JP6678659B2 - 非水性電解液及びこれを含むリチウム二次電池 - Google Patents
非水性電解液及びこれを含むリチウム二次電池 Download PDFInfo
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- JP6678659B2 JP6678659B2 JP2017516688A JP2017516688A JP6678659B2 JP 6678659 B2 JP6678659 B2 JP 6678659B2 JP 2017516688 A JP2017516688 A JP 2017516688A JP 2017516688 A JP2017516688 A JP 2017516688A JP 6678659 B2 JP6678659 B2 JP 6678659B2
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- Prior art keywords
- lithium
- secondary battery
- carbonate
- lithium secondary
- aqueous electrolyte
- Prior art date
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- 229910052744 lithium Inorganic materials 0.000 title claims description 64
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims description 62
- 239000011255 nonaqueous electrolyte Substances 0.000 title claims description 32
- -1 fluorinated benzene compound Chemical class 0.000 claims description 20
- 239000007774 positive electrode material Substances 0.000 claims description 20
- 229910003002 lithium salt Inorganic materials 0.000 claims description 18
- 159000000002 lithium salts Chemical class 0.000 claims description 18
- 239000000126 substance Substances 0.000 claims description 16
- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 claims description 11
- 239000000203 mixture Substances 0.000 claims description 11
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 9
- 150000001555 benzenes Chemical class 0.000 claims description 9
- 150000001875 compounds Chemical class 0.000 claims description 9
- 238000002156 mixing Methods 0.000 claims description 9
- 239000000654 additive Substances 0.000 claims description 8
- 229910013870 LiPF 6 Inorganic materials 0.000 claims description 7
- SOXUFMZTHZXOGC-UHFFFAOYSA-N [Li].[Mn].[Co].[Ni] Chemical compound [Li].[Mn].[Co].[Ni] SOXUFMZTHZXOGC-UHFFFAOYSA-N 0.000 claims description 7
- 230000000996 additive effect Effects 0.000 claims description 7
- 239000002904 solvent Substances 0.000 claims description 7
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 6
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 6
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 6
- 239000011356 non-aqueous organic solvent Substances 0.000 claims description 5
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 claims description 4
- GDHXJNRAJRCGMX-UHFFFAOYSA-N 2-fluorobenzonitrile Chemical compound FC1=CC=CC=C1C#N GDHXJNRAJRCGMX-UHFFFAOYSA-N 0.000 claims description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 4
- 150000005676 cyclic carbonates Chemical class 0.000 claims description 4
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 claims description 4
- CYEDOLFRAIXARV-UHFFFAOYSA-N ethyl propyl carbonate Chemical compound CCCOC(=O)OCC CYEDOLFRAIXARV-UHFFFAOYSA-N 0.000 claims description 4
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 4
- 150000002825 nitriles Chemical class 0.000 claims description 4
- SUSQOBVLVYHIEX-UHFFFAOYSA-N phenylacetonitrile Chemical compound N#CCC1=CC=CC=C1 SUSQOBVLVYHIEX-UHFFFAOYSA-N 0.000 claims description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 4
- 238000000926 separation method Methods 0.000 claims description 4
- 239000012528 membrane Substances 0.000 claims description 3
- GKPHNZYMLJPYJJ-UHFFFAOYSA-N 2,3-difluorobenzonitrile Chemical compound FC1=CC=CC(C#N)=C1F GKPHNZYMLJPYJJ-UHFFFAOYSA-N 0.000 claims description 2
