JP6826816B2 - リチウムイオン二次電池 - Google Patents
リチウムイオン二次電池 Download PDFInfo
- Publication number
- JP6826816B2 JP6826816B2 JP2016069972A JP2016069972A JP6826816B2 JP 6826816 B2 JP6826816 B2 JP 6826816B2 JP 2016069972 A JP2016069972 A JP 2016069972A JP 2016069972 A JP2016069972 A JP 2016069972A JP 6826816 B2 JP6826816 B2 JP 6826816B2
- Authority
- JP
- Japan
- Prior art keywords
- positive electrode
- active material
- electrode active
- lithium
- negative electrode
- 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.)
- Active
Links
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims description 30
- 229910001416 lithium ion Inorganic materials 0.000 title claims description 23
- 239000007774 positive electrode material Substances 0.000 claims description 43
- 239000008151 electrolyte solution Substances 0.000 claims description 32
- 239000007773 negative electrode material Substances 0.000 claims description 28
- 239000002131 composite material Substances 0.000 claims description 27
- -1 methylene methanedisulfonic acid ester Chemical class 0.000 claims description 26
- 239000000203 mixture Substances 0.000 claims description 16
- KLARSDUHONHPRF-UHFFFAOYSA-N [Li].[Mn] Chemical compound [Li].[Mn] KLARSDUHONHPRF-UHFFFAOYSA-N 0.000 claims description 14
- 238000010248 power generation Methods 0.000 claims description 10
- 239000000654 additive Substances 0.000 claims description 8
- 239000011148 porous material Substances 0.000 claims description 8
- 230000000996 additive effect Effects 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 6
- 239000003792 electrolyte Substances 0.000 claims description 6
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 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 5
- 229910052596 spinel Inorganic materials 0.000 claims description 5
- 239000011029 spinel Substances 0.000 claims description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 24
- 238000012216 screening Methods 0.000 description 16
- 239000002253 acid Substances 0.000 description 11
- 150000001875 compounds Chemical class 0.000 description 11
- 229910002804 graphite Inorganic materials 0.000 description 11
- 239000010439 graphite Substances 0.000 description 11
- 229910052782 aluminium Inorganic materials 0.000 description 10
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 9
- 239000011230 binding agent Substances 0.000 description 9
- 229910003481 amorphous carbon Inorganic materials 0.000 description 8
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 7
- 239000012752 auxiliary agent Substances 0.000 description 7
- 239000011888 foil Substances 0.000 description 7
- 239000002033 PVDF binder Substances 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 6
- 239000011889 copper foil Substances 0.000 description 6
- 210000001787 dendrite Anatomy 0.000 description 6
- 239000010419 fine particle Substances 0.000 description 6
- RSNHXDVSISOZOB-UHFFFAOYSA-N lithium nickel Chemical compound [Li].[Ni] RSNHXDVSISOZOB-UHFFFAOYSA-N 0.000 description 6
- 239000000463 material Substances 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 6
- 239000002184 metal Substances 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical class C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 6
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 5
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 5
