JP5279756B2 - リチウム2次電池用負極及びこれを含むリチウム2次電池 - Google Patents
リチウム2次電池用負極及びこれを含むリチウム2次電池 Download PDFInfo
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- JP5279756B2 JP5279756B2 JP2010097881A JP2010097881A JP5279756B2 JP 5279756 B2 JP5279756 B2 JP 5279756B2 JP 2010097881 A JP2010097881 A JP 2010097881A JP 2010097881 A JP2010097881 A JP 2010097881A JP 5279756 B2 JP5279756 B2 JP 5279756B2
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- PCEVCXPUGOBVFG-UHFFFAOYSA-N 5,6-dichloro-5-methylcyclohexa-1,3-diene Chemical compound CC1(Cl)C=CC=CC1Cl PCEVCXPUGOBVFG-UHFFFAOYSA-N 0.000 description 1
- CMTFMQAGUXZMHD-UHFFFAOYSA-N 5,6-difluoro-5-methylcyclohexa-1,3-diene Chemical compound CC1(F)C=CC=CC1F CMTFMQAGUXZMHD-UHFFFAOYSA-N 0.000 description 1
- DTWXIVZRKZIBPP-UHFFFAOYSA-N 5,6-diiodo-5-methylcyclohexa-1,3-diene Chemical compound CC1(I)C=CC=CC1I DTWXIVZRKZIBPP-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
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- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 229910017767 Cu—Al Inorganic materials 0.000 description 1
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 1
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 1
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 1
- 229910010238 LiAlCl 4 Inorganic materials 0.000 description 1
- 229910010090 LiAlO 4 Inorganic materials 0.000 description 1
- 229910015015 LiAsF 6 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
- 229910010707 LiFePO 4 Inorganic materials 0.000 description 1
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 1
- 229910013716 LiNi Inorganic materials 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- 229910012513 LiSbF 6 Inorganic materials 0.000 description 1
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 1
- MKYBYDHXWVHEJW-UHFFFAOYSA-N N-[1-oxo-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propan-2-yl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(C(C)NC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 MKYBYDHXWVHEJW-UHFFFAOYSA-N 0.000 description 1
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 1
- 239000004677 Nylon Substances 0.000 description 1
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- 229920000265 Polyparaphenylene Polymers 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- JYVXNLLUYHCIIH-ZCFIWIBFSA-N R-mevalonolactone, (-)- Chemical compound C[C@@]1(O)CCOC(=O)C1 JYVXNLLUYHCIIH-ZCFIWIBFSA-N 0.000 description 1
- 229910004219 SiNi Inorganic materials 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910001128 Sn alloy Inorganic materials 0.000 description 1
- 229920005993 acrylate styrene-butadiene rubber polymer Polymers 0.000 description 1
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- YCOXTKKNXUZSKD-UHFFFAOYSA-N as-o-xylenol Natural products CC1=CC=C(O)C=C1C YCOXTKKNXUZSKD-UHFFFAOYSA-N 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- KCXMKQUNVWSEMD-UHFFFAOYSA-N benzyl chloride Chemical compound ClCC1=CC=CC=C1 KCXMKQUNVWSEMD-UHFFFAOYSA-N 0.000 description 1
- 239000004917 carbon fiber Substances 0.000 description 1
- 239000003660 carbonate based solvent Substances 0.000 description 1
- NKCVNYJQLIWBHK-UHFFFAOYSA-N carbonodiperoxoic acid Chemical compound OOC(=O)OO NKCVNYJQLIWBHK-UHFFFAOYSA-N 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000005466 carboxylated polyvinylchloride Substances 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 210000004027 cell Anatomy 0.000 description 1
