CN104380520B - 用于硫‑锂离子电池的电极组件和包括该电极组件的硫‑锂离子电池 - Google Patents
用于硫‑锂离子电池的电极组件和包括该电极组件的硫‑锂离子电池 Download PDFInfo
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- CN104380520B CN104380520B CN201480001576.8A CN201480001576A CN104380520B CN 104380520 B CN104380520 B CN 104380520B CN 201480001576 A CN201480001576 A CN 201480001576A CN 104380520 B CN104380520 B CN 104380520B
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- Prior art keywords
- lithium
- sulphur
- ion battery
- lithium ion
- electrode
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- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 35
- JDZCKJOXGCMJGS-UHFFFAOYSA-N [Li].[S] Chemical compound [Li].[S] JDZCKJOXGCMJGS-UHFFFAOYSA-N 0.000 title claims abstract description 33
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 37
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 32
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 28
- 150000001875 compounds Chemical class 0.000 claims abstract description 22
- 239000011149 active material Substances 0.000 claims abstract description 15
- 229910052717 sulfur Inorganic materials 0.000 claims abstract description 10
- 239000011593 sulfur Substances 0.000 claims abstract description 10
- 238000000034 method Methods 0.000 claims description 38
- 239000000463 material Substances 0.000 claims description 28
- 238000004519 manufacturing process Methods 0.000 claims description 26
- 239000005864 Sulphur Substances 0.000 claims description 21
- -1 Sulphur class compound Chemical class 0.000 claims description 19
- 239000000853 adhesive Substances 0.000 claims description 16
- 230000001070 adhesive effect Effects 0.000 claims description 16
- 239000003792 electrolyte Substances 0.000 claims description 12
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 12
- 239000000203 mixture Substances 0.000 claims description 11
- 239000007784 solid electrolyte Substances 0.000 claims description 11
- 238000007600 charging Methods 0.000 claims description 10
- 239000004020 conductor Substances 0.000 claims description 10
- GLNWILHOFOBOFD-UHFFFAOYSA-N lithium sulfide Chemical class [Li+].[Li+].[S-2] GLNWILHOFOBOFD-UHFFFAOYSA-N 0.000 claims description 10
- 239000002033 PVDF binder Substances 0.000 claims description 9
- 229910052782 aluminium Inorganic materials 0.000 claims description 9
- 239000010949 copper Substances 0.000 claims description 9
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 8
- 239000003960 organic solvent Substances 0.000 claims description 8
- 229910052802 copper Inorganic materials 0.000 claims description 7
- 229910052759 nickel Inorganic materials 0.000 claims description 7
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical group CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 6
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical group CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 6
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical group CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 6
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 claims description 6
- 229910052742 iron Inorganic materials 0.000 claims description 6
- 230000004087 circulation Effects 0.000 claims description 5
- 229910003480 inorganic solid Inorganic materials 0.000 claims description 5
- 229920000573 polyethylene Polymers 0.000 claims description 5
- 229920000642 polymer Polymers 0.000 claims description 5
- 239000000126 substance Substances 0.000 claims description 5