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 5
- 239000003575 carbonaceous material Substances 0.000 description 5
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 5
- 239000007772 electrode material Substances 0.000 description 5
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 5
- 239000011572 manganese Substances 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 239000002245 particle Substances 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
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- 229920003049 isoprene rubber Polymers 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
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- 229920005672 polyolefin resin Polymers 0.000 description 4
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 4
- 239000004810 polytetrafluoroethylene Substances 0.000 description 4
- 229920002620 polyvinyl fluoride Polymers 0.000 description 4
- 150000003839 salts Chemical class 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- 125000000020 sulfo group Chemical group O=S(=O)([*])O[H] 0.000 description 4
- 229920000049 Carbon (fiber) Polymers 0.000 description 3
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
- 239000004743 Polypropylene Substances 0.000 description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 3
- 150000001450 anions Chemical class 0.000 description 3
- 239000004917 carbon fiber Substances 0.000 description 3
- 239000001768 carboxy methyl cellulose Substances 0.000 description 3
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 3
- 210000004027 cell Anatomy 0.000 description 3
- 239000013078 crystal Substances 0.000 description 3
- 150000005676 cyclic carbonates Chemical class 0.000 description 3
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 description 3
- 150000002148 esters Chemical class 0.000 description 3
- 238000011049 filling Methods 0.000 description 3
- 229910052736 halogen Inorganic materials 0.000 description 3
- 150000002367 halogens Chemical class 0.000 description 3
- 229910052744 lithium Inorganic materials 0.000 description 3
- 229910052748 manganese Inorganic materials 0.000 description 3
- 229910021645 metal ion Inorganic materials 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 239000011255 nonaqueous electrolyte Substances 0.000 description 3
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- 239000007787 solid Substances 0.000 description 3
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- ABSXMLODUTXQDJ-UHFFFAOYSA-N 4-(4-sulfophenyl)benzenesulfonic acid Chemical compound C1=CC(S(=O)(=O)O)=CC=C1C1=CC=C(S(O)(=O)=O)C=C1 ABSXMLODUTXQDJ-UHFFFAOYSA-N 0.000 description 2
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 description 2
- XMWRBQBLMFGWIX-UHFFFAOYSA-N C60 fullerene Chemical class C12=C3C(C4=C56)=C7C8=C5C5=C9C%10=C6C6=C4C1=C1C4=C6C6=C%10C%10=C9C9=C%11C5=C8C5=C8C7=C3C3=C7C2=C1C1=C2C4=C6C4=C%10C6=C9C9=C%11C5=C5C8=C3C3=C7C1=C1C2=C4C6=C2C9=C5C3=C12 XMWRBQBLMFGWIX-UHFFFAOYSA-N 0.000 description 2
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 2
- 229920002907 Guar gum Polymers 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 2
- 229910013870 LiPF 6 Inorganic materials 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
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- 239000011149 active material Substances 0.000 description 2