- DAVJMKMVLKOQQC-UHFFFAOYSA-N 2-(2-fluorophenyl)acetonitrile Chemical compound FC1=CC=CC=C1CC#N DAVJMKMVLKOQQC-UHFFFAOYSA-N 0.000 claims description 2
- HIXDQWDOVZUNNA-UHFFFAOYSA-N 2-(3,4-dimethoxyphenyl)-5-hydroxy-7-methoxychromen-4-one Chemical compound C=1C(OC)=CC(O)=C(C(C=2)=O)C=1OC=2C1=CC=C(OC)C(OC)=C1 HIXDQWDOVZUNNA-UHFFFAOYSA-N 0.000 claims description 2
- JHQBLYITVCBGTO-UHFFFAOYSA-N 2-(4-fluorophenyl)acetonitrile Chemical compound FC1=CC=C(CC#N)C=C1 JHQBLYITVCBGTO-UHFFFAOYSA-N 0.000 claims description 2
- AEKVBBNGWBBYLL-UHFFFAOYSA-N 4-fluorobenzonitrile Chemical compound FC1=CC=C(C#N)C=C1 AEKVBBNGWBBYLL-UHFFFAOYSA-N 0.000 claims description 2
- 229910010238 LiAlCl 4 Inorganic materials 0.000 claims description 2
- 229910010090 LiAlO 4 Inorganic materials 0.000 claims description 2
- 229910015015 LiAsF 6 Inorganic materials 0.000 claims description 2
- 229910013684 LiClO 4 Inorganic materials 0.000 claims description 2
- 229910012513 LiSbF 6 Inorganic materials 0.000 claims description 2
- RFFFKMOABOFIDF-UHFFFAOYSA-N Pentanenitrile Chemical compound CCCCC#N RFFFKMOABOFIDF-UHFFFAOYSA-N 0.000 claims description 2
- KVNRLNFWIYMESJ-UHFFFAOYSA-N butyronitrile Chemical compound CCCC#N KVNRLNFWIYMESJ-UHFFFAOYSA-N 0.000 claims description 2
- VBWIZSYFQSOUFQ-UHFFFAOYSA-N cyclohexanecarbonitrile Chemical compound N#CC1CCCCC1 VBWIZSYFQSOUFQ-UHFFFAOYSA-N 0.000 claims description 2
- SVPZJHKVRMRREG-UHFFFAOYSA-N cyclopentanecarbonitrile Chemical compound N#CC1CCCC1 SVPZJHKVRMRREG-UHFFFAOYSA-N 0.000 claims description 2
- 150000002148 esters Chemical class 0.000 claims description 2
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 2
- SDAXRHHPNYTELL-UHFFFAOYSA-N heptanenitrile Chemical compound CCCCCCC#N SDAXRHHPNYTELL-UHFFFAOYSA-N 0.000 claims description 2
- 150000002576 ketones Chemical class 0.000 claims description 2
- 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 claims description 2
- YSIMAPNUZAVQER-UHFFFAOYSA-N octanenitrile Chemical compound CCCCCCCC#N YSIMAPNUZAVQER-UHFFFAOYSA-N 0.000 claims description 2
- FVSKHRXBFJPNKK-UHFFFAOYSA-N propionitrile Chemical compound CCC#N FVSKHRXBFJPNKK-UHFFFAOYSA-N 0.000 claims description 2
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims 3
- 229910013063 LiBF 4 Inorganic materials 0.000 claims 1
- 230000003796 beauty Effects 0.000 claims 1
- 125000000118 dimethyl group Chemical group [H]C([H])([H])* 0.000 claims 1
- 238000005868 electrolysis reaction Methods 0.000 claims 1
- 230000000052 comparative effect Effects 0.000 description 20
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 17
- 239000003792 electrolyte Substances 0.000 description 15
- 150000002500 ions Chemical class 0.000 description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 12
- 239000010408 film Substances 0.000 description 11
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 9
- 229910052799 carbon Inorganic materials 0.000 description 9
- 229910001416 lithium ion Inorganic materials 0.000 description 9
- 239000008151 electrolyte solution Substances 0.000 description 8
- 229910052723 transition metal Inorganic materials 0.000 description 8
- 239000010410 layer Substances 0.000 description 7
- 238000007086 side reaction Methods 0.000 description 7
