JPWO2006009177A1 - リチウム二次電池用正極活物質及びその製造方法 - Google Patents
リチウム二次電池用正極活物質及びその製造方法 Download PDFInfo
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- JPWO2006009177A1 JPWO2006009177A1 JP2006529249A JP2006529249A JPWO2006009177A1 JP WO2006009177 A1 JPWO2006009177 A1 JP WO2006009177A1 JP 2006529249 A JP2006529249 A JP 2006529249A JP 2006529249 A JP2006529249 A JP 2006529249A JP WO2006009177 A1 JPWO2006009177 A1 JP WO2006009177A1
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- Prior art keywords
- positive electrode
- electrode active
- active material
- lithium
- secondary battery
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- 239000007774 positive electrode material Substances 0.000 title claims abstract description 66
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 43
- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 43
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 13
- 229910052719 titanium Inorganic materials 0.000 claims abstract description 20
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910001416 lithium ion Inorganic materials 0.000 claims abstract description 13
- 239000002245 particle Substances 0.000 claims description 52
- 239000011777 magnesium Substances 0.000 claims description 43
- 229910052782 aluminium Inorganic materials 0.000 claims description 36
- 239000002994 raw material Substances 0.000 claims description 29
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 25
- 229910052749 magnesium Inorganic materials 0.000 claims description 24
- 239000002131 composite material Substances 0.000 claims description 23
- 239000000203 mixture Substances 0.000 claims description 23
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical group [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 22
- -1 cobalt oxyhydroxide Chemical compound 0.000 claims description 22
- CKFRRHLHAJZIIN-UHFFFAOYSA-N cobalt lithium Chemical compound [Li].[Co] CKFRRHLHAJZIIN-UHFFFAOYSA-N 0.000 claims description 20
- 239000010941 cobalt Substances 0.000 claims description 16
- 229910017052 cobalt Inorganic materials 0.000 claims description 15
- 239000000463 material Substances 0.000 claims description 15
- 229910021503 Cobalt(II) hydroxide Inorganic materials 0.000 claims description 14
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 13
- ASKVAEGIVYSGNY-UHFFFAOYSA-L cobalt(ii) hydroxide Chemical compound [OH-].[OH-].[Co+2] ASKVAEGIVYSGNY-UHFFFAOYSA-L 0.000 claims description 13
- 229910052731 fluorine Inorganic materials 0.000 claims description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 8
- 239000001301 oxygen Substances 0.000 claims description 8
- 229910052760 oxygen Inorganic materials 0.000 claims description 8
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims description 7
- 239000011737 fluorine Substances 0.000 claims description 7
- 229910052758 niobium Inorganic materials 0.000 claims description 7
- 239000006104 solid solution Substances 0.000 claims description 6
- 239000011149 active material Substances 0.000 claims description 3
- 239000000126 substance Substances 0.000 claims description 3
- 238000001354 calcination Methods 0.000 claims description 2
- 239000000843 powder Substances 0.000 description 61
- 239000010936 titanium Substances 0.000 description 24
