JP2023547555A - 非水電解液およびそれを含むリチウム二次電池 - Google Patents
非水電解液およびそれを含むリチウム二次電池 Download PDFInfo
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- JP2023547555A JP2023547555A JP2023533750A JP2023533750A JP2023547555A JP 2023547555 A JP2023547555 A JP 2023547555A JP 2023533750 A JP2023533750 A JP 2023533750A JP 2023533750 A JP2023533750 A JP 2023533750A JP 2023547555 A JP2023547555 A JP 2023547555A
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- negative electrode
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 65
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 53
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 50
- 239000000126 substance Substances 0.000 claims abstract description 48
- 150000001875 compounds Chemical class 0.000 claims abstract description 47
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 18
- 239000011356 non-aqueous organic solvent Substances 0.000 claims abstract description 17
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 16
- 125000004432 carbon atom Chemical group C* 0.000 claims description 29
- 229910052731 fluorine Inorganic materials 0.000 claims description 19
- 229910052757 nitrogen Inorganic materials 0.000 claims description 17
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims description 16
- 239000011737 fluorine Substances 0.000 claims description 16
- 125000000217 alkyl group Chemical group 0.000 claims description 15
- 125000004433 nitrogen atom Chemical group N* 0.000 claims description 15
- 125000004366 heterocycloalkenyl group Chemical group 0.000 claims description 12
- 229910052751 metal Inorganic materials 0.000 claims description 9
- 239000002184 metal Substances 0.000 claims description 9
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 7
- 229910052710 silicon Inorganic materials 0.000 claims description 7
- 239000010703 silicon Substances 0.000 claims description 7
- 125000000392 cycloalkenyl group Chemical group 0.000 claims description 6
- 229910052723 transition metal Inorganic materials 0.000 claims description 5
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 claims description 3
- 229910008326 Si-Y Inorganic materials 0.000 claims description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910006773 Si—Y Inorganic materials 0.000 claims description 2
- 229910052783 alkali metal Inorganic materials 0.000 claims description 2
- 150000001340 alkali metals Chemical class 0.000 claims description 2
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- 229910052800 carbon group element Inorganic materials 0.000 claims description 2
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 2
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 2
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- 150000003624 transition metals Chemical class 0.000 claims description 2
- 239000002409 silicon-based active material Substances 0.000 claims 2
- 239000002388 carbon-based active material Substances 0.000 claims 1
- 230000001976 improved effect Effects 0.000 abstract description 10
- 239000007773 negative electrode material Substances 0.000 description 40
- -1 LiCH 3 SO 3 Inorganic materials 0.000 description 38
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 35
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- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 21
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- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 5
- 239000010949 copper Substances 0.000 description 5
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- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 4
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- 239000002033 PVDF binder Substances 0.000 description 4
- 239000002131 composite material Substances 0.000 description 4
- 229910052802 copper Inorganic materials 0.000 description 4
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 description 4
- 125000001153 fluoro group Chemical group F* 0.000 description 4
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- 229910001220 stainless steel Inorganic materials 0.000 description 4
- 239000010935 stainless steel Substances 0.000 description 4
