JP6269475B2 - 二次電池 - Google Patents
二次電池 Download PDFInfo
- Publication number
- JP6269475B2 JP6269475B2 JP2014502090A JP2014502090A JP6269475B2 JP 6269475 B2 JP6269475 B2 JP 6269475B2 JP 2014502090 A JP2014502090 A JP 2014502090A JP 2014502090 A JP2014502090 A JP 2014502090A JP 6269475 B2 JP6269475 B2 JP 6269475B2
- Authority
- JP
- Japan
- Prior art keywords
- group
- secondary battery
- negative electrode
- fluorinated
- halogenated
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Fee Related
Links
- -1 phosphoric acid ester compound Chemical class 0.000 claims description 67
- 239000007773 negative electrode material Substances 0.000 claims description 49
- 239000008151 electrolyte solution Substances 0.000 claims description 48
- 229910044991 metal oxide Inorganic materials 0.000 claims description 43
- 150000004706 metal oxides Chemical class 0.000 claims description 43
- 229910052751 metal Inorganic materials 0.000 claims description 42
- 239000002184 metal Substances 0.000 claims description 42
- 239000002245 particle Substances 0.000 claims description 34
- 125000000217 alkyl group Chemical group 0.000 claims description 31
- 239000003575 carbonaceous material Substances 0.000 claims description 28
- 125000000753 cycloalkyl group Chemical group 0.000 claims description 27
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 26
- 125000003342 alkenyl group Chemical group 0.000 claims description 26
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 25
- 229910001416 lithium ion Inorganic materials 0.000 claims description 25
- 229910052744 lithium Inorganic materials 0.000 claims description 23
- 125000003545 alkoxy group Chemical group 0.000 claims description 20
- 229910019142 PO4 Inorganic materials 0.000 claims description 16
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 16
- 238000000034 method Methods 0.000 claims description 15
- 239000010452 phosphate Substances 0.000 claims description 15
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 14
- 239000011883 electrode binding agent Substances 0.000 claims description 13
- 150000001875 compounds Chemical class 0.000 claims description 11
- 229910052731 fluorine Inorganic materials 0.000 claims description 11
- 239000000203 mixture Substances 0.000 claims description 11
- 229910052710 silicon Inorganic materials 0.000 claims description 11
- 239000002904 solvent Substances 0.000 claims description 11
- 229910052782 aluminium Inorganic materials 0.000 claims description 10
- 239000010703 silicon Substances 0.000 claims description 10
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 9
- 125000005843 halogen group Chemical group 0.000 claims description 9
- 229910003002 lithium salt Inorganic materials 0.000 claims description 9
- 159000000002 lithium salts Chemical class 0.000 claims description 9
- 229920002312 polyamide-imide Polymers 0.000 claims description 9
- 239000004642 Polyimide Substances 0.000 claims description 8
- 125000001153 fluoro group Chemical group F* 0.000 claims description 8
- 239000005001 laminate film Substances 0.000 claims description 8
- 229920001721 polyimide Polymers 0.000 claims description 8
- 239000004962 Polyamide-imide Substances 0.000 claims description 7
- 125000004432 carbon atom Chemical group C* 0.000 claims description 6