- 229920002678 cellulose Polymers 0.000 description 1
- 239000001913 cellulose 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
- 238000001816 cooling Methods 0.000 description 1
- 229920001577 copolymer Polymers 0.000 description 1
- 125000004122 cyclic group Chemical group 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 150000004862 dioxolanes Chemical class 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
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- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 1
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- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 125000001188 haloalkyl group Chemical group 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 150000002430 hydrocarbons Chemical group 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- SNHMUERNLJLMHN-UHFFFAOYSA-N iodobenzene Chemical compound IC1=CC=CC=C1 SNHMUERNLJLMHN-UHFFFAOYSA-N 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000005304 joining Methods 0.000 description 1
- UIDWHMKSOZZDAV-UHFFFAOYSA-N lithium tin Chemical compound [Li].[Sn] UIDWHMKSOZZDAV-UHFFFAOYSA-N 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 229940057061 mevalonolactone Drugs 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- PYLWMHQQBFSUBP-UHFFFAOYSA-N monofluorobenzene Chemical compound FC1=CC=CC=C1 PYLWMHQQBFSUBP-UHFFFAOYSA-N 0.000 description 1
- 150000002825 nitriles Chemical class 0.000 description 1
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 1
- 229920001778 nylon Polymers 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- GHZRKQCHJFHJPX-UHFFFAOYSA-N oxacycloundecan-2-one Chemical compound O=C1CCCCCCCCCO1 GHZRKQCHJFHJPX-UHFFFAOYSA-N 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
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- 238000007747 plating Methods 0.000 description 1
- 229920003207 poly(ethylene-2,6-naphthalate) Polymers 0.000 description 1
- 229920002492 poly(sulfone) Polymers 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
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- 229920000139 polyethylene terephthalate Polymers 0.000 description 1
- 239000005020 polyethylene terephthalate Substances 0.000 description 1
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- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 229920000973 polyvinylchloride carboxylated Polymers 0.000 description 1
- 229920000036 polyvinylpyrrolidone Polymers 0.000 description 1
- 239000001267 polyvinylpyrrolidone Substances 0.000 description 1
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 1
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
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- 238000005096 rolling process Methods 0.000 description 1
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- 239000011871 silicon-based negative electrode active material Substances 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 229920003048 styrene butadiene rubber Polymers 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical class O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 239000002345 surface coating layer Substances 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
