonic welder burn-on aluminum extraction
Obtain positive plate after line, the thickness of pole plate is between 100-115 μm；
The negative pole preparation process is：By 96:1:1.2:1.8 mass ratio mixing silicon-carbon cathode, conductive carbon black, binding agent
Butadiene-styrene rubber and carboxymethyl cellulose, dispersion in deionized water, obtains cathode size, cathode size is coated on the two of Copper Foil
On face, through drying, calendering and it is vacuum dried, and is burn-on after nickel lead-out wire with supersonic welder negative plate is obtained, pole plate
Between 115-135 μm of thickness；
The electrolyte preparation process is：By ethylene carbonate, Allyl carbonate, diethyl carbonate is EC in mass ratio:
PC:DEC=10:20:70 are mixed, and add concentration for the lithium hexafluoro phosphate of 1.15mol/L, add based on electrolyte after mixing
The fluorinated ethylene carbonate (FEC) of the 15wt% of gross weight, the 1,3,5- Triallyl isocyanurate of 1wt%, the 1 of 4wt%,
3- propane sultone, the adiponitrile of 2wt%.
The barrier film preparation process is：Barrier film is coated with Al using one side2O3Ceramic diaphragm；
The preparation of lithium ion battery：Obtained positive plate, barrier film, negative plate are folded in order, barrier film are made in positive and negative
In the middle of pole piece, winding obtains naked battery core；Naked battery core is placed in outer package, the electrolyte of above-mentioned preparation is injected into dried
In battery, encapsulation, standing, chemical conversion, shaping, partial volume, complete the preparation (model 454261PL) of lithium ion battery.
1) normal-temperature circulating performance test：At 25 DEG C, the cobalt acid lithium battery after partial volume is charged to 4.4V with 1C constant current constant voltage,
Then with 1C constant-current discharge to 3.0V.The conservation rate of the 500th circulation volume, computing formula is calculated after 500 circulations of charge/discharge
As follows：
500th circulation volume conservation rate (%)=(the 500th cyclic discharge capacity/1st time cyclic discharge capacity) ×
100%；
2) high-temperature storage performance：Battery after partial volume is charged to 4.4V with 0.5C constant current constant voltage at normal temperatures, measures battery
Original depth, initial discharge capacity, then 4h is stored at 85 DEG C, under the conditions of 85 DEG C, heat surveys battery final thickness, calculates battery thickness
Degree expansion rate；Afterwards the holding capacity of 3.0V measurement battery is discharged to 0.5C and recovers capacity.Computing formula is as follows：
Cell thickness expansion rate (%)=(final thickness-original depth)/original depth × 100%；
Battery capacity conservation rate (%)=holding capacity/initial capacity × 100%；
Capacity resuming rate (%)=recovery capacity/initial capacity × 100%.
3) 45 DEG C of cycle performance tests：Under the conditions of 45 DEG C, the cobalt acid lithium battery after partial volume is charged to 1C constant current constant voltage
4.4V, then with 1C constant-current discharge to 3.0V.The conservation rate of the 400th circulation volume, meter is calculated after 400 circulations of charge/discharge
Calculate formula as follows：
400th circulation volume conservation rate (%)=(the 400th cyclic discharge capacity/1st time cyclic discharge capacity) ×
100%；2nd, embodiment 2～11 and comparative example 1～6
Embodiment 2～11 and comparative example 1～6, except additive composition presses 1 institute of table with content (based on electrolyte gross weight)
Show that interpolation is outer, other are all same as Example 1.
In table, 1,3-PS are PS, and it is adiponitrile that PRS is propenyl-1,3-sulfonic acid lactone, AN, and SN is fourth
Dintrile DTD for sulfuric acid vinyl ester POH for cyanuric acid POP be 1,3,5- tripropyl isocyanuric acid ester POA be 1,3,5- tri-
Allyl iso cyanurate.
Using technical scheme 1～embodiment of embodiment 11 with more preferable normal-temperature circulating performance, high-temperature storage
And high temperature cyclic performance；And normal temperature circulation, high temperature can not be taken into account simultaneously using the battery of 1～comparative example of comparative example, 6 electrolyte and followed
Ring and high-temperature storage performance.
Embodiment 1, embodiment 11 with comparative example 1～6 compare understand：
Comparative example 2 without FEC and comparative example the 5, the 500th are enclosed normal temperature circulation conservation rate and are respectively 29.6% 36.6%, far
Less than embodiment 1 (83.6%) and 11 (83.8%) conservation rate of embodiment, normal-temperature circulating performance is poor；Corresponding high-temperature storage and
High temperature cyclic performance is also bad.The presence of fluorinated ethylene carbonate (FEC) is described, is formed in silicon-carbon cathode and stablize and with toughness
SEI film, bear the battery volumetric expansion that silicon is produced during repeated charge, comprehensive lifting circulating battery and high temperatures
Energy.
Comparative example 1 without 1,3,5- Triallyl isocyanurate (POA) and 1,3,5- tripropyl isocyanuric acid is not contained
The comparative example 4 of ester (POP), battery high-temperature storge quality flatulence is serious, while 45 DEG C of circulations, 400 weeks conservation rates are not higher than
51.8%, far below embodiment 1 (80.6%) and embodiment 11 (81.9%), corresponding normal-temperature circulating performance is also bad.Explanation
1,3,5- Triallyl isocyanurate (POA) present in embodiment and 1,3,5- tripropyl isocyanuric acid ester (POP) can
It is obviously improved high temperature cyclic performance and the high temperature storage life-span of lithium ion battery.