- 125000003808 silyl group Chemical group [H][Si]([H])([H])[*] 0.000 claims description 6
- 230000008569 process Effects 0.000 claims description 5
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 4
- 125000003277 amino group Chemical group 0.000 claims description 4
- 125000004093 cyano group Chemical group *C#N 0.000 claims description 4
- 125000004122 cyclic group Chemical group 0.000 claims description 4
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 4
- 239000012280 lithium aluminium hydride Substances 0.000 claims description 4
- 229910000103 lithium hydride Inorganic materials 0.000 claims description 4
- 125000000449 nitro group Chemical group [O-][N+](*)=O 0.000 claims description 4
- 229910052702 rhenium Inorganic materials 0.000 claims description 4
- 125000003118 aryl group Chemical group 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 2
- 238000004519 manufacturing process Methods 0.000 claims 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 25
- 210000004027 cell Anatomy 0.000 description 21
- 150000003839 salts Chemical class 0.000 description 20
- 229910013870 LiPF 6 Inorganic materials 0.000 description 15
- 235000021317 phosphate Nutrition 0.000 description 15
- 229910052799 carbon Inorganic materials 0.000 description 12
- 239000007774 positive electrode material Substances 0.000 description 12
- 230000008859 change Effects 0.000 description 11
- 229910002804 graphite Inorganic materials 0.000 description 11
- 239000010439 graphite Substances 0.000 description 11
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 10
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 9
- 239000007789 gas Substances 0.000 description 9
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 9
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 8
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 8
- 239000011230 binding agent Substances 0.000 description 8
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 8
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 7
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 7
- 238000009863 impact test Methods 0.000 description 7
- 229910052718 tin Inorganic materials 0.000 description 7
- 229910013872 LiPF Inorganic materials 0.000 description 6
- 101150058243 Lipf gene Proteins 0.000 description 6
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 6
- 239000003792 electrolyte Substances 0.000 description 6
- 238000003701 mechanical milling Methods 0.000 description 6
- 229910045601 alloy Inorganic materials 0.000 description 5
- 239000000956 alloy Substances 0.000 description 5
- 230000006866 deterioration Effects 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- DHKHKXVYLBGOIT-UHFFFAOYSA-N 1,1-Diethoxyethane Chemical compound CCOC(C)OCC DHKHKXVYLBGOIT-UHFFFAOYSA-N 0.000 description 4
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 4
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 description 4
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 4
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 description 4
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 4
- GUUVPOWQJOLRAS-UHFFFAOYSA-N Diphenyl disulfide Chemical compound C=1C=CC=CC=1SSC1=CC=CC=C1 GUUVPOWQJOLRAS-UHFFFAOYSA-N 0.000 description 4
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 4
- 239000004743 Polypropylene Substances 0.000 description 4