- ZHNUHDYFZUAESO-UHFFFAOYSA-N Formamide Chemical group NC=O ZHNUHDYFZUAESO-UHFFFAOYSA-N 0.000 claims description 4
- 239000004698 Polyethylene Substances 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 4
- 150000004862 dioxolanes Chemical group 0.000 claims description 4
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 claims description 4
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 claims description 4
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 claims description 4
- 229910003002 lithium salt Inorganic materials 0.000 claims description 4
- 159000000002 lithium salts Chemical class 0.000 claims description 4
- 230000014759 maintenance of location Effects 0.000 claims description 4
- TZIHFWKZFHZASV-UHFFFAOYSA-N methyl formate Chemical group COC=O TZIHFWKZFHZASV-UHFFFAOYSA-N 0.000 claims description 4
- PYOKUURKVVELLB-UHFFFAOYSA-N trimethyl orthoformate Chemical group COC(OC)OC PYOKUURKVVELLB-UHFFFAOYSA-N 0.000 claims description 4
- 229910052725 zinc Inorganic materials 0.000 claims description 4
- KDXKERNSBIXSRK-UHFFFAOYSA-N Lysine Natural products NCCCCC(N)C(O)=O KDXKERNSBIXSRK-UHFFFAOYSA-N 0.000 claims description 3
- 239000004472 Lysine Substances 0.000 claims description 3
- 229920003171 Poly (ethylene oxide) Polymers 0.000 claims description 3
- 239000002253 acid Substances 0.000 claims description 3
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 claims description 3
- 229920000728 polyester Polymers 0.000 claims description 3
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 3
- 238000006467 substitution reaction Methods 0.000 claims description 3
- 229910052723 transition metal Inorganic materials 0.000 claims description 3
- 150000003624 transition metals Chemical class 0.000 claims description 3
- LZDKZFUFMNSQCJ-UHFFFAOYSA-N 1,2-diethoxyethane Chemical compound CCOCCOCC LZDKZFUFMNSQCJ-UHFFFAOYSA-N 0.000 claims description 2
- 125000006091 1,3-dioxolane group Chemical class 0.000 claims description 2
- ANLVEXKNRYNLDH-UHFFFAOYSA-N 1,3-dioxonan-2-one Chemical compound O=C1OCCCCCCO1 ANLVEXKNRYNLDH-UHFFFAOYSA-N 0.000 claims description 2
- JWUJQDFVADABEY-UHFFFAOYSA-N 2-methyltetrahydrofuran Chemical class CC1CCCO1 JWUJQDFVADABEY-UHFFFAOYSA-N 0.000 claims description 2
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 claims description 2
- 229910001558 CF3SO3Li Inorganic materials 0.000 claims description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical class COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 2
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical group COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 claims description 2
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 2
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims description 2
- 229910007101 Li1+yMn2-yO4 Inorganic materials 0.000 claims description 2
- 229910007132 Li1+yMn2−yO4 Inorganic materials 0.000 claims description 2
- 229910010228 Li2Mn3MO8 Inorganic materials 0.000 claims description 2
- 229910007558 Li2SiS3 Inorganic materials 0.000 claims description 2
- 229910012722 Li3N-LiI-LiOH Inorganic materials 0.000 claims description 2
- 229910012716 Li3N-LiI—LiOH Inorganic materials 0.000 claims description 2
- 229910012734 Li3N—LiI—LiOH Inorganic materials 0.000 claims description 2
- 229910013043 Li3PO4-Li2S-SiS2 Inorganic materials 0.000 claims description 2
- 229910013035 Li3PO4-Li2S—SiS2 Inorganic materials 0.000 claims description 2
- 229910012810 Li3PO4—Li2S-SiS2 Inorganic materials 0.000 claims description 2
- 229910012797 Li3PO4—Li2S—SiS2 Inorganic materials 0.000 claims description 2