- 229910052716 thallium Inorganic materials 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
- GETTZEONDQJALK-UHFFFAOYSA-N trifluorotoluene Substances FC(F)(F)C1=CC=CC=C1 GETTZEONDQJALK-UHFFFAOYSA-N 0.000 description 1
- 229920002554 vinyl polymer Polymers 0.000 description 1
- 238000003466 welding Methods 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
Images
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/40—Alloys based on alkali metals
-
- 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
- H01M4/04—Processes of manufacture in general
-
- 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
- H01M4/04—Processes of manufacture in general
- H01M4/0471—Processes of manufacture in general involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis
-
- 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
- H01M4/134—Electrodes based on metals, Si or alloys
-
- 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
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
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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
- 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
- H01M4/364—Composites as mixtures
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- H—ELECTRICITY
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- 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
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- H—ELECTRICITY
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- 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
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/386—Silicon or alloys based on silicon
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- H—ELECTRICITY
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- 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
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- H—ELECTRICITY
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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
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- H01M4/46—Alloys based on magnesium or aluminium
- H01M4/463—Aluminium based
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- 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
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- Chemical & Material Sciences (AREA)
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- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Coating By Spraying Or Casting (AREA)
Description
LiaA1−bXbD2(上記の式で、0.95≦a≦1.1、及び0≦b≦0.5である);LiaA1−bXbO2−cDc(上記の式で、0.95≦a≦1.1、0≦b≦0.5、及び0≦c≦0.05である);LiaE1−bXbO2−cDc(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05である);LiaE2−bXbO4−cDc(上記の式で、0≦b≦0.5、0≦c≦0.05である);LiaNi1−b−cCobXcDα(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05、0<α≦2である);LiaNi1−b−cCobXcO2−αTα(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05、0<α<2である);LiaNi1−b−cCobXcO2−αT2(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05、0<α<2である);LiaNi1−b−cMnbXcDα(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05、0<α≦2である);LiaNi1−b−cMnbXcO2−αTα(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05、0<α<2である);LiaNi1−b−cMnbXcO2−αT2(上記の式で、0.95≦a≦1.1、0≦b≦0.5、0≦c≦0.05、0<α<2である);LiaNibEcGdO2(上記の式で、0.90≦a≦1.1、0≦b≦0.9、0≦c≦0.9、0.001≦d≦0.2である);LiaNibCocMndGeO2(上記の式で、0.90≦a≦1.1、0≦b≦0.9、0≦c≦0.5、0≦d≦0.5、0.001≦e≦0.2である);LiaNiGbO2(上記の式で、0.90≦a≦1.1、0.001≦b≦0.1である);LiaCoGbO2(上記の式で、0.90≦a≦1.1、0.001≦b≦0.1である);LiaMnGbO2(上記の式で、0.90≦a≦1.1、0.001≦b≦0.1である);LiaMn2GbO4(上記の式で、0.90≦a≦1.1、0.001≦b≦0.2である);QO2;QS2;LiQS2;V2O5;LiV2O5;LiZO2;LiNiVO4;Li(3−f)J2(PO4)3(0≦f≦3);Li(3−f)Fe2(PO4)3(0≦f≦2);LiFePO4。