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 4
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 description 4
- 229910052794 bromium Inorganic materials 0.000 description 4
- 239000000460 chlorine Substances 0.000 description 4
- 229910052801 chlorine Inorganic materials 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000011267 electrode slurry Substances 0.000 description 4
- 239000010408 film Substances 0.000 description 4
- 239000011737 fluorine Substances 0.000 description 4
- GAEKPEKOJKCEMS-UHFFFAOYSA-N gamma-valerolactone Chemical compound CC1CCC(=O)O1 GAEKPEKOJKCEMS-UHFFFAOYSA-N 0.000 description 4
- 229910052740 iodine Inorganic materials 0.000 description 4
- 239000011630 iodine Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000002923 metal particle Substances 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 238000002156 mixing Methods 0.000 description 4
- 229920001155 polypropylene Polymers 0.000 description 4
- 239000000843 powder Substances 0.000 description 4
- DQWPFSLDHJDLRL-UHFFFAOYSA-N triethyl phosphate Chemical compound CCOP(=O)(OCC)OCC DQWPFSLDHJDLRL-UHFFFAOYSA-N 0.000 description 4
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 description 4
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 3
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 description 3
- WFDIJRYMOXRFFG-UHFFFAOYSA-N Acetic anhydride Chemical compound CC(=O)OC(C)=O WFDIJRYMOXRFFG-UHFFFAOYSA-N 0.000 description 3
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 3
- 239000002033 PVDF binder Substances 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
- 239000011149 active material Substances 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 239000011246 composite particle Substances 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 229910052736 halogen Inorganic materials 0.000 description 3
- 150000002367 halogens Chemical class 0.000 description 3
- 239000011159 matrix material Substances 0.000 description 3
- 230000007246 mechanism Effects 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- RJCRUVXAWQRZKQ-UHFFFAOYSA-N oxosilicon;silicon Chemical compound [Si].[Si]=O RJCRUVXAWQRZKQ-UHFFFAOYSA-N 0.000 description 3
- 229920000573 polyethylene Polymers 0.000 description 3
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 3
- 229910052723 transition metal Inorganic materials 0.000 description 3
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 description 2
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 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 description 2
- FALRKNHUBBKYCC-UHFFFAOYSA-N 2-(chloromethyl)pyridine-3-carbonitrile Chemical compound ClCC1=NC=CC=C1C#N FALRKNHUBBKYCC-UHFFFAOYSA-N 0.000 description 2
- IUVGGESEBFJHPK-UHFFFAOYSA-N 2-ethoxy-1,3,2$l^{5}-dioxaphospholane 2-oxide Chemical compound CCOP1(=O)OCCO1 IUVGGESEBFJHPK-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- DHXVGJBLRPWPCS-UHFFFAOYSA-N Tetrahydropyran Chemical compound C1CCOCC1 DHXVGJBLRPWPCS-UHFFFAOYSA-N 0.000 description 2
- 239000007983 Tris buffer Substances 0.000 description 2
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 2
- 230000002411 adverse Effects 0.000 description 2
- 229910003481 amorphous carbon Inorganic materials 0.000 description 2