- 229910012047 Li4SiO4-LiI-LiOH Inorganic materials 0.000 claims description 2
- 229910012075 Li4SiO4-LiI—LiOH Inorganic materials 0.000 claims description 2
- 229910012057 Li4SiO4—LiI—LiOH Inorganic materials 0.000 claims description 2
- 229910010739 Li5Ni2 Inorganic materials 0.000 claims description 2
- 229910003253 LiB10Cl10 Inorganic materials 0.000 claims description 2
- 229910000552 LiCF3SO3 Inorganic materials 0.000 claims description 2
- 229910015645 LiMn Inorganic materials 0.000 claims description 2
- 229910014385 LiMn2-yMyO2 Inorganic materials 0.000 claims description 2
- 229910014439 LiMn2−yMyO2 Inorganic materials 0.000 claims description 2
- 229910014383 LiNi1-yMyO2 Inorganic materials 0.000 claims description 2
- 229910014952 LiNi1−yMyO2 Inorganic materials 0.000 claims description 2
- 229910001290 LiPF6 Inorganic materials 0.000 claims description 2
- 229910012346 LiSiO4-LiI-LiOH Inorganic materials 0.000 claims description 2
- 229910012345 LiSiO4-LiI—LiOH Inorganic materials 0.000 claims description 2
- 229910012348 LiSiO4—LiI—LiOH Inorganic materials 0.000 claims description 2
- 241001597008 Nomeidae Species 0.000 claims description 2
- 229910019142 PO4 Inorganic materials 0.000 claims description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 2
- 229910006145 SO3Li Inorganic materials 0.000 claims description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 2
- BEKPOUATRPPTLV-UHFFFAOYSA-N [Li].BCl Chemical compound [Li].BCl BEKPOUATRPPTLV-UHFFFAOYSA-N 0.000 claims description 2
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Chemical group COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 claims description 2
- 229910052796 boron Inorganic materials 0.000 claims description 2
- 150000001732 carboxylic acid derivatives Chemical class 0.000 claims description 2
- 229910052804 chromium Inorganic materials 0.000 claims description 2
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical class [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 claims description 2
- 238000010494 dissociation reaction Methods 0.000 claims description 2
- 230000005593 dissociations Effects 0.000 claims description 2
- 229910052733 gallium Inorganic materials 0.000 claims description 2
- 150000004820 halides Chemical class 0.000 claims description 2
- 125000001841 imino group Chemical group [H]N=* 0.000 claims description 2
- 229910052909 inorganic silicate Inorganic materials 0.000 claims description 2
- 229910001547 lithium hexafluoroantimonate(V) Inorganic materials 0.000 claims description 2
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 claims description 2
- 229910002102 lithium manganese oxide Inorganic materials 0.000 claims description 2
- QEXMICRJPVUPSN-UHFFFAOYSA-N lithium manganese(2+) oxygen(2-) Chemical compound [O-2].[Mn+2].[Li+] QEXMICRJPVUPSN-UHFFFAOYSA-N 0.000 claims description 2
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 2
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 2
- 229910001537 lithium tetrachloroaluminate Inorganic materials 0.000 claims description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 2
- HSFDLPWPRRSVSM-UHFFFAOYSA-M lithium;2,2,2-trifluoroacetate Chemical compound [Li+].[O-]C(=O)C(F)(F)F HSFDLPWPRRSVSM-UHFFFAOYSA-M 0.000 claims description 2
- 229910052749 magnesium Inorganic materials 0.000 claims description 2
- 229910052748 manganese Inorganic materials 0.000 claims description 2
- 239000011572 manganese Substances 0.000 claims description 2