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 2
- 239000003125 aqueous solvent Substances 0.000 description 2
- MIAUJDCQDVWHEV-UHFFFAOYSA-N benzene-1,2-disulfonic acid Chemical compound OS(=O)(=O)C1=CC=CC=C1S(O)(=O)=O MIAUJDCQDVWHEV-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 229910001593 boehmite Inorganic materials 0.000 description 2
- VERAMNDAEAQRGS-UHFFFAOYSA-N butane-1,4-disulfonic acid Chemical compound OS(=O)(=O)CCCCS(O)(=O)=O VERAMNDAEAQRGS-UHFFFAOYSA-N 0.000 description 2
- 239000002134 carbon nanofiber Substances 0.000 description 2
- 229910021393 carbon nanotube Inorganic materials 0.000 description 2
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- 239000000919 ceramic Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
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- AFAXGSQYZLGZPG-UHFFFAOYSA-N ethanedisulfonic acid Chemical compound OS(=O)(=O)CCS(O)(=O)=O AFAXGSQYZLGZPG-UHFFFAOYSA-N 0.000 description 2
- 229910003472 fullerene Inorganic materials 0.000 description 2
- 230000004927 fusion Effects 0.000 description 2
- 150000004676 glycans Chemical class 0.000 description 2
- 239000000665 guar gum Substances 0.000 description 2
- 235000010417 guar gum Nutrition 0.000 description 2
- 229960002154 guar gum Drugs 0.000 description 2
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 2
- 239000003273 ketjen black Substances 0.000 description 2
- 239000005001 laminate film Substances 0.000 description 2
- 230000014759 maintenance of location Effects 0.000 description 2
- OPUAWDUYWRUIIL-UHFFFAOYSA-N methanedisulfonic acid Chemical compound OS(=O)(=O)CS(O)(=O)=O OPUAWDUYWRUIIL-UHFFFAOYSA-N 0.000 description 2
- YZMHQCWXYHARLS-UHFFFAOYSA-N naphthalene-1,2-disulfonic acid Chemical compound C1=CC=CC2=C(S(O)(=O)=O)C(S(=O)(=O)O)=CC=C21 YZMHQCWXYHARLS-UHFFFAOYSA-N 0.000 description 2
- 229920001277 pectin Polymers 0.000 description 2
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- 239000000843 powder Substances 0.000 description 2
- MGNVWUDMMXZUDI-UHFFFAOYSA-N propane-1,3-disulfonic acid Chemical compound OS(=O)(=O)CCCS(O)(=O)=O MGNVWUDMMXZUDI-UHFFFAOYSA-N 0.000 description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 2
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 239000000230 xanthan gum Substances 0.000 description 2
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- LIKMAJRDDDTEIG-UHFFFAOYSA-N 1-hexene Chemical compound CCCCC=C LIKMAJRDDDTEIG-UHFFFAOYSA-N 0.000 description 1
- JPLNAQJTXYXDAV-UHFFFAOYSA-N 4,4,5-trichloro-1,3-dioxolan-2-one Chemical compound ClC1OC(=O)OC1(Cl)Cl JPLNAQJTXYXDAV-UHFFFAOYSA-N 0.000 description 1
- CRJXZTRTJWAKMU-UHFFFAOYSA-N 4,4,5-trifluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1(F)F CRJXZTRTJWAKMU-UHFFFAOYSA-N 0.000 description 1
- HIGQQEOWQNDHJD-UHFFFAOYSA-N 4,4-dichloro-1,3-dioxolan-2-one Chemical compound ClC1(Cl)COC(=O)O1 HIGQQEOWQNDHJD-UHFFFAOYSA-N 0.000 description 1
- DSMUTQTWFHVVGQ-UHFFFAOYSA-N 4,5-difluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1F DSMUTQTWFHVVGQ-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
- 239000005995 Aluminium silicate Substances 0.000 description 1
- 229910000873 Beta-alumina solid electrolyte Inorganic materials 0.000 description 1
- 229910013063 LiBF 4 Inorganic materials 0.000 description 1