- 229910052786 argon Inorganic materials 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- JKJWYKGYGWOAHT-UHFFFAOYSA-N bis(prop-2-enyl) carbonate Chemical compound C=CCOC(=O)OCC=C JKJWYKGYGWOAHT-UHFFFAOYSA-N 0.000 description 2
- 239000006229 carbon black Substances 0.000 description 2
- 208000037998 chronic venous disease Diseases 0.000 description 2
- 229920001577 copolymer Polymers 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 150000005676 cyclic carbonates Chemical class 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 description 2
- 239000002019 doping agent Substances 0.000 description 2
- 238000002149 energy-dispersive X-ray emission spectroscopy Methods 0.000 description 2
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 230000002427 irreversible effect Effects 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 description 2
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- 239000011812 mixed powder Substances 0.000 description 2
- 239000011255 nonaqueous electrolyte Substances 0.000 description 2
- MHYFEEDKONKGEB-UHFFFAOYSA-N oxathiane 2,2-dioxide Chemical compound O=S1(=O)CCCCO1 MHYFEEDKONKGEB-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 2
- 238000010248 power generation Methods 0.000 description 2
- 230000002040 relaxant effect Effects 0.000 description 2
- 229910052709 silver Inorganic materials 0.000 description 2
- 238000004544 sputter deposition Methods 0.000 description 2
- 229940014800 succinic anhydride Drugs 0.000 description 2
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 2
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 description 2
- GSURLQOINUQIIH-UHFFFAOYSA-N triheptyl phosphate Chemical compound CCCCCCCOP(=O)(OCCCCCCC)OCCCCCCC GSURLQOINUQIIH-UHFFFAOYSA-N 0.000 description 2
- SFENPMLASUEABX-UHFFFAOYSA-N trihexyl phosphate Chemical compound CCCCCCOP(=O)(OCCCCCC)OCCCCCC SFENPMLASUEABX-UHFFFAOYSA-N 0.000 description 2
- QJAVUVZBMMXBRO-UHFFFAOYSA-N tripentyl phosphate Chemical compound CCCCCOP(=O)(OCCCCC)OCCCCC QJAVUVZBMMXBRO-UHFFFAOYSA-N 0.000 description 2
- RXPQRKFMDQNODS-UHFFFAOYSA-N tripropyl phosphate Chemical compound CCCOP(=O)(OCCC)OCCC RXPQRKFMDQNODS-UHFFFAOYSA-N 0.000 description 2
- HYFGMEKIKXRBIP-UHFFFAOYSA-N tris(trifluoromethyl) phosphate Chemical compound FC(F)(F)OP(=O)(OC(F)(F)F)OC(F)(F)F HYFGMEKIKXRBIP-UHFFFAOYSA-N 0.000 description 2
- 238000004804 winding Methods 0.000 description 2
- WFLOTYSKFUPZQB-UPHRSURJSA-N (z)-1,2-difluoroethene Chemical group F\C=C/F WFLOTYSKFUPZQB-UPHRSURJSA-N 0.000 description 1
- WDXYVJKNSMILOQ-UHFFFAOYSA-N 1,3,2-dioxathiolane 2-oxide Chemical compound O=S1OCCO1 WDXYVJKNSMILOQ-UHFFFAOYSA-N 0.000 description 1
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 description 1
- RYHBNJHYFVUHQT-UHFFFAOYSA-N 1,4-Dioxane Chemical compound C1COCCO1 RYHBNJHYFVUHQT-UHFFFAOYSA-N 0.000 description 1
- NVJUHMXYKCUMQA-UHFFFAOYSA-N 1-ethoxypropane Chemical compound CCCOCC NVJUHMXYKCUMQA-UHFFFAOYSA-N 0.000 description 1
- CXBDYQVECUFKRK-UHFFFAOYSA-N 1-methoxybutane Chemical compound CCCCOC CXBDYQVECUFKRK-UHFFFAOYSA-N 0.000 description 1
- LDMIKSKELVYBIZ-UHFFFAOYSA-N 2-methoxy-1,3,2$l^{5}-dioxaphospholane 2-oxide Chemical compound COP1(=O)OCCO1 LDMIKSKELVYBIZ-UHFFFAOYSA-N 0.000 description 1
- FAYFWMOSHFCQPG-UHFFFAOYSA-N 3-Methyl sulfolene Chemical compound CC1=CCS(=O)(=O)C1 FAYFWMOSHFCQPG-UHFFFAOYSA-N 0.000 description 1