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 20
- 238000000034 method Methods 0.000 description 20
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 13
- 238000010304 firing Methods 0.000 description 13
- 238000004458 analytical method Methods 0.000 description 11
- 230000020169 heat generation Effects 0.000 description 11
- 229910013733 LiCo Inorganic materials 0.000 description 10
- 230000014759 maintenance of location Effects 0.000 description 10
- 229910052757 nitrogen Inorganic materials 0.000 description 10
- 238000001179 sorption measurement Methods 0.000 description 10
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 9
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 8
- 238000002441 X-ray diffraction Methods 0.000 description 8
- 230000001133 acceleration Effects 0.000 description 8
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical compound [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 description 8
- 230000000694 effects Effects 0.000 description 7
- 238000005259 measurement Methods 0.000 description 7
- 238000011056 performance test Methods 0.000 description 7
- 230000000704 physical effect Effects 0.000 description 7
- 239000011164 primary particle Substances 0.000 description 7
- 239000011163 secondary particle Substances 0.000 description 7
- 239000002002 slurry Substances 0.000 description 7
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 6
- 102100025490 Slit homolog 1 protein Human genes 0.000 description 6
- 101710123186 Slit homolog 1 protein Proteins 0.000 description 6
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 6
- 239000003792 electrolyte Substances 0.000 description 6
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 6
- 239000010955 niobium Substances 0.000 description 6
- 238000001228 spectrum Methods 0.000 description 6
- 125000001153 fluoro group Chemical group F* 0.000 description 5
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 description 5
- 239000000347 magnesium hydroxide Substances 0.000 description 5
- 229910001862 magnesium hydroxide Inorganic materials 0.000 description 5
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 229910052808 lithium carbonate Inorganic materials 0.000 description 4
- 239000007787 solid Substances 0.000 description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 3
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 3
- MXRIRQGCELJRSN-UHFFFAOYSA-N O.O.O.[Al] Chemical compound O.O.O.[Al] MXRIRQGCELJRSN-UHFFFAOYSA-N 0.000 description 3
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 239000013078 crystal Substances 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 239000008151 electrolyte solution Substances 0.000 description 3
- 239000011888 foil Substances 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 239000007773 negative electrode material Substances 0.000 description 3
- 239000011255 nonaqueous electrolyte Substances 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- 239000006230 acetylene black Substances 0.000 description 2
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 2
- 229910021529 ammonia Inorganic materials 0.000 description 2