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- 239000002000 Electrolyte additive Substances 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
- 229910052759 nickel Inorganic materials 0.000 description 5
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 4
- 239000005977 Ethylene Substances 0.000 description 4
- 239000004743 Polypropylene Substances 0.000 description 4
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- 238000004519 manufacturing process Methods 0.000 description 4
- 239000007773 negative electrode material Substances 0.000 description 4
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- 150000003624 transition metals Chemical class 0.000 description 4
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- 239000011572 manganese Substances 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 3
- 230000008961 swelling Effects 0.000 description 3
- PEBWOGPSYUIOBP-UHFFFAOYSA-N 1,2,4-trifluorobenzene Chemical compound FC1=CC=C(F)C(F)=C1 PEBWOGPSYUIOBP-UHFFFAOYSA-N 0.000 description 2
- 229910000733 Li alloy Inorganic materials 0.000 description 2
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 2
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 2
- 239000004698 Polyethylene Substances 0.000 description 2
- 239000011149 active material Substances 0.000 description 2
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- 229910045601 alloy Inorganic materials 0.000 description 2
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- 238000010828 elution Methods 0.000 description 2
- 239000003063 flame retardant Substances 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 239000001989 lithium alloy Substances 0.000 description 2
- 229910021450 lithium metal oxide Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
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- AJKNNUJQFALRIK-UHFFFAOYSA-N 1,2,3-trifluorobenzene Chemical compound FC1=CC=CC(F)=C1F AJKNNUJQFALRIK-UHFFFAOYSA-N 0.000 description 1
- GOYDNIKZWGIXJT-UHFFFAOYSA-N 1,2-difluorobenzene Chemical compound FC1=CC=CC=C1F GOYDNIKZWGIXJT-UHFFFAOYSA-N 0.000 description 1
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 description 1
- 229910015902 Bi 2 O 3 Inorganic materials 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910005793 GeO 2 Inorganic materials 0.000 description 1
- 229910003945 Li(Ni0.5Co0.3Mn0.2)O2 Inorganic materials 0.000 description 1
- 229910004403 Li(Ni0.6Co0.2Mn0.2)O2 Inorganic materials 0.000 description 1
- 229910007969 Li-Co-Ni Inorganic materials 0.000 description 1
- 229910013075 LiBF Inorganic materials 0.000 description 1
- 229910012424 LiSO 3 Inorganic materials 0.000 description 1
- 229910016599 LixFe Inorganic materials 0.000 description 1
- 229910006555 Li—Co—Ni Inorganic materials 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 229910006404 SnO 2 Inorganic materials 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- ZYXUQEDFWHDILZ-UHFFFAOYSA-N [Ni].[Mn].[Li] Chemical compound [Ni].[Mn].[Li] ZYXUQEDFWHDILZ-UHFFFAOYSA-N 0.000 description 1
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 239000003125 aqueous solvent Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 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
- 239000003660 carbonate based solvent Substances 0.000 description 1
- 239000006182 cathode active material 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