- 229920003048 styrene butadiene rubber Polymers 0.000 description 4
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 description 3
- 229920000049 Carbon (fiber) Polymers 0.000 description 3
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- 229910019142 PO4 Inorganic materials 0.000 description 3
- 239000006229 carbon black Substances 0.000 description 3
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- 239000004917 carbon fiber Substances 0.000 description 3
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- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 3
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229910044991 metal oxide Inorganic materials 0.000 description 3
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical class [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 3
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- 238000003860 storage Methods 0.000 description 3
- OQYOVYWFXHQYOP-UHFFFAOYSA-N 1,3,2-dioxathiane 2,2-dioxide Chemical compound O=S1(=O)OCCCO1 OQYOVYWFXHQYOP-UHFFFAOYSA-N 0.000 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 description 2
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- 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 description 2
- VGYDTVNNDKLMHX-UHFFFAOYSA-N lithium;manganese;nickel;oxocobalt Chemical compound [Li].[Mn].[Ni].[Co]=O VGYDTVNNDKLMHX-UHFFFAOYSA-N 0.000 description 2
- VLXXBCXTUVRROQ-UHFFFAOYSA-N lithium;oxido-oxo-(oxomanganiooxy)manganese Chemical compound [Li+].[O-][Mn](=O)O[Mn]=O VLXXBCXTUVRROQ-UHFFFAOYSA-N 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
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- 229910052787 antimony Inorganic materials 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- 150000001555 benzenes Chemical class 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- 229910021475 bohrium Inorganic materials 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- IAQRGUVFOMOMEM-UHFFFAOYSA-N butene Natural products CC=CC IAQRGUVFOMOMEM-UHFFFAOYSA-N 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000009831 deintercalation Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 description 1
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 description 1
- 238000010828 elution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 229940093499 ethyl acetate Drugs 0.000 description 1
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 229920002313 fluoropolymer Polymers 0.000 description 1
- 239000004811 fluoropolymer Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 229910052735 hafnium Inorganic materials 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 229910021473 hassium Inorganic materials 0.000 description 1
- 229920001519 homopolymer Polymers 0.000 description 1
- 150000003949 imides Chemical class 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 239000010954 inorganic particle Substances 0.000 description 1
- 238000009830 intercalation Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 150000007527 lewis bases Chemical class 0.000 description 1
- 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 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- FRMOHNDAXZZWQI-UHFFFAOYSA-N lithium manganese(2+) nickel(2+) oxygen(2-) Chemical class [O-2].[Mn+2].[Ni+2].[Li+] FRMOHNDAXZZWQI-UHFFFAOYSA-N 0.000 description 1
- 229910021450 lithium metal oxide Inorganic materials 0.000 description 1
- 229910000686 lithium vanadium oxide Inorganic materials 0.000 description 1
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 1
- IGILRSKEFZLPKG-UHFFFAOYSA-M lithium;difluorophosphinate Chemical compound [Li+].[O-]P(F)(F)=O IGILRSKEFZLPKG-UHFFFAOYSA-M 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000002931 mesocarbon microbead Substances 0.000 description 1
- 239000011302 mesophase pitch Substances 0.000 description 1
- 239000002905 metal composite material Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 229940017219 methyl propionate Drugs 0.000 description 1
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 1