- HKJLJJFTDJTNFV-UHFFFAOYSA-N 3-fluoropropyl methyl carbonate Chemical compound COC(=O)OCCCF HKJLJJFTDJTNFV-UHFFFAOYSA-N 0.000 description 1
- UJEGMXFDCQSTKY-UHFFFAOYSA-N 4,4,4-trifluorobutyl hydrogen carbonate Chemical compound OC(=O)OCCCC(F)(F)F UJEGMXFDCQSTKY-UHFFFAOYSA-N 0.000 description 1
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- OYOKPDLAMOMTEE-UHFFFAOYSA-N 4-chloro-1,3-dioxolan-2-one Chemical compound ClC1COC(=O)O1 OYOKPDLAMOMTEE-UHFFFAOYSA-N 0.000 description 1
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- 239000005947 Dimethoate Substances 0.000 description 1
- 229910010238 LiAlCl 4 Inorganic materials 0.000 description 1
- 229910015015 LiAsF 6 Inorganic materials 0.000 description 1
- 229910013063 LiBF 4 Inorganic materials 0.000 description 1
- 229910013372 LiC 4 Inorganic materials 0.000 description 1
- 229910013684 LiClO 4 Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910014689 LiMnO Inorganic materials 0.000 description 1
- 229910011456 LiNi0.80Co0.15Al0.05O2 Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- 229910012513 LiSbF 6 Inorganic materials 0.000 description 1
- 229910001228 Li[Ni1/3Co1/3Mn1/3]O2 (NCM 111) Inorganic materials 0.000 description 1
- XOBKSJJDNFUZPF-UHFFFAOYSA-N Methoxyethane Chemical compound CCOC XOBKSJJDNFUZPF-UHFFFAOYSA-N 0.000 description 1
- HJFQASWJCUWFBJ-UHFFFAOYSA-N P(=O)(OC(F)(F)F)(OC(F)(F)F)OC(F)(F)F.P1(=O)(OC(CCCO1)CC)O Chemical compound P(=O)(OC(F)(F)F)(OC(F)(F)F)OC(F)(F)F.P1(=O)(OC(CCCO1)CC)O HJFQASWJCUWFBJ-UHFFFAOYSA-N 0.000 description 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
- 230000001070 adhesive effect Effects 0.000 description 1
- 150000007933 aliphatic carboxylic acids Chemical class 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- RDOXTESZEPMUJZ-UHFFFAOYSA-N anisole Chemical compound COC1=CC=CC=C1 RDOXTESZEPMUJZ-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- JKIZUKLNAQCQSX-UHFFFAOYSA-N bis(1-fluoroethyl) carbonate Chemical compound CC(F)OC(=O)OC(C)F JKIZUKLNAQCQSX-UHFFFAOYSA-N 0.000 description 1
- YZWIIIGEQKTIMS-UHFFFAOYSA-N bis(2-fluoroethyl) carbonate Chemical compound FCCOC(=O)OCCF YZWIIIGEQKTIMS-UHFFFAOYSA-N 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
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- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- PMGNOQUKCGLETL-TYYBGVCCSA-N carbonic acid;(e)-1,2-difluoroethene Chemical compound OC(O)=O.F\C=C\F PMGNOQUKCGLETL-TYYBGVCCSA-N 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
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- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000006482 condensation reaction Methods 0.000 description 1
- 230000003750 conditioning effect Effects 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 239000006184 cosolvent Substances 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- UAEWCWCMYQAIDR-UHFFFAOYSA-N diethyl methyl phosphate Chemical compound CCOP(=O)(OC)OCC UAEWCWCMYQAIDR-UHFFFAOYSA-N 0.000 description 1
- IJKVHSBPTUYDLN-UHFFFAOYSA-N dihydroxy(oxo)silane Chemical compound O[Si](O)=O IJKVHSBPTUYDLN-UHFFFAOYSA-N 0.000 description 1
- MCWXGJITAZMZEV-UHFFFAOYSA-N dimethoate Chemical compound CNC(=O)CSP(=S)(OC)OC MCWXGJITAZMZEV-UHFFFAOYSA-N 0.000 description 1
- VONWDASPFIQPDY-UHFFFAOYSA-N dimethyl methylphosphonate Chemical compound COP(C)(=O)OC VONWDASPFIQPDY-UHFFFAOYSA-N 0.000 description 1