- 229920001940 conductive polymer Polymers 0.000 description 1
- 150000004696 coordination complex Chemical class 0.000 description 1
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- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical group COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 125000001153 fluoro group Chemical group F* 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
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- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- 229920001519 homopolymer Polymers 0.000 description 1
- 239000012212 insulator Substances 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 238000002955 isolation Methods 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- PYLWMHQQBFSUBP-UHFFFAOYSA-N monofluorobenzene Chemical compound FC1=CC=CC=C1 PYLWMHQQBFSUBP-UHFFFAOYSA-N 0.000 description 1
- 229910021470 non-graphitizable carbon Inorganic materials 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
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Classifications
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- 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
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- H—ELECTRICITY
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
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- 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
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- H01M10/0566—Liquid materials
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- 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
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M4/622—Binders being polymers
- H01M4/623—Binders being polymers fluorinated polymers
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- H—ELECTRICITY
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
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Description
本出願は、2014年9月26日付韓国特許出願第10-2014-0128878号に基づいた優先権の利益を主張し、当該韓国特許出願の文献に開示されている全ての内容は本明細書の一部として含まれる。
本発明は、リチウムビスフルオロスルホニルイミド(Lithium bis(fluorosulfonyl)imide;LiFSI)及びフルオロ化ベンゼン系化合物添加剤を含む非水性電解液、正極活物質としてリチウム-ニッケル-マンガン-コバルト系酸化物を含む正極、負極及び分離膜を含むものであるリチウム二次電池に関する。
[化学式(1)]
Li1+x(NiaCobMnc)O2
前記化学式(1)で、0.55≦a≦0.65、0.18≦b≦0.22、0.18≦c≦0.22、-0.2≦x≦0.2及びx+a+b+c=1である。
[化学式(1)]
Li1+x(NiaCobMnc)O2
(前記化学式(1)で、0.55≦a≦0.65、0.18≦b≦0.22、0.18≦c≦0.22、-0.2≦x≦0.2及びx+a+b+c=1である。)
具体的に、前記R1は、前記フルオロ化ベンゼン系化合物がフルオロベンゼン、ジフルオロベンゼン、トリフルオロベンゼン及びその誘導体からなる群より選択される1種以上であってよく、本発明の一実施形態によれば、前記フルオロ化ベンゼン系化合物は1,3,6トリフルオロベンゼンであってよい。
実施例
実施例1
[電解液の製造]
エチレンカーボネート(EC):エチルメチルカーボネート(EMC)3:7(体積比)の組成を有する非水性有機溶媒、及びリチウム塩として非水性電解液の総量を基準にLiPF6 0.9mol/l及びリチウムビスフルオロスルホニルイミド 0.1mol/l、添加剤として1,3,6トリフルオロ化ベンゼンを非水電解液の総重量を基準に5重量%を添加して非水性電解液を製造した。
正極活物質としてLi(Ni0.6Co0.2Mn0.2)O2 92重量%、導電材としてカーボンブラック(carbon black)4重量%、バインダとしてポリビニリデンフルオリド(PVdF)4重量%を、溶媒であるN-メチル-2-ピロリドン(NMP)に添加して正極混合物スラリーを製造した。前記正極混合物スラリーを厚さが20μm程度の正極集電体であるアルミニウム(Al)薄膜に塗布し、乾燥して正極を製造したあと、ロールプレス(roll press)を実施して正極を製造した。
前記リチウム塩を、非水性電解液の総量を基準にLiPF6 0.7mol/l及びリチウムビスフルオロスルホニルイミド0.3mol/lを用いたことを除き、実施例1と同様にして非水性電解液及びリチウム二次電池を製造した。
前記リチウム塩を、非水性電解液の総量を基準にLiPF6 0.6mol/l及びリチウムビスフルオロスルホニルイミド0.4mol/lを用いたことを除き、実施例1と同様にして非水性電解液及びリチウム二次電池を製造した。
前記リチウム塩を、非水性電解液の総量を基準にLiPF6 0.5mol/l及びリチウムビスフルオロスルホニルイミド0.5mol/lを用いたことを除き、実施例1と同様にして非水性電解液及びリチウム二次電池を製造した。
前記リチウム塩を、非水性電解液の総量を基準にLiPF6 0.4mol/l及びリチウムビスフルオロスルホニルイミド0.6mol/lを用いたことを除き、実施例1と同様にして非水性電解液及びリチウム二次電池を製造した。