- PYLWMHQQBFSUBP-UHFFFAOYSA-N monofluorobenzene Chemical compound FC1=CC=CC=C1 PYLWMHQQBFSUBP-UHFFFAOYSA-N 0.000 description 1
- YKYONYBAUNKHLG-UHFFFAOYSA-N n-Propyl acetate Natural products CCCOC(C)=O YKYONYBAUNKHLG-UHFFFAOYSA-N 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 229910052762 osmium Inorganic materials 0.000 description 1
- MHYFEEDKONKGEB-UHFFFAOYSA-N oxathiane 2,2-dioxide Chemical compound O=S1(=O)CCCCO1 MHYFEEDKONKGEB-UHFFFAOYSA-N 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 239000011295 pitch Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 229910052699 polonium Inorganic materials 0.000 description 1
- 229920000139 polyethylene terephthalate Polymers 0.000 description 1
- 239000005020 polyethylene terephthalate Substances 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 229940090181 propyl acetate Drugs 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 229920001384 propylene homopolymer Polymers 0.000 description 1
- 239000002296 pyrolytic carbon Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 229910052702 rhenium Inorganic materials 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 229910021481 rutherfordium Inorganic materials 0.000 description 1
- 150000003839 salts Chemical group 0.000 description 1
- 229910052706 scandium Inorganic materials 0.000 description 1
- 229910021477 seaborgium Inorganic materials 0.000 description 1
- 125000002914 sec-butyl group Chemical group [H]C([H])([H])C([H])([H])C([H])(*)C([H])([H])[H] 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 150000004756 silanes Chemical class 0.000 description 1
- 229910021384 soft carbon Inorganic materials 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000005728 strengthening Methods 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- 239000011271 tar pitch Substances 0.000 description 1
- 229910052713 technetium Inorganic materials 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- UFHILTCGAOPTOV-UHFFFAOYSA-N tetrakis(ethenyl)silane Chemical compound C=C[Si](C=C)(C=C)C=C UFHILTCGAOPTOV-UHFFFAOYSA-N 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- ZMQDTYVODWKHNT-UHFFFAOYSA-N tris(2,2,2-trifluoroethyl) phosphate Chemical compound FC(F)(F)COP(=O)(OCC(F)(F)F)OCC(F)(F)F ZMQDTYVODWKHNT-UHFFFAOYSA-N 0.000 description 1
- CBIQXUBDNNXYJM-UHFFFAOYSA-N tris(2,2,2-trifluoroethyl) phosphite Chemical compound FC(F)(F)COP(OCC(F)(F)F)OCC(F)(F)F CBIQXUBDNNXYJM-UHFFFAOYSA-N 0.000 description 1
- QJMMCGKXBZVAEI-UHFFFAOYSA-N tris(trimethylsilyl) phosphate Chemical compound C[Si](C)(C)OP(=O)(O[Si](C)(C)C)O[Si](C)(C)C QJMMCGKXBZVAEI-UHFFFAOYSA-N 0.000 description 1
- VMZOBROUFBEGAR-UHFFFAOYSA-N tris(trimethylsilyl) phosphite Chemical compound C[Si](C)(C)OP(O[Si](C)(C)C)O[Si](C)(C)C VMZOBROUFBEGAR-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- NQPDZGIKBAWPEJ-UHFFFAOYSA-N valeric acid Chemical compound CCCCC(O)=O NQPDZGIKBAWPEJ-UHFFFAOYSA-N 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 238000012795 verification Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- PAPBSGBWRJIAAV-UHFFFAOYSA-N ε-Caprolactone Chemical compound O=C1CCCCCO1 PAPBSGBWRJIAAV-UHFFFAOYSA-N 0.000 description 1
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Abstract
Description
リチウム塩と、
非水性有機溶媒と、
下記化学式1で表される化合物と、を含む、非水電解液を提供する。
R1は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基、または-OR3(R3は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基である)であり、
R2は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基、または-C(O)-R4(R4は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基である)である。
一実施形態によると、本発明は、非水電解液を提供する。
リチウム塩と、
非水性有機溶媒と、
下記化学式1で表される化合物と、を含む。
R1は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基、または-OR3(R3は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基である)であり、
R2は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基、または-C(O)-R4(R4は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基である)である。
先ず、リチウム塩について説明すると、次のとおりである。
また、非水性有機溶媒についての説明は、次のとおりである。
本発明の非水電解液は、添加剤として、下記化学式1で表される化合物を含んでもよい。
R1は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基、または-OR3(R3は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基である)であり、