- 229910014689 LiMnO Inorganic materials 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- QJFSQWZVVOVYEZ-UHFFFAOYSA-N [Li+].[Li+].[Co++].[O-][Mn]([O-])(=O)=O.[O-][Mn]([O-])(=O)=O Chemical compound [Li+].[Li+].[Co++].[O-][Mn]([O-])(=O)=O.[O-][Mn]([O-])(=O)=O QJFSQWZVVOVYEZ-UHFFFAOYSA-N 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
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- 125000000129 anionic group Chemical group 0.000 description 1
- 229910052586 apatite Inorganic materials 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
- 229910002113 barium titanate Inorganic materials 0.000 description 1
- UXXXZMDJQLPQPH-UHFFFAOYSA-N bis(2-methylpropyl) carbonate Chemical compound CC(C)COC(=O)OCC(C)C UXXXZMDJQLPQPH-UHFFFAOYSA-N 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 150000005678 chain carbonates Chemical class 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
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- QLVWOKQMDLQXNN-UHFFFAOYSA-N dibutyl carbonate Chemical compound CCCCOC(=O)OCCCC QLVWOKQMDLQXNN-UHFFFAOYSA-N 0.000 description 1
- LANCTRRJXQFVPH-UHFFFAOYSA-L dilithium;methanedisulfonate Chemical compound [Li+].[Li+].[O-]S(=O)(=O)CS([O-])(=O)=O LANCTRRJXQFVPH-UHFFFAOYSA-L 0.000 description 1
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- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 description 1
- VUPKGFBOKBGHFZ-UHFFFAOYSA-N dipropyl carbonate Chemical compound CCCOC(=O)OCCC VUPKGFBOKBGHFZ-UHFFFAOYSA-N 0.000 description 1
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- 239000006185 dispersion Substances 0.000 description 1
- ODCCJTMPMUFERV-UHFFFAOYSA-N ditert-butyl carbonate Chemical compound CC(C)(C)OC(=O)OC(C)(C)C ODCCJTMPMUFERV-UHFFFAOYSA-N 0.000 description 1
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- 229910021385 hard carbon Inorganic materials 0.000 description 1
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- 229910052742 iron Inorganic materials 0.000 description 1
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 1
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- 229910052745 lead Inorganic materials 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
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- 159000000002 lithium salts Chemical class 0.000 description 1
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- OPUAWDUYWRUIIL-UHFFFAOYSA-L methanedisulfonate Chemical compound [O-]S(=O)(=O)CS([O-])(=O)=O OPUAWDUYWRUIIL-UHFFFAOYSA-L 0.000 description 1
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- PFPYHYZFFJJQFD-UHFFFAOYSA-N oxalic anhydride Chemical compound O=C1OC1=O PFPYHYZFFJJQFD-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- VSIIXMUUUJUKCM-UHFFFAOYSA-D pentacalcium;fluoride;triphosphate Chemical compound [F-].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O VSIIXMUUUJUKCM-UHFFFAOYSA-D 0.000 description 1
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- 239000002244 precipitate Substances 0.000 description 1
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- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
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- 239000010457 zeolite Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
- 239000004711 α-olefin Substances 0.000 description 1
Images
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
- H01M50/105—Pouches or flexible bags
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