[実施例]
平均粒子直径200nmのSi粉末と平均粒子直径1μmのCu粉末を40:60の質量比で混合して混合物を製造した。前記製造された混合物を、Cu集電体に対し、15000℃の熱源をマッハ(Mach)3の速度で通過するように熱噴射することによって活物質層を形成して、リチウム2次電池用負極を製造した。この時形成された活物質層の厚さは20μmであった。
平均粒子直径1μmのSn粉末と平均粒子直径1μmのTi粉末を50:50の質量比で混合した混合物を使用したことを除いては、前記実施例1と同様な方法によってリチウム2次電池用負極を製造した。
平均粒子直径200nmのSi粉末と平均粒子直径1μmのCu−Al合金粉末を50:50の質量比で混合した混合物を使用したことを除いては、前記実施例1と同様な方法によってリチウム2次電池用負極を製造した。
平均粒子直径200nmのSiNi合金粉末と平均粒子直径1μmのTi粉末を50:50の質量比で混合した混合物を使用したことを除いては、前記実施例1と同様な方法によってリチウム2次電池用負極を製造した。
負極活物質として、平均粒子直径が200nmのSi粉末、バインダーとして、ポリフッ化ビニリデン(PVDF)、及び導電剤としてカーボン(Super−P)を94/3/3の質量比で混合した後、N−メチル−2−ピロリドンに分散させて負極スラリーを製造した。このスラリーを厚さ10μmの銅箔にコーティングした後、乾燥、圧延して負極を製造した。
シリコン90%、ニッケル10%が完全に溶解された1400℃の熔湯を銅鋳型に流入させ、急冷して、シリコンニッケル合金のインゴット(ingot)を製造した。このインゴットを粉砕して得られた平均粒子直径0.1−10μmのシリコンニッケル合金粒子と、平均粒子直径30μmのニッケル粒子を80:20の質量比で混合した後、磨砕機(attritor)を利用して混合粉砕して、シリコンニッケル合金とニッケルが均一に混合された混合粒子を得た。
[充放電試験用テストセルの製造]
前記方法で製造されたコイン半電池を、0.2Cで充電を1回行った後負極の厚さを測定した。充電を行った後の負極の厚さを、充放電を行う前の負極の厚さに対する%比率で下記表1に示した。
前記方法で製造されたコイン型半電池を、0.2Cで0.005Vカット−オフ充電及び1.0Vカット−オフ放電で充放電を1回行って充電及び放電容量を測定し、その結果を下記表1に示した。
前記方法で製造されたコイン型半電池を0.2Cで50サイクル充放電を行った後の容量を、初期容量に対する%比率で下記表1に示した。
2 集電体
3 活物質層
4 気孔
10 リチウム二次電池
20 正極
30 負極
40 セパレータ
50 電池容器
60 封入部材
Claims (13)
- 集電体;及び
前記集電体に形成される活物質層;を含み、
前記活物質層は、金属Mの固溶体(前記Mは、Cu、Ti、Cu−X合金、Ti−X合金(前記Xは、アルカリ金属、アルカリ土類金属、13族元素、14族元素、遷移金属、希土類元素、及びこれらの組み合わせからなる群より選択される元素であり、Cu及びTiではない)及びこれらの混合物からなる群より選択される)と、リチウム含有化合物を形成することができる活物質とからなり、
前記活物質層は、100nm乃至1μmの平均粒径の活物質粉末から形成され、10体積%乃至70体積%の気孔度を有し、
前記金属Mの固溶体は、100nm乃至1μmの平均粒径を有する金属M粉末からなり、
前記活物質層が熱噴射プロセスを用いつつ、前記金属Mの固溶体は全体的に完全に溶融しつつ前記活物質粉末は表面のみ溶融した状態に形成されたものであるリチウム2次電池用負極。 - 前記Xは、Mg、Ca、Sr、Ba、Ra、Sc、Y、Ti、Zr、Hf、Rf、V、Nb、Ta、Db、Cr、Mo、W、Sg、Tc、Re、Bh、Fe、Ru、Os、Hs、Rh、Ir、Pd、Pt、Ag、Au、Zn、Cd、B、Al、Ga、In、Si、Ge、Sn、P、As、Sb、Bi、S、Se、Te、Po、及びこれらの組み合わせからなる群より選択される、請求項1に記載のリチウム2次電池用負極。
- 前記活物質は、Si、Sn、Si−Q1合金、Sn−Q2合金(前記Q1及びQ2は、互いに独立的に、アルカリ金属、アルカリ土類金属、13族元素、14族元素、遷移金属、希土類元素、及びこれらの組み合わせからなる群より選択される元素であり、Si及びSnではない)及びこれらの混合物からなる群より選択される、請求項1に記載のリチウム2次電池用負極。
- 前記活物質はSiまたはSnである、請求項1に記載のリチウム2次電池用負極。
- 前記活物質は、活物質層の質量全体に対して50質量%以上で含まれる、請求項1に記載のリチウム2次電池用負極。
- 前記活物質は、活物質層の質量全体に対して60乃至70質量%で含まれる、請求項1に記載のリチウム2次電池用負極。
- リチウム含有化合物を形成することができる活物質粉末及び金属M(前記Mは、Cu、Ti、Cu−X合金、Ti−X合金(前記Xは、アルカリ金属、アルカリ土類金属、13族元素、14族元素、遷移金属、希土類元素、及びこれらの組み合わせからなる群より選択される元素であり、Cu及びTiではない)及びこれらの混合物からなる群より選択される)粉末を混合して混合物を製造する段階;及び
前記混合物を集電体に、10000乃至18000℃の温度で100乃至400m/secの噴射速度で熱噴射して、前記金属Mは全体的に完全に溶融しつつ前記活物質粉末は表面のみ溶融した状態にして、活物質層を形成する段階;を含むリチウム2次電池用負極の製造方法。 - 前記活物質は、Si、Sn、Si−Q1合金、Sn−Q2合金(前記Q1及びQ2は、互いに独立的に、アルカリ金属、アルカリ土類金属、13族元素、14族元素、遷移金属、希土類元素、及びこれらの組み合わせからなる群より選択される元素であり、Si及びSnではない)及びこれらの混合物からなる群より選択される、請求項7に記載のリチウム2次電池用負極の製造方法。
- 前記活物質粉末は100nm乃至1μmの平均粒径を有する、請求項7記載のリチウム2次電池用負極の製造方法。
- 前記金属M粉末は100nm乃至1μmの平均粒径を有する、請求項7に記載のリチウム2次電池用負極の製造方法。
- 前記活物質粉末と金属M粉末は、30:70乃至70:30の質量比で混合される、請求項7に記載のリチウム2次電池用負極の製造方法。
- 前記熱噴射工程は、プラズマ溶射法、アーク溶射法、高速フレーム溶射法、ガス溶射法、及びこれらの組み合わせからなる群より選択される、請求項7に記載のリチウム2次電池用負極の製造方法。
- 請求項1乃至6のうちのいずれか一項に記載のリチウム2次電池用負極;
正極;及び
電解質;
を含むリチウム2次電池。
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JP2011100712A (ja) | 2011-05-19 |
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EP2328214A1 (en) | 2011-06-01 |
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