前記添加剤を利用していないことを除き、実施例2と同様にして非水性電解液及びリチウム二次電池を製造した。
前記正極活物質としてのLi(Ni0.5Co0.3Mn0.2)O2を除き、実施例2と同様にして非水性電解液及びリチウム二次電池を製造した。
<低温出力特性>
実施例1から4及び比較例1から3で製造された二次電池を-30℃で0.5Cで10秒間充電及び放電する場合に発生する電圧差を利用して出力を計算した。このとき、比較例1の出力は4.18Wであった。比較例1を基準にして、実施例1から4及び比較例2から3の出力を百分率で計算した。その結果を下記表1に記載した。試験はSOC(充電状態、state of charge)が50%で行った。
実施例1から4及び比較例1から3で製造された二次電池を23℃で0.5Cで10秒間充電及び放電する場合に発生する電圧差を利用して出力を計算した。このとき、比較例1の出力は45.9Wであった。比較例1を基準にして、実施例1から4及び比較例2から3の出力を百分率で計算した。その結果を下記表1に記載した。試験はSOC(充電状態、state of charge)が50%で行った。
実施例1から4及び比較例1から3のリチウム二次電池を45℃で定電流/定電圧(CC/CV)条件で4.2V/38mAまで1Cで充電したあと、定電流(CC)条件で2.5Vまで3Cで放電し、その放電容量を測定した。これを1から800サイクルで繰り返して行い、1回目のサイクルを基準に800回目のサイクルを百分率で計算(800回目の容量/1回目の容量*100(%))して測定した放電容量を表1に示した。
実施例1から4及び比較例1から3で製造された二次電池を定電流/定電圧(CC/CV)条件で4.2V/38mAまで1Cで充電したあと、定電流(CC)条件で2.5Vまで3Cで放電し、その放電容量を測定した。その後、実施例1から4及び比較例1から3で製造された二次電池を60℃で20週間保存したあと、再度前記二次電池等をそれぞれ23℃で定電流/定電圧(CC/CV)条件で4.2V/38mAまで1Cで充電してから、定電流(CC)条件で2.5Vまで3Cで放電し、その放電容量を測定した。最初の放電容量を基準に24週後の放電容量を百分率で計算(20週後の放電容量/最初の放電容量*100(%))して測定した結果を下記表1に記載した。
実施例2、4及び比較例1、2で製造された二次電池を用いて4.2Vまで充電したあと、1m/minの速度で釘で電池を貫くネイルテストを実施して安全性を評価するとともに、熱電対(thermocouple)を電池に付着して電池の温度の上昇を確認した。それぞれのネイルテスト時の電池の最大の上昇温度を下記表1に記載した。
Claims (9)
- リチウムビスフルオロスルホニルイミド(Lithium bis(fluorosulfonyl)imide;LiFSI)及びフルオロ化ベンゼン系化合物添加剤を含む非水性電解液;正極活物質としてリチウム-ニッケル-マンガン-コバルト系酸化物を含む正極;負極;及び分離膜を含むリチウム二次電池であって、
前記リチウム−ニッケル−マンガン−コバルト系酸化物は、下記化学式(1)で表される酸化物を含み、
[化学式(1)]
Li1+x(NiaCobMnc)O2
(前記化学式(1)で、0.55≦a≦0.65、0.18≦b≦0.22、0.18≦c≦0.22、-0.2≦x≦0.2及びx+a+b+c=1である。)
前記フルオロ化ベンゼン系化合物は、化学式(2)で表される化合物からなる群より選択される1種以上であり、
前記非水性電解液は、リチウム塩をさらに含み、
前記リチウム塩とリチウムビスフルオロスルホニルイミドの混合比は、モル比として1:0.01から1:1であるリチウム二次電池。 - 前記リチウムビスフルオロスルホニルイミドは、非水性電解液中の濃度が0.01mol/lから2mol/lである請求項1に記載のリチウム二次電池。
- 前記リチウム塩は、LiPF6、LiAsF6、LiCF3SO3、LiN(CF3SO2)2、LiBF 4 、LiSbF6、LiN(C2F5SO2)2、LiAlO4、LiAlCl4 、及びLiClO4からなる群より選択されるいずれか一つまたはこれらのうち2種以上の混合物を含む請求項1又は2のいずれか一項に記載のリチウム二次電池。
- 前記フルオロ化ベンゼン系化合物は、1,3,6−トリフルオロ化ベンゼンである請求項1に記載のリチウム二次電池。
- 前記フルオロ化ベンゼン系化合物添加剤の含量は、前記非水性電解液の総重量を基準に1〜20重量%である請求項1に記載のリチウム二次電池。
- 前記非水性電解液は非水性有機溶媒を含み、前記非水性有機溶媒は、ニトリル系溶媒、線形カーボネート、環状カーボネート、エステル、エーテル、ケトンまたはこれらの組み合わせを含む請求項1に記載のリチウム二次電池。
- 前記環状カーボネートは、エチレンカーボネート(EC)、プロピレンカーボネート(PC)及びブチレンカーボネート(BC)からなる群より選択されるいずれか一つまたはこれらのうち2種以上の混合物であり、線形カーボネートは、ジメチルカーボネート(DMC)、ジエチルカーボネート(DEC)、ジプロピルカーボネート(DPC)、エチルメチルカーボネート(EMC)、メチルプロピルカーボネート(MPC)及びエチルプロピルカーボネート(EPC)からなる群より選択されるいずれか一つまたはこれらのうち2種以上の混合物である請求項6に記載のリチウム二次電池。
- 前記ニトリル系溶媒は、アセトニトリル、プロピオニトリル、ブチロニトリル、バレロニトリル、カプリロニトリル、ヘプタンニトリル、シクロペンタンカルボニトリル、シクロヘキサンカルボニトリル、2−フルオロベンゾニトリル、4−フルオロベンゾニトリル、ジフルオロベンゾニトリル、トリフルオロベンゾニトリル、フェニルアセトニトリル、2−フルオロフェニルアセトニトリル、4−フルオロフェニルアセトニトリルからなる群より選択される1種以上である請求項6に記載のリチウム二次電池。
- 請求項1から請求項8のいずれか一項に記載の二次電池は、パウチ型リチウム二次電池であるリチウム二次電池。
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EP3051618B1 (en) * | 2013-09-26 | 2018-11-14 | Mitsubishi Chemical Corporation | Nonaqueous electrolyte solution and nonaqueous electrolyte battery using same |
CN103762352B (zh) | 2014-01-16 | 2016-04-06 | 东莞新能源科技有限公司 | 改性的锂镍钴锰三元正极材料及其制备方法 |
EP3176864A4 (en) | 2014-08-01 | 2018-08-15 | UBE Industries, Ltd. | Non-aqueous electrolyte and power storage device using same |
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CN107078353A (zh) | 2017-08-18 |
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JP2017528894A (ja) | 2017-09-28 |
US10276894B2 (en) | 2019-04-30 |
CN107078353B (zh) | 2019-08-16 |
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