- POLCUAVZOMRGSN-UHFFFAOYSA-N dipropyl ether Chemical compound CCCOCCC POLCUAVZOMRGSN-UHFFFAOYSA-N 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 238000007606 doctor blade method Methods 0.000 description 1
- 229920001971 elastomer Polymers 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 150000002170 ethers Chemical class 0.000 description 1
- KLKFAASOGCDTDT-UHFFFAOYSA-N ethoxymethoxyethane Chemical compound CCOCOCC KLKFAASOGCDTDT-UHFFFAOYSA-N 0.000 description 1
- JQVXMIPNQMYRPE-UHFFFAOYSA-N ethyl dimethyl phosphate Chemical compound CCOP(=O)(OC)OC JQVXMIPNQMYRPE-UHFFFAOYSA-N 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 229910003437 indium oxide Inorganic materials 0.000 description 1
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 1
- 239000002608 ionic liquid Substances 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
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- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- VNKYTQGIUYNRMY-UHFFFAOYSA-N methoxypropane Chemical compound CCCOC VNKYTQGIUYNRMY-UHFFFAOYSA-N 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- 239000013081 microcrystal Substances 0.000 description 1
- GKTNLYAAZKKMTQ-UHFFFAOYSA-N n-[bis(dimethylamino)phosphinimyl]-n-methylmethanamine Chemical compound CN(C)P(=N)(N(C)C)N(C)C GKTNLYAAZKKMTQ-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
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- 239000004745 nonwoven fabric Substances 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
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- 229910052697 platinum Inorganic materials 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- WYVAMUWZEOHJOQ-UHFFFAOYSA-N propionic anhydride Chemical compound CCC(=O)OC(=O)CC WYVAMUWZEOHJOQ-UHFFFAOYSA-N 0.000 description 1
- FVSKHRXBFJPNKK-UHFFFAOYSA-N propionitrile Chemical compound CCC#N FVSKHRXBFJPNKK-UHFFFAOYSA-N 0.000 description 1
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- 150000003377 silicon compounds Chemical class 0.000 description 1
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- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 1
- 239000011871 silicon-based negative electrode active material Substances 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- APSBXTVYXVQYAB-UHFFFAOYSA-M sodium docusate Chemical compound [Na+].CCCCC(CC)COC(=O)CC(S([O-])(=O)=O)C(=O)OCC(CC)CCCC APSBXTVYXVQYAB-UHFFFAOYSA-M 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- MBDNRNMVTZADMQ-UHFFFAOYSA-N sulfolene Chemical compound O=S1(=O)CC=CC1 MBDNRNMVTZADMQ-UHFFFAOYSA-N 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 229920001187 thermosetting polymer Polymers 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 1
- 229910001887 tin oxide Inorganic materials 0.000 description 1
- 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 description 1
- WBJDAYNUJLJYHT-UHFFFAOYSA-N tris(1,1,2,2,2-pentafluoroethyl) phosphate Chemical compound FC(F)(F)C(F)(F)OP(=O)(OC(F)(F)C(F)(F)F)OC(F)(F)C(F)(F)F WBJDAYNUJLJYHT-UHFFFAOYSA-N 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
- QETBFZRDHPYSIW-UHFFFAOYSA-N tris(3,3,3-trifluoropropyl) phosphate Chemical compound FC(F)(F)CCOP(=O)(OCCC(F)(F)F)OCCC(F)(F)F QETBFZRDHPYSIW-UHFFFAOYSA-N 0.000 description 1
- 238000007740 vapor deposition Methods 0.000 description 1