Too high levels (＞ 2%, FEC and the POA mass hundred of 1,3,5- Triallyl isocyanurates (POA) in comparative example 3
Divide than being 5：1), cell output is deteriorated with respect to embodiment 1.As isocyanurate compound easily occurs electricity in cathode interface
Chemical reduction reaction generates the larger solid electrolyte interface film (SEI film) of impedance ratio, is unfavorable for lithium ion in negative material table
The migration in face, so as to deteriorate cell output.
It is further advanced by each embodiment and finds, the present invention passes through fluorinated ethylene carbonate (FEC) with the contrast of comparative example 1-6
It is applied in combination with isocyanurate compound, and aids in adding PS, 1,3- propene sultone, sulphuric acid ethylene
One or more in ester, adiponitrile and succinonitrile, further the addition of control additive reach change SEI composition and
Stability, the stability height of the overall less, structure of the SEI membrane impedance for being formed, so as to substantially increase silicon-carbon cathode lithium ion
The reversible capacity of battery and actual discharge ability, so guarantee battery still keep under high voltages excellent normal-temperature circulating performance,
High temperature cyclic performance and high-temperature storage performance.
It is more than illustrating for possible embodiments for the present invention, but the embodiment is not used to limit the present invention's
The scope of the claims, all equivalence enforcements without departing from carried out by the technology of the present invention spirit or change, are intended to be limited solely by the patent model of the present invention
Within enclosing.
Claims (10)
1. a kind of silicon-carbon composite cathode high-voltage lithium ion batteries, including：Negative electrode, anode, be placed between negative electrode and anode every
Film and nonaqueous electrolytic solution, it is characterised in that：
The active substance of negative electrode is lithium transition-metal oxide；
The active substance of anode is the material based on Si；
Barrier film is ceramic diaphragm；
The nonaqueous electrolytic solution includes：Non-aqueous organic solvent, lithium salts and additive, additive includes fluorinated ethylene carbonate and different
Cyanurate compound, and the mass fraction ratio of fluorinated ethylene carbonate and chlorinated isocyanurates is 6 ~ 36: 1；The isocyanide urea
Acid esters includes with least one in the compound shown in structure Formulas I：
Structure Formulas I
R in formula1R2R3It is independently selected from H or saturation/unsaturated alkyl that carbon number is 1～10.
2. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that the non-aqueous solution electrolysis
The additive of liquid also include 1,3- propane sultone, 1,4- butane sultone, 1,3- propene sultone, sulfuric acid vinyl ester, oneself two
One or more in nitrile and succinonitrile, and above-mentioned each additive mass percent in the electrolytic solution be respectively 0.1～
10%.
3. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：The active matter of negative electrode
It is Al, Sr, Mg, Ti, Ca, Zr, Zn, Si that matter-lithium transition-metal oxide is LiNixCoyMnz L (1-x-y-z) O2, wherein L
With the one kind in Fe, 0≤x≤1,0≤y≤1,0≤z≤1.
4. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 3, it is characterised in that：The work of the negative electrode
Property material be.
5. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：The work of the anode
The silicon-carbon that property material is composited with graphite for nano-silicon or SiOx.
6. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：The barrier film is adopted
One side is coated with Al2O3Ceramic diaphragm or dual coating PVDF ceramic diaphragm.
7. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：The fluoro carbonic acid
The content of vinyl acetate mass percent in the electrolytic solution is 6%～26%；Described with compound shown in Formulas I in the electrolytic solution
Weight/mass percentage composition is 0.1%～2%.
8. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：The lithium salts is selected from
Lithium hexafluoro phosphate, lithium perchlorate, LiBF4, di-oxalate lithium borate, two (trimethyl fluoride sulfonyl) imine lithium and double fluorine sulphonyl
One or more in imines lithium salts.
9. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：The non-aqueous solution electrolysis
In liquid, lithium salts is the lithium hexafluoro phosphate of concentration 1.15mol/L.
10. silicon-carbon composite cathode high-voltage lithium ion batteries according to claim 1, it is characterised in that：Described is non-aqueous
Organic solvent is selected from ethylene carbonate, Allyl carbonate, butylene, dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate
Ester, methyl propyl carbonate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, propyl propionate, methyl butyrate,
One or more in ethyl n-butyrate., γ-butyrolactone, γ-valerolactone, δ-valerolactone, ε-caprolactone.
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| CN110120553A (en) * | 2018-02-05 | 2019-08-13 | 宁德新能源科技有限公司 | A kind of electrolyte and lithium ion battery |
| CN112366354A (en) * | 2020-12-02 | 2021-02-12 | 蜂巢能源科技有限公司 | Electrolyte and lithium ion battery |
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| CN110120553A (en) * | 2018-02-05 | 2019-08-13 | 宁德新能源科技有限公司 | A kind of electrolyte and lithium ion battery |
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| CN113078356A (en) * | 2021-02-09 | 2021-07-06 | 东莞市杉杉电池材料有限公司 | High-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte and lithium ion battery |
| CN113078356B (en) * | 2021-02-09 | 2022-05-27 | 东莞市杉杉电池材料有限公司 | High-voltage lithium cobalt oxide lithium ion battery non-aqueous electrolyte and lithium ion battery |
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