R2は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基、または-C(O)-R4(R4は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基である)である。
R2は、少なくとも1つの窒素原子を含む炭素数2~6のヘテロシクロアルケニル基、または-C(O)-R4(R4は、少なくとも1つの窒素原子を含む炭素数2~6のヘテロシクロアルケニル基である)である。
また、本発明の非水電解液は、高出力の環境で非水電解液が分解されて負極の崩壊が引き起こされることを防止するか、低温高率放電特性、高温安定性、過充電防止、高温での電池膨張抑制効果などをより向上させるために、その他の付加的添加剤をさらに含んでもよい。
また、本発明の他の実施形態は、正極と、負極と、前記正極と負極との間に介在されるセパレータと、前述の本発明の非水電解液と、を含むリチウム二次電池を提供する。
本発明に係る正極は、正極活物質を含む正極活物質層を含み、必要に応じて、前記正極活物質層は、導電材および/またはバインダーをさらに含んでもよい。
次に、負極について説明する。
本発明のリチウム二次電池に含まれる前記セパレータとしては、一般に用いられる通常の多孔性高分子フィルム、例えば、エチレン単独重合体、プロピレン単独重合体、エチレン/ブテン共重合体、エチレン/ヘキセン共重合体、およびエチレン/メタクリレート共重合体などのようなポリオレフィン系高分子で製造した多孔性高分子フィルムを単独で、またはこれらを積層して用いてもよく、または、通常の多孔性不織布、例えば、高融点のガラス繊維、ポリエチレンテレフタレート繊維などからなる不織布を用いてもよいが、これらに限定されるものではない。
実施例1.
(非水電解液の製造)
エチレンカーボネート(EC)とエチルメチルカーボネート(EMC)を30:70の体積比で混合した非水性有機溶媒にLiPF6が1.0Mとなるように溶解した後、前記化学式1-1で表される化合物0.5重量%およびフルオロエチレンカーボネート0.5重量%を添加し、非水電解液を製造した(下記表1参照)。
N-メチル-2-ピロリドン(NMP)に、正極活物質(Li(Ni0.86Co0.05Mn0.07Al0.02)O2)、導電材(カーボンブラック)、およびバインダー(ポリビニリデンフルオライド)を97.5:1:1.5の重量比で添加し、正極スラリー(固形分の含量:50重量%)を製造した。前記正極スラリーを厚さ12μmの正極集電体であるアルミニウム(Al)薄膜に塗布および乾燥した後、ロールプレス(roll press)を行って正極を製造した。
非水性有機溶媒にLiPF6が1.0Mとなるように溶解した後、化学式1-1で表される化合物3.0重量%およびフルオロエチレンカーボネート0.5重量%を添加して非水電解液を製造した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
非水性有機溶媒にLiPF6が1.0Mとなるように溶解した後、化学式1-1で表される化合物5.0重量%およびフルオロエチレンカーボネート0.5重量%を添加して非水電解液を製造した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
非水性有機溶媒にLiPF6が1.0Mとなるように溶解した後、化学式1-1で表される化合物6.0重量%およびフルオロエチレンカーボネート0.5重量%を添加して非水電解液を製造した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
化学式1-1で表される化合物に代えて、化学式1-2で表される化合物を添加して非水電解液を製造した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
化学式1-1で表される化合物に代えて、化学式1-2で表される化合物を添加して非水電解液を製造した点を除き、前記実施例3と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
エチレンカーボネート(EC)とエチルメチルカーボネート(EMC)を30:70の体積比で混合した非水性有機溶媒に、LiPF6が1.0Mとなるように溶解した後、フルオロエチレンカーボネート0.5重量%を添加して非水電解液を製造した(下記表1参照)。
実施例1の非水電解液に代えて、上記で製造された非水電解液を添加した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
化学式1-1で表される化合物に代えて、化学式3で表される化合物を添加して非水電解液を製造した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
化学式1-1で表される化合物に代えて、下記化学式4で表される化合物を添加して非水電解液を製造した点を除き、前記実施例1と同様の方法により非水電解液およびリチウム二次電池を製造した(下記表1参照)。
実験例1.初期抵抗評価
前記実施例1~6で製造されたリチウム二次電池と比較例2および3で製造されたリチウム二次電池のそれぞれを、常温(25℃)で、0.33Cレート(C rate)で定電流/定電圧条件で4.2Vまで充電した後、DOD(depth of discharge)50%まで放電してSOC50%に調整した後、2.5Cレート(C rate)条件で10秒間放電し、PNE-0506充放電器(製造社:PNEソリューション)を用いて初期抵抗を測定した。その結果を下記表2に記載した。
実施例1~3、5および6で製造されたリチウム二次電池と、比較例1~3で製造されたリチウム二次電池のそれぞれを、45℃で、0.33Cレート(C rate)で定電流/定電圧条件下で4.2Vまで充電した後、0.33Cレート(C rate)で定電流条件下で3Vまで放電することを1サイクルとし、200サイクルの充放電を行った後、容量維持率(%)および抵抗増加率(%)を測定した。容量維持率(%)は下記[式1]により計算し、抵抗増加率(%)は下記[式2]により計算した。測定結果は下記表3に記載した。
容量維持率(%)=(200サイクル後の放電容量/1サイクル後の放電容量)×100
抵抗増加率(%)={(200サイクル後の抵抗-1サイクル後の抵抗)/1サイクル後の抵抗}×100
実施例1~6で製造されたリチウム二次電池と、比較例1~3で製造されたリチウム二次電池のそれぞれを、常温(25℃)で、0.33Cレート(C rate)で定電流/定電圧条件で4.2Vまで充電した後、DOD(depth of discharge)50%まで放電してSOC50%に調整した後、2.5Cレート(C rate)条件で10秒間放電した後、初期厚さを測定した。
Claims (10)
- リチウム塩と、
非水性有機溶媒と、
下記化学式1で表される化合物と、を含む、非水電解液:
R1は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基、または-OR3(R3は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~5のアルキル基である)であり、
R2は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基、または-C(O)-R4(R4は、少なくとも1つの窒素原子を含む炭素数2~8のヘテロシクロアルケニル基である)である。 - 前記化学式1中、R1は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~3のアルキル基、または-OR3(R3は、少なくとも1つのフッ素元素で置換されているかまたは置換されていない炭素数1~3のアルキル基である)であり、
R2は、少なくとも1つの窒素原子を含む炭素数2~6のヘテロシクロアルケニル基、または-C(O)-R4(R4は、少なくとも1つの窒素原子を含む炭素数2~6のヘテロシクロアルケニル基である)である、請求項1に記載の非水電解液。 - 前記化学式1中、
R1は、-CH3、CF3、-OCH3、およびOCF3から選択される少なくとも1つであり、
R2は、
- 前記化学式1で表される化合物は、下記化学式1-1~化学式1-4で表される化合物から選択される少なくとも1つである、請求項1に記載の非水電解液。
- 前記化学式1で表される化合物は、非水電解液の全重量を基準として0.1重量%~7.0重量%で含まれる、請求項1に記載の非水電解液。
- 前記化学式1で表される化合物は、非水電解液の全重量を基準として0.5重量%~5.0重量%で含まれる、請求項1に記載の非水電解液。
- 正極と、負極と、前記正極と前記負極との間に介在されるセパレータと、
請求項1から6のいずれか一項に記載の非水電解液と、を含む、リチウム二次電池。 - 前記負極は、シリコン系活物質を含む、請求項7に記載のリチウム二次電池。
- 前記シリコン系活物質は、金属シリコン(Si)、シリコン酸化物(SiOx、ここで、0<x<2)、炭化ケイ素(SiC)、およびSi-Y合金(前記Yは、アルカリ金属、アルカリ土類金属、13族元素、14族元素、遷移金属、希土類元素、およびこれらの組み合わせからなる群から選択される元素であり、Siではない)からなる群から選択される少なくとも1つを含む、請求項8に記載のリチウム二次電池。
- 前記負極は、炭素系活物質をさらに含む、請求項7に記載のリチウム二次電池。
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