- 239000002966 varnish Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 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
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Description
負極は、負極活物質が負極用結着剤によって負極集電体を覆うように結着されてなる。そして、本発明では、リチウムと合金可能な金属(a)、リチウムイオンを吸蔵、放出し得る金属酸化物(b)、およびリチウムイオンを吸蔵、放出し得る炭素材料(c)を含む負極活物質を用いる。
正極は、例えば、正極活物質が正極用結着剤によって正極集電体を覆うように結着されてなる。
本発明で用いる電解液は、65vol%以上のリン酸エステル化合物と、0vol%超、20vol%未満のフッ素化カーボネート化合物を含む溶媒に、支持塩であるリチウム塩を溶解したものである。この電解液の溶媒は、70〜99vol%のリン酸エステル化合物と、1〜15vol%のフッ素化カーボネート化合物を含むことが好ましい。溶媒中のリン酸エステル化合物の含有率は、85〜99vol%がより好ましく、90〜95vol%がさらに好ましい。溶媒中のフッ素化カーボネート化合物の含有率は、1〜15vol%がより好ましく、2〜5vol%がさらに好ましい。フッ素化カーボネート化合物を混合することで、シリコンのような非炭素系負極の表面に被膜を形成し、リン酸エステル化合物系電解液の分解を抑制することができる。さらに、溶媒中のリン酸エステル化合物の含有率を65vol%以上、溶媒中のフッ素化カーボネート化合物の含有率を20vol%未満とすることにより、衝撃を受けても温度上昇が少ない二次電池を得ることができる。衝撃による温度上昇が少ない二次電池を用いることで、二次電池を組み込んだデバイスに温度制御装置等の余分な機構を備え付ける必要がなくなる。
セパレータとしては、例えば、ポリプロピレン、ポリエチレン等の多孔質フィルムや、不織布を用いることができる。また、セパレータとして、それらを積層したものを用いることもできる。
外装体としては、電解液に対して安定で、かつ十分な水蒸気バリア性を持つものであれば特に限定されず、適宜選択することができる。例えば、積層ラミネート型の二次電池の場合、外装体としては、アルミニウムまたはシリカをコーティングしたポリプロピレン、ポリエチレン等のラミネートフィルムを用いることができる。特に、体積膨張を抑制する観点から、アルミニウムラミネートフィルムを用いることが好ましい。
金属(a)としての平均粒径5μmのすずと、酸化物(b)としての平均粒径10μmのシリコン酸化物と、炭素材料(c)としての平均粒径20μmの黒鉛とを、30:60:10の質量比で計量・混合して、負極活物質を得た。この負極活物質と、負極用結着剤としてのポリアミドイミド(PAI,東洋紡績株式会社製、商品名:バイロマックス(登録商標))とを、85:15の質量比で計量し、それらをn−メチルピロリドンと混合して、負極スラリーとした。負極スラリーを厚さ15μmの銅箔に塗布した後に乾燥し、さらに窒素雰囲気300℃の熱処理を行うことで、負極を作製した。
得られた二次電池を、20℃環境下で0.1Cの電流にて、上限電圧4.2V、下限電圧2.7Vで充放電を行い、そのときの初回放電容量を測定した。結果を表1に示す。
45℃に保った恒温槽中で、0.5Cの電流にて、上限電圧4.2V、下限電圧2.7Vで50回充放電を繰り返し、1回目の放電容量に対する50回目の放電容量の比率を維持率とした。結果を表1に示す。
正極1層および負極1層をセパレータを介して配置し、電解液を注入したこと以外は、上記と同様の方法でアルミラミネートセルを作製した。得られたセルのコンディショニングを行った後、0.2Cの電流にて上限電圧4.3Vまで充電し、セルの外側に熱電対を取り付けてセルの温度を測定した。そして、充電状態のセルに対して、上から重さ5kgの重りを高さ50cmから落とすことで衝撃を与えた後、セルの外側に取り付けた熱電対によりセルの温度を測定した。衝撃試験後のセル上昇温度(=(衝撃試験後のセル最高到達温度)−(衝撃試験前のセル温度))を算出した。結果を表1に示す。
電解液として、TEPとFECを98:2(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとFECを95:5(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとFECを90:10(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとFECと混合カーボネート電解液(エチレンカーボネート/プロピレンカーボネート/ジエチルカーボネート/エチルメチルカーボネート/ジメチルカーボネート=2/2/2/2/2(体積比))を70:1:29(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとFECと混合カーボネート電解液(エチレンカーボネート/プロピレンカーボネート/ジエチルカーボネート/エチルメチルカーボネート/ジメチルカーボネート=2/2/2/2/2(体積比))を70:15:15(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPと混合カーボネート電解液(エチレンカーボネート/プロピレンカーボネート/ジエチルカーボネート/エチルメチルカーボネート/ジメチルカーボネート=2/2/2/2/2(体積比))を99:1(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPと混合カーボネート電解液(エチレンカーボネート/プロピレンカーボネート/ジエチルカーボネート/エチルメチルカーボネート/ジメチルカーボネート=2/2/2/2/2(体積比))を65:35(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとFECと混合カーボネート電解液(エチレンカーボネート/プロピレンカーボネート/ジエチルカーボネート/エチルメチルカーボネート/ジメチルカーボネート=2/2/2/2/2(体積比))を63:2:35(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとFECを80:20(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例1と同様に二次電池を作製し、評価した。結果を表1に示す。
負極活物質として、平均粒径20μmの黒鉛を用いた以外は、実施例2と同様に二次電池を作製し、評価した。結果を表1に示す。
負極活物質として、金属(a)としての平均粒径5μmのシリコンと、炭素材料(c)としての平均粒径20μmの黒鉛とを、80:20の質量比で計量し、いわゆるメカニカルミリングで24時間混合を行って作製した物質を用いた以外は、実施例2と同様に二次電池を作製し、評価した。結果を表1に示す。
実施例2と同じ負極活物質に水素化リチウムを質量比(1:10)で混合し、アルゴンガス中、600℃で1時間の熱処理を行った(リチウムドープ処理)。負極活物質に熱処理を行った後は、実施例2と同様に二次電池を作製し、評価した。結果を表1に示す。
実施例2と同じ負極活物質に水素化アルミニウムリチウムを質量比(1:10)で混合し、アルゴンガス中、600℃で1時間の熱処理を行った(リチウムドープ処理)。負極活物質に熱処理を行った後は、実施例2と同様に二次電池を作製し、評価した。結果を表1に示す。