- 229940017219 methyl propionate Drugs 0.000 claims description 2
- LYGJENNIWJXYER-UHFFFAOYSA-N nitromethane Chemical group C[N+]([O-])=O LYGJENNIWJXYER-UHFFFAOYSA-N 0.000 claims description 2
- 150000002898 organic sulfur compounds Chemical class 0.000 claims description 2
- 239000010452 phosphate Substances 0.000 claims description 2
- 238000006116 polymerization reaction Methods 0.000 claims description 2
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- 238000003756 stirring Methods 0.000 claims description 2
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical group O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 claims description 2
- 229910052715 tantalum Inorganic materials 0.000 claims description 2
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 claims description 2
- BHZCMUVGYXEBMY-UHFFFAOYSA-N trilithium;azanide Chemical compound [Li+].[Li+].[Li+].[NH2-] BHZCMUVGYXEBMY-UHFFFAOYSA-N 0.000 claims description 2
- PNWSHHILERSSLF-UHFFFAOYSA-N 4-methylbenzene-1,3-dicarboxylic acid Chemical class CC1=CC=C(C(O)=O)C=C1C(O)=O PNWSHHILERSSLF-UHFFFAOYSA-N 0.000 claims 1
- 229910003349 Li2CuO2 Inorganic materials 0.000 claims 1
- 229910012820 LiCoO Inorganic materials 0.000 claims 1
- 229910003005 LiNiO2 Inorganic materials 0.000 claims 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical group CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims 1
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- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 claims 1
- 150000001768 cations Chemical group 0.000 claims 1
- XYIBRDXRRQCHLP-UHFFFAOYSA-N ethyl acetoacetate Chemical compound CCOC(=O)CC(C)=O XYIBRDXRRQCHLP-UHFFFAOYSA-N 0.000 claims 1
- 125000004494 ethyl ester group Chemical group 0.000 claims 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 claims 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims 1
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- 150000003457 sulfones Chemical class 0.000 claims 1
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- 230000008569 process Effects 0.000 description 15
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 13
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- XAQHXGSHRMHVMU-UHFFFAOYSA-N [S].[S] Chemical compound [S].[S] XAQHXGSHRMHVMU-UHFFFAOYSA-N 0.000 description 1
- 239000006230 acetylene black Substances 0.000 description 1
- 238000001994 activation Methods 0.000 description 1
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- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical group 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 150000003863 ammonium salts Chemical class 0.000 description 1
- SMWDFEZZVXVKRB-UHFFFAOYSA-N anhydrous quinoline Natural products N1=CC=CC2=CC=CC=C21 SMWDFEZZVXVKRB-UHFFFAOYSA-N 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 230000008901 benefit Effects 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
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- DMSZORWOGDLWGN-UHFFFAOYSA-N ctk1a3526 Chemical class NP(N)(N)=O DMSZORWOGDLWGN-UHFFFAOYSA-N 0.000 description 1
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- 150000002118 epoxides Chemical class 0.000 description 1
- PWEHMQBAMSTRDF-UHFFFAOYSA-N ethyl carbonofluoridate Chemical compound CCOC(F)=O PWEHMQBAMSTRDF-UHFFFAOYSA-N 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
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- 150000002367 halogens Chemical class 0.000 description 1
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- HNJBEVLQSNELDL-UHFFFAOYSA-N pyrrolidin-2-one Chemical compound O=C1CCCN1 HNJBEVLQSNELDL-UHFFFAOYSA-N 0.000 description 1