- 229910052786 argon Inorganic materials 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 229920001577 copolymer Polymers 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 2
- 150000004679 hydroxides Chemical class 0.000 description 2
- 229910003002 lithium salt Inorganic materials 0.000 description 2
- 159000000002 lithium salts Chemical class 0.000 description 2
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 2
- 239000001095 magnesium carbonate Substances 0.000 description 2
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 239000005518 polymer electrolyte Substances 0.000 description 2
- 229920001155 polypropylene Polymers 0.000 description 2
- 239000004810 polytetrafluoroethylene Substances 0.000 description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 2
- 239000012266 salt solution Substances 0.000 description 2
- 238000004544 sputter deposition Methods 0.000 description 2
- 229910052715 tantalum Inorganic materials 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- IRPGOXJVTQTAAN-UHFFFAOYSA-N 2,2,3,3,3-pentafluoropropanal Chemical compound FC(F)(F)C(F)(F)C=O IRPGOXJVTQTAAN-UHFFFAOYSA-N 0.000 description 1
- 229920000178 Acrylic resin Polymers 0.000 description 1
- 239000004925 Acrylic resin Substances 0.000 description 1
- KLZUFWVZNOTSEM-UHFFFAOYSA-K Aluminum fluoride Inorganic materials F[Al](F)F KLZUFWVZNOTSEM-UHFFFAOYSA-K 0.000 description 1
- 229910017008 AsF 6 Inorganic materials 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 229910020366 ClO 4 Inorganic materials 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910000733 Li alloy Inorganic materials 0.000 description 1
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 239000004952 Polyamide Substances 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 229910018286 SbF 6 Inorganic materials 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 229910021383 artificial graphite Inorganic materials 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- INAHAJYZKVIDIZ-UHFFFAOYSA-N boron carbide Chemical class B12B3B4C32B41 INAHAJYZKVIDIZ-UHFFFAOYSA-N 0.000 description 1
- 239000002775 capsule Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 150000001722 carbon compounds Chemical class 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 150000005678 chain carbonates Chemical class 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 150000003841 chloride salts Chemical class 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 229910000428 cobalt oxide Inorganic materials 0.000 description 1
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 150000005676 cyclic carbonates Chemical class 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 230000001351 cycling effect 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
- 239000002612 dispersion medium Substances 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 125000002573 ethenylidene group Chemical group [*]=C=C([H])[H] 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 239000012025 fluorinating agent Substances 0.000 description 1
- 150000002222 fluorine compounds Chemical class 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000001989 lithium alloy Substances 0.000 description 1
- ORUIBWPALBXDOA-UHFFFAOYSA-L magnesium fluoride Chemical compound [F-].[F-].[Mg+2] ORUIBWPALBXDOA-UHFFFAOYSA-L 0.000 description 1