金属(a)としての平均粒径5μmのすずと、酸化物(b)としての平均粒径10μmのシリコン酸化物を30:60の質量比で計量し、いわゆるメカニカルミリングで24時間混合して、平均粒径D50=5〜10μmのすず粒子が酸化物マトリックスに分散した金属・酸化物複合粒子を得た。メカニカルミリング処理により、酸化物はアモルファス化が進んでいた。この金属・酸化物複合粒子と、炭素材料(c)としての平均粒径20μmの黒鉛とを、90:10の質量比で計量・混合して、負極活物質を得た。この負極活物質を用いたこと以外は、実施例7と同様に二次電池を作製し、評価した。結果を表1に示す。
金属(a)としての平均粒径5μmのすずと、酸化物(b)としての平均粒径10μmのシリコン酸化物と、炭素材料(c)としての平均粒径20μmの黒鉛とを、30:60:10の質量比で計量し、いわゆるメカニカルミリングで24時間混合して、平均粒径D50=5〜10μmの負極活物質を得た。メカニカルミリング処理により、すず粒子は酸化物マトリックス中に分散し、酸化物はアモルファス化が進み、炭素粒子は、すず・酸化物複合粒子の表面付近に局在化していた。この負極活物質を用いたこと以外は、実施例7と同様に二次電池を作製し、評価した。結果を表1に示す。
一般式SiOで表されるケイ素−酸化ケイ素混合粉末(酸化ケイ素とケイ素との混合物)を、メタンガスを含む雰囲気下1150℃で6時間CVD処理を行うことで、酸化ケイ素中のケイ素が酸化物マトリックス中に分散し、酸化物はアモルファスであり、炭素粒子が被覆されたケイ素−酸化ケイ素混合粉末の表面付近に局在化した負極活物質を得た。ケイ素/酸化ケイ素/カーボンの質量比は、およそ30/60/10となるように調整した。この負極活物質を用いたこと以外は、実施例7と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、トリメチルフォスフェート(MEP)とTEPとFECを10:88:2(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例11と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、トリス(トリフルオロメチル)フォスフェート(TTFP)とTEPとFECを10:88:2(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例11と同様に二次電池を作製し、評価した。結果を表1に示す。
電解液として、TEPとcis−1,2−ジフルオロエチレンカーボネート(DFEC)を98:2(体積比)の割合で混合し、さらに支持塩としてLiPF6を1mol/Lの濃度で溶解したものを用いた以外は、実施例11と同様に二次電池を作製し、評価した。結果を表1に示す。
負極用結着材として、ポリイミド(PI,宇部興産株式会社製、商品名:UワニスA)を用いた以外は、実施例11と同様に二次電池を作製し、評価した。結果を表1に示す。
負極用結着材として、ポリアミドイミド(PAI,東洋紡績株式会社製、商品名:バイロマックス(登録商標))と、ポリイミド(PI,宇部興産株式会社製、商品名:UワニスA)の重量比1:1の混合物を用いた以外は、実施例11と同様に二次電池を作製し、評価した。結果を表1に示す。
b セパレータ
c 正極
d 負極集電体
e 正極集電体
f 正極端子
g 負極端子
Claims (14)
- 正極および負極が対向配置された電極素子と、電解液と、前記電極素子および前記電解液を内包する外装体とを有し、
前記負極は、リチウムと合金可能な金属(a)、リチウムイオンを吸蔵、放出し得る金属酸化物(b)、およびリチウムイオンを吸蔵、放出し得る炭素材料(c)を含む負極活物質が、負極結着剤によって負極集電体と結着されてなり、
前記電解液が、65vol%以上のリン酸エステル化合物と、0vol%超、20vol%未満のフッ素化カーボネート化合物を含む溶媒に、リチウム塩を溶解してなることを特徴とする二次電池。 - 前記電解液の溶媒が、70〜99vol%のリン酸エステル化合物と、1〜15vol%のフッ素化カーボネート化合物を含むことを特徴とする請求項1に記載の二次電池。
- 前記式(1)中のRs、RtおよびRuがいずれも炭素数10以下のアルキル基であることを特徴とする請求項3に記載の二次電池。
- 前記フッ素化カーボネート化合物が、下記式(2a)または(2b)で表される化合物、または下記式(3)で表される化合物であることを特徴とする請求項1乃至4のいずれかに記載の二次電池。
- 前記フッ素化カーボネート化合物が、フルオロエチレンカーボネート、またはジフルオロエチレンカーボネートであることを特徴とする請求項5に記載の二次電池。
- 前記金属(a)の全部または一部が、前記金属酸化物(b)中に分散していることを特徴とする請求項1乃至6のいずれかに記載の二次電池。
- 前記金属酸化物(b)の全部または一部が、アモルファス構造を有することを特徴とする請求項1乃至7のいずれかに記載の二次電池。
- 前記炭素材料(c)の全部または一部が、前記アモルファス構造を有する金属酸化物(b)中に前記金属(a)が分散している粒子の表面付近に局在化していることを特徴とする請求項8に記載の二次電池。
- 前記金属(a)がシリコンであり、前記酸化物(b)が酸化シリコンであることを特徴とする請求項1乃至9のいずれかに記載の二次電池。
- 前記負極結着剤が、ポリイミド、ポリアミドイミド、または、ポリイミドとポリアミドイミドの混合物からなることを特徴とする請求項1乃至10のいずれかに記載の二次電池。
- 前記電極素子が、平面的な積層構造を有していることを特徴とする請求項1乃至11のいずれかに記載の二次電池。
- 前記外装体が、アルミニウムラミネートフィルムであることを特徴とする請求項1乃至12のいずれかに記載の二次電池。
- 請求項1〜13のいずれか1項に記載の二次電池の製造方法であって、負極活物質を、水素化リチウムおよび/または水素化リチウムアルミニウムと混合した後、温度200℃以上800℃以下で加熱処理する工程を有することを特徴とする、二次電池の製造方法。
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JP5748193B2 (ja) | 2009-09-29 | 2015-07-15 | Necエナジーデバイス株式会社 | 二次電池 |
JP5145367B2 (ja) | 2010-03-11 | 2013-02-13 | 株式会社日立製作所 | 非水電解液及びこれを用いたリチウム二次電池 |
JP5411780B2 (ja) * | 2010-04-05 | 2014-02-12 | 信越化学工業株式会社 | 非水電解質二次電池用負極材及び非水電解質二次電池用負極材の製造方法並びにリチウムイオン二次電池 |
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2013
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US9748608B2 (en) | 2017-08-29 |
US20150093631A1 (en) | 2015-04-02 |
WO2013129033A1 (ja) | 2013-09-06 |
CN104170153A (zh) | 2014-11-26 |
JPWO2013129033A1 (ja) | 2015-07-30 |
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