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Description
リチウム・ニッケル系複合酸化物(ニッケル・コバルト・マンガン酸リチウム(「NCM433」、すなわちニッケル:コバルト:マンガン=4:3:3))と、スピネル構造を有するリチウム・マンガン系複合酸化物(Li1.1Mn1.9O4の粉末)とを、表1に記載の割合で混合したものと、導電助剤としてカーボンブラック粉末(CB)と、バインダー樹脂としてPVDF(クレハ製、#7200)とを、固形分質量比で複合酸化物:CB:PVDFが93:4:3の割合となるように混合し、溶媒であるNMPに添加した。さらに、この混合物に有機系水分捕捉剤として無水シュウ酸(分子量90)を、上記混合物からNMPを除いた固形分100質量部に対して0.03質量部添加した上で遊星方式の分散混合を30分間実施することで、これらの材料を均一に分散させてスラリーを作製した。得られたスラリーを、正極集電体となる厚み20μmのアルミニウム箔上に乾燥後重量が片面あたり20mg/cm2となるように塗布した。次いで、125℃にて10分間、電極を加熱し、NMPを蒸発させることにより正極活物質層を形成した。さらに、正極活物質層の空孔率が25%となるように電極をプレスして、正極集電体の片面上に厚さ63μmの正極活物質層を塗布した正極を作製した。
負極活物質として、非晶質炭素で被覆された粒子状黒鉛粉末(平均粒子径20μm)を用いた。この黒鉛粉末と、導電助剤としてCBとを、バインダー樹脂であるスチレンブタジエンラバーとカルボキシメチルセルロースとの水溶液に、固形分質量比が黒鉛粉末:導電助剤:バインダー=96.7:0.3:3の割合となるように均一に混合してスラリーを作製した。得られたスラリーを、負極集電体となる厚み10μmの銅箔上に乾燥後重量が片面あたり16mg/cm2となるように塗布した。次いで、125℃にて10分間、電極を加熱し、水を蒸発させることにより負極活物質層を形成した。さらに、負極活物質層の空孔率が33%となるように電極をプレスして、負極集電体の片面上に厚さ62μmの負極活物質層を塗布した負極を作製した。
耐熱微粒子としてベーマイトを用いた耐熱微粒子層とポリプロピレンおよびポリエチレンからなる厚さ18μmのオレフィン系樹脂層都から構成される、全体の厚さが25μm、空孔率が55%のセラミックセパレータを使用した。
エチレンカーボネート(EC)、ジエチルカーボネート(DEC)、およびエチルメチルカーボネート(EMC)とを、EC:DEC:EMC=30:60:10の体積比で混合した非水溶媒を用意した。この混合非水溶媒に電解質塩としての六フッ化リン酸リチウム(LiPF6)を濃度が0.9mol/Lとなるように溶解させ、次いで、添加剤としてMMDS、VCおよびFEC(MMDS:VC:FEC=:1:1:1)を、これらの合計濃度が3重量%となるように溶解させた。
上記のように作製した正極ならびに負極を、各活物質が塗布されていない集電体延長部が残るようにサイズ220mm×190mmの矩形に切り出して正極版と負極板とを用意した。セパレータの両面に上記負極板と正極板とを両活物質層がセパレータを隔てて重なるように配置したものを20層重ね電極積層体を得た。そして、負極板の負極集電体延長部に対し負極端子の内側端(一端部)を接合した。同様に正極板の正極集電体延長部にたいし正極端子の内側端(一端部)を接合した。この電極板積層体を外装体となる2枚のアルミニウムラミネートフィルムで包み、比較的小さな充填孔のみを残して周囲の四辺を熱融着により接着した。次いで、後に行うスクリーニング検出性試験時に電解液量が表1に示すような体積割合となるように、充填高から電解液を注入した。なお四辺のうち一辺は正極端子および負極端子を引き出した状態でアルミニウムラミネートフィルムの熱融着を行った。この熱融着部と電極板積層体との距離は、端子引き出し辺においては15mm、それ以外の辺においては5mmとした。電解液を注入した後に外装体内部を真空含浸させ、減圧して充填孔を熱融着により封止して、積層型リチウムイオン電池を作成した。この積層型リチウムイオン電池の初充電を行った後、45℃でエージングを数日間行い、各実施例ならびに比較例の積層型リチウムイオン電池を得た。
電極の空孔率は、材料の真密度と部材厚み、塗布量、混合比より算出した。セパレータの空孔率は、材料の真密度と部材厚みより算出した。
上記の通り作製した電池を、温度45℃環境下で、充電:1C電流、上限電圧4.15Vでの定電流定電圧充電、放電:1C電流、下限電圧2.5V終止で定電流放電の充放電サイクルを1000回繰り返した。1000サイクル後の放電容量維持率(%)を測定した。
電池の作製時に、正極に銅箔切断屑(サイズ10μm×10μm×1mm)を固定した正極を用いた電池を別途作製した。スクリーニング検出性試験用電池の残容量(SOC)を5%となるまで充電し、2つのスペーサ板の間に挟んだ。この状態で2つのスペーサに荷重を加え、電池の外装体が弾性変形を生じるまで押圧し、この状態で電池の電圧を測定した。25℃で4日間加圧状態を保った後、再び電池の電圧を測定し、加圧時の電圧低下量を算出した。一方銅箔切断屑を固定しない電池についても同様の試験を行って電圧低下量を算出し、銅箔切断屑を固定した電池の電圧低下量が有意に大きい場合、この電池を「検出可」と評価した。一方、銅箔切断屑を固定しない電池と、これを固定しない電池とで電圧低下量に有意な差が見られない場合、この電池を「検出不可」と評価した。
11 負極集電体
12 正極集電体
13 負極活物質層
15 正極活物質層
17 セパレータ
25 負極リード
27 正極リード
29 外装体
31 電解液
Claims (5)
- 正極活物質層が正極集電体に配置された正極と、
負極活物質層が負極集電体に配置された負極と、
セパレータと、
電解液と、
を含む発電要素を、外装体内部に含む、ラミネート型のリチウムイオン二次電池であって、
該正極活物質層が、リチウムニッケルコバルトマンガン複合酸化物のみ、または、スピネル構造を有するリチウム・マンガン系複合酸化物とリチウムニッケルコバルトマンガン複合酸化物との混合物から構成され、該リチウム・マンガン系複合酸化物が正極活物質の重量に対して50重量%以下である、該混合物を含み、
該発電要素中に含まれる該電解液の体積が、該正極活物質層、該負極活物質層および該セパレータに存在する空孔の体積の合計の値に対して1.15〜1.35倍である、
前記リチウムイオン二次電池。 - 該正極活物質層が、リチウムニッケルコバルトマンガン複合酸化物のみ、または、スピネル構造を有するリチウム・マンガン系複合酸化物とリチウムニッケルコバルトマンガン複合酸化物との混合物から構成され、該リチウム・マンガン系複合酸化物が正極活物質の重量に対して30重量%以下である、該混合物を含み、
該発電要素中に含まれる該電解液の体積が、該正極活物質層、該負極活物質層および該セパレータに存在する空孔の体積の合計の値に対して1.15〜1.30倍である、請求項1に記載のリチウムイオン二次電池。 - 前記正極活物質層が、スピネル構造を有するリチウム・マンガン系複合酸化物が30重量%と、リチウムニッケルコバルトマンガン複合酸化物が70重量%との混合物から構成される、
請求項2に記載のリチウムイオン二次電池。 - 該正極および該負極の面積が75cm2以上である、請求項1〜3のいずれかに記載のリチウムイオン二次電池。
- 該電解液が、メチレンメタンジスルホン酸エステル、ビニレンカーボネート、フルオロエチレンカーボネートおよびこれらの混合物からなる群より選択される添加剤を含む、請求項1〜4のいずれかに記載のリチウムイオン二次電池。
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