- 229910001635 magnesium fluoride Inorganic materials 0.000 description 1
- 229910001512 metal fluoride Inorganic materials 0.000 description 1
- RCIJMMSZBQEWKW-UHFFFAOYSA-N methyl propan-2-yl carbonate Chemical compound COC(=O)OC(C)C RCIJMMSZBQEWKW-UHFFFAOYSA-N 0.000 description 1
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910000484 niobium oxide Inorganic materials 0.000 description 1
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 1
- 150000002823 nitrates Chemical class 0.000 description 1
- 150000007524 organic acids Chemical class 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 230000000737 periodic effect Effects 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 229920000573 polyethylene Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- 239000002689 soil Substances 0.000 description 1
- 238000010532 solid phase synthesis reaction Methods 0.000 description 1
- 239000012798 spherical particle Substances 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 229910001936 tantalum oxide Inorganic materials 0.000 description 1
- 238000012360 testing method Methods 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
- VXYADVIJALMOEQ-UHFFFAOYSA-K tris(lactato)aluminium Chemical compound CC(O)C(=O)O[Al](OC(=O)C(C)O)OC(=O)C(C)O VXYADVIJALMOEQ-UHFFFAOYSA-K 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
- H01M4/52—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
-
- 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/582—Halogenides
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Composite Materials (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
Description
さらに、本発明者は、上記のTi、Nb、及び/又はTaを、粒子状のコバルト酸リチウム系複合酸化物の表面に存在させることにより、これらの含有元素による効果が効果的に作用するのでさらに好ましいことを見出した。
(1)一般式(1):LiaCobAlcMgdAeOfFg(式中、AはTi、Nb、又はTa、0.90≦a≦1.10、0.97≦b≦1.00、0.0001≦c≦0.02、0.0001≦d≦0.02、0.0001≦e≦0.01、1.98≦f≦2.02、0≦g≦0.02、0.0003≦c+d+e≦0.03)で表される粒子状のリチウムコバルト系複合酸化物を含むことを特徴とするリチウム二次電池用正極活物質。
(2)一般式(1)において、さらに、0.5≦c/d≦2であり、かつ0.002≦c+d≦0.025である上記(1)に記載のリチウム二次電池用正極活物質。
(3)一般式(1)において、さらに、0.01≦e/d≦1であり、かつ0.002≦e+d≦0.02である上記(1)又は(2)に記載のリチウム二次電池用正極活物質。(4)元素Aが、粒子状のリチウムコバルト系複合酸化物の表面に偏在している上記(1)ないし(3)のいずれかに記載のリチウム二次電池用正極活物質。
(5)元素Fが、粒子状のリチウムコバルト系複合酸化物の表面に存在している上記(1)ないし(4)のいずれか1項に記載のリチウム二次電池用正極活物質。
(6)Al、Mg及びAで表される元素の少なくとも一部がリチウムコバルト系複合酸化物粒子のコバルト原子を置換した固溶体である上記(1)ないし(5)のいずれか1項に記載のリチウム二次電池用正極活物質。
(7)単独酸化物として含有されるAlが、リチウムコバルト系複合酸化物に含有される全Alの20モル%以下である上記(1)ないし(6)のいずれかに記載のリチウム二次電池用正極活物質。
(8)粒子状のリチウムコバルト系複合酸化物が、プレス密度3.0〜3.4g/cm3を有する上記(1)〜(7)のいずれかに記載のリチウム二次電池用正極活物質。
(9)一般式(1):LiaCobAlcMgdAeOfFg(式中、AはTi、Nb、又はTa、0.90≦a≦1.10、0.97≦b≦1.00、0.0001≦c≦0.02、0.0001≦d≦0.02、0.0001≦e≦0.01、1.98≦f≦2.02、0≦g≦0.02、0.0003≦c+d+e≦0.03)で表される粒子状のリチウムイオン二次電池用正極活物質で表される粒子状のリチウムコバルト系複合酸化物からなるリチウムイオン二次電池用正極活物質の製造方法であって、少なくともオキシ水酸化コバルト、四三酸化コバルト、又は水酸化コバルトのいずれか含むコバルト原料と、リチウム原料と、アルミニウム原料と、マグネシウム原料と、元素A原料と、必要に応じてフッ素原料との混合物を800〜1050℃の酸素含有雰囲気で焼成することを特徴とするリチウム二次電池用正極活物質の製造方法。
(10)アルミニウム原料、マグネシウム原料及び元素A原料の少なくとも1種を溶液状として、少なくともコバルト原料と混合する上記(9)に記載のリチウム二次電池用正極活物質の製造方法。
一般式(1)で、A、a、b、c、d、及びeは上記したとおりである。a及びbの上記範囲が外れると放電容量が低下したり、充放電サイクル耐久性が低下するので好ましくない。c、d及びeがそれらの下限値を下回ると、安全性、放電電圧、充放電サイクル耐久性の向上効果が低下するので好ましくない。c、d、e及びgがそれらの上限値を上回ると放電容量が低下するので好ましくない。なかでも、Aは、チタンが好ましく、また、c、d、e及びgの特に好ましい範囲は、0.0003≦c≦0.01、0.0003≦d≦0.01、0.0002≦e≦0.007、0≦g≦0.01、0.0005≦c+d+e≦0.02である。
一次粒子が50個以上凝集して二次粒子を形成した平均粒径D50が13.2μmの水酸化コバルト粉末と、平均粒径15μmの炭酸リチウム粉末と、粒径1.5μmの水酸化アルミニウム粉末と、平均粒径3.7μmの水酸化マグネシウム粉末と、平均粒径0.6μmの酸化チタン粉末を所定量混合した。これら4種の粉末を乾式混合した後、大気中、400℃で3時間焼成した後、950℃にて10時間焼成した。焼成後の粉末を湿式溶解し、ICP及び原子吸光分析により、コバルト、アルミニウム、マグネシウム、チタン及びリチウムの含量を測定した結果、粉末の組成はLiCo0.9975Al0.001Mg0.001Ti0.0005O2であった。
酸化チタンを使用する代わりに、酸化ニオブを用いた他は実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCo0.9975Al0.001Mg0.001Nb0.0005O2であった。
酸化チタンを使用する代わりに、酸化タンタルを用いた他は実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCo0.9975Al0.001Mg0.001Ta0.0005O2であった。
一次粒子が50個以上凝集して二次粒子を形成した平均粒径D50が10.7μmのオキシ水酸化コバルト粉末と、炭酸リチウム粉末と、水酸化アルミニウム粉末と、水酸化マグネシウム粉末と、酸化チタン粉末と、フッ化リチウム粉末を所定量混合した他は実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCo0.9975Al0.001Mg0.001Ti0.0005O1.993F0.007であ
った。
水酸化アルミニウム粉末と、水酸化マグネシウム粉末と、酸化チタン粉末を使用しなかった他は、実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCoO2であった。
酸化チタンを使用しなかった他は、実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCo0.998Al0.001Mg0.001O2であった。
水酸化マグネシウムを使用しなかった他は、実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCo0.9985Al0.001Ti0.0005O2であった。
水酸化アルミニウムと水酸化マグネシウムと酸化チタンの添加量を変えた他は実施例1と同様な方法で正極活物質を合成し、組成分析と物性測定ならびに電池性能試験を行った。その結果、組成はLiCo0.9952Al0.002Mg0.002Ti0.0008O2であった。
炭酸マグネシウム粉末1.97gとクエン酸2.88gと水133.20gを添加し、アンモニアを1.50g添加することにより、pH9.5のマグネシウムが均一に溶解したカルボン酸からなる塩の水溶液を得た。上記水溶液を、平均粒径D50が13.5μm、D10が5.5μm、D90が18.1μmである水酸化コバルト193.4gに加えてスラリー状にした。スラリー中の固形分濃度は76重量%であった。
このスラリーを120℃で2時間、乾燥機にて脱水して、マグネシウム添加水酸化コバルト粉末を得た。
炭酸マグネシウム粉末1.97gと乳酸アルミニウム3.13gとクエン酸5.34gと水130.07gを添加し、アンモニアを1.50g添加することにより、pH9.5のマグネシウムとアルミニウムが均一に溶解したカルボン酸からなる塩の水溶液を得た。上記水溶液を、平均粒径D50が13.5μm、D10が5.5μm、D90が18.1μmである水酸化コバルト195.0gに加えてスラリー状にした。スラリー中の固形分濃度は76重量%であった。
なお、2004年7月20日に出願された日本特許出願2004−212078号の明細書、特許請求の範囲、図面及び要約書の全内容をここに引用し、本発明の明細書の開示として、取り入れるものである。
Claims (10)
- 一般式(1):LiaCobAlcMgdAeOfFg(式中、AはTi、Nb、又はTa、0.90≦a≦1.10、0.97≦b≦1.00、0.0001≦c≦0.02、0.0001≦d≦0.02、0.0001≦e≦0.01、1.98≦f≦2.02、0≦g≦0.02、0.0003≦c+d+e≦0.03)で表される粒子状のリチウムコバルト系複合酸化物を含むことを特徴とするリチウム二次電池用正極活物質。
- 一般式(1)において、さらに、0.5≦c/d≦2であり、かつ0.002≦c+d≦0.025である請求項1に記載のリチウム二次電池用正極活物質。
- 一般式(1)において、さらに、0.01≦e/d≦1であり、かつ0.002≦e+d≦0.02である請求項1又は2に記載のリチウム二次電池用正極活物質。
- 元素Aが、粒子状のリチウムコバルト系複合酸化物の表面に存在している請求項1ないし3のいずれか1項に記載のリチウム二次電池用正極活物質。
- 元素Fが、粒子状のリチウムコバルト系複合酸化物の表面に存在している請求項1ないし4のいずれか1項に記載のリチウム二次電池用正極活物質。
- Al、Mg及びAで表される元素の少なくとも一部がリチウムコバルト系複合酸化物粒子のコバルト原子を置換した固溶体である請求項1ないし5のいずれか1項に記載のリチウム二次電池用正極活物質。
- 単独酸化物として含有されるAlが、リチウムコバルト系複合酸化物に含有される全Alの20モル%以下である請求項1ないし6のいずれか1項に記載のリチウム二次電池用正極活物質。
- 粒子状のリチウムコバルト系複合酸化物が、プレス密度3.0〜3.4g/cm3を有する請求項1ないし7のいずれかに記載のリチウム二次電池用正極活物質。
- 一般式(1):LiaCobAlcMgdAeOfFg(式中、AはTi、Nb、又はTa、0.90≦a≦1.10、0.97≦b≦1.00、0.0001≦c≦0.02、0.0001≦d≦0.02、0.0001≦e≦0.01、1.98≦f≦2.02、0≦g≦0.02、0.0003≦c+d+e≦0.03)で表される粒子状のリチウムイオン二次電池用正極活物質で表される粒子状のリチウムコバルト系複合酸化物からなるリチウムイオン二次電池用正極活物質の製造方法であって、少なくともオキシ水酸化コバルト、四三酸化コバルト、又は水酸化コバルトのいずれかを含むコバルト原料と、リチウム原料と、アルミニウム原料と、マグネシウム原料と、元素A原料と、必要に応じてフッ素原料との混合物を800〜1050℃の酸素含有雰囲気で焼成することを特徴とするリチウム二次電池用正極活物質の製造方法。
- アルミニウム原料、マグネシウム原料及び元素A原料の少なくとも1種を溶液状として、少なくともコバルト原料と混合する請求項9に記載のリチウム二次電池用正極活物質の製造方法。
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KR20070033337A (ko) | 2007-03-26 |
US20070117014A1 (en) | 2007-05-24 |
JP5080808B2 (ja) | 2012-11-21 |
CN1981396A (zh) | 2007-06-13 |
WO2006009177A1 (ja) | 2006-01-26 |
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