- 150000004060 quinone imines Chemical class 0.000 description 1
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- ISIJQEHRDSCQIU-UHFFFAOYSA-N tert-butyl 2,7-diazaspiro[4.5]decane-7-carboxylate Chemical compound C1N(C(=O)OC(C)(C)C)CCCC11CNCC1 ISIJQEHRDSCQIU-UHFFFAOYSA-N 0.000 description 1
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Classifications
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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
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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
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- H—ELECTRICITY
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- 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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- 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
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- H—ELECTRICITY
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- 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
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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
- H01M4/58—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
- H01M4/581—Chalcogenides or intercalation compounds thereof
- H01M4/5815—Sulfides
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- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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Abstract
本申请公开的是一种用于硫‑锂离子电池的电极组件以及包括该电极组件的硫‑锂离子电池,该电极组件使用含锂化合物作为阴极活性材料并使用含硫化合物作为阳极活性材料。
Description
技术领域
本发明涉及用于硫-锂离子电池的电极组件以及包括该电极组件的硫-锂离子电池,所述电极组件包括作为阴极活性材料的含锂化合物和作为阳极活性材料的含硫化合物。
背景技术
与便携式电子设备的小型化、高集成度以及混合动力电动汽车(HEV)和电动汽车(EV)的发展一致,需要具有高能量密度的二次电池。
锂-硫电池是使用硫作为阴极活性材料和使用锂金属作为阳极活性材料的电池系统。在放电过程中,阴极的硫通过接受电子被还原,阳极的锂经电离被氧化。
硫还原是硫-硫(S-S)键通过接受两个电子转化为硫的阴离子的过程。同时,锂氧化是锂金属通过释放电子转化为锂离子并且锂离子经电解质转移至阴极以形成硫的阴离子和盐的过程。
硫在放电前具有环状S8结构,并通过还原反应转化为多硫化锂。多硫化锂被完全还原以形成硫化锂(Li2S)。
设置在阴极和阳极之间的电解质充当介质,锂离子通过该介质移动。
另一方面,在充电过程中,阴极处的硫通过释放电子被氧化,阳极处的锂离子通过接受电子经还原反应转化为锂金属。
在充电过程中,发生硫释放电子形成S-S键的反应,并在Li阳极表面发生锂离子通过接受电子被还原为锂金属的反应。
当环状硫中的键经还原反应断裂时,形成Sn 2-的聚硫离子,其中n是硫链的长度。在这方面,n可以为8以上,环状硫和聚硫离子可以经下列反应转化为具有相对长链的聚硫离子:
S8+Sn 2-→Sn+8 2-。
此类锂-硫电池系统最显著的特性是远高于其他电池系统的理论能量密度。高能量密度源于硫和锂的高比容量。但是,为了实现高能量密度,必须确保硫和锂的高利用率。
此外,锂-硫电池可以以降低的制造成本制造。
特别地,将廉价且丰富的硫用作阴极活性材料,因此,可以降低锂-硫电池的制造成本。此外,锂离子电池的阳极制造包括制备浆料的制备和涂布、干燥和压制,而锂-硫电池使用锂金属作为阳极,无需对其进行预处理,由此可以简化制造工艺,因此可以降低制造成本。此外,在锂离子电池中,当锂嵌入作为阳极活性材料的碳材料中时生成的气体经活化除去,而在锂-硫电池中,因为锂离子沉积在锂金属表面,所以不生成气体,因此也不需要活化过程。由于省略了此类过程,因此,在降低电池制造成本方面具有很大的影响。
发明内容
技术问题
但是,尽管具有上述优点,锂-硫电池仍存在锂金属的安全问题,并且由此硫的利用率较低。此外,在放电过程中在阴极处生成的多硫化锂在充电过程中在锂金属表面处被还原,在锂金属表面处形成了不稳定的膜,由此活性硫的量持续降低,结果,循环特性劣化。
本发明的发明人证实,使用硫作为阳极活性材料的电池系统会解决上述问题,从而完成了本发明。
因此,本发明的目的是提供一种新型电池系统,该电池系统与传统锂-硫电池相比具有提高的安全性和循环特性。
技术方案
根据本发明的方面,提供的是一种电极组件,包括:阴极,该阴极包含作为阴极活性材料的含锂化合物;阳极,该阳极包含作为阳极活性材料的含硫化合物;以及设置在阴极与阳极之间的隔板,以及通过在电池外壳中容纳该电极组件、用电解质浸渍该电极组件并密封该电池外壳来制造的硫-锂离子电池。
特别地,根据本发明的电极组件和硫-锂离子电池使用含锂化合物作为阴极活性材料并使用含硫化合物作为阳极活性材料。
本文中使用的含锂化合物可以理解为能够在初始充电过程中通过氧化反应向阳极供给锂离子的化合物。特别地,该含锂化合物是能够在充电和放电过程中使锂离子嵌入和脱嵌的化合物,并可以是选自以下中的至少一种:锂过渡金属氧化物及其衍生物、以及锂过渡金属磷酸盐及其衍生物。
更特别地,含锂化合物的实例包括但不限于层状化合物,如锂钴氧化物(LiCoO2)和锂镍氧化物(LiNiO2),或用一种或多种过渡金属取代的化合物;具有式Li1+yMn2-yO4的锂锰氧化物,其中0≤y≤0.33,如LiMnO3、LiMn2O3和LiMnO2;锂铜氧化物(Li2CuO2);钒氧化物如LiV3O8、LiV3O4、V2O5和Cu2V2O7;式LiNi1-yMyO2的Ni位型锂镍氧化物,其中M=Co、Mn、Al、Cu、Fe、Mg、B或Ga,并且0.01≤y≤0.3;式LiMn2-yMyO2的锂锰复合氧化物,其中M=Co、Ni、Fe、Cr、Zn或Ta,并且0.01≤y≤0.1,或式Li2Mn3MO8的锂锰复合氧化物,其中M=Fe、Co、Ni、Cu或Zn;其中一部分Li原子被碱土金属离子取代的LiMn2O4;二硫化合物;以及Fe2(MoO4)3。
本文中使用的含硫化合物可以理解为在初始充电过程中经还原反应接受锂离子的化合物。特别地,该含硫化合物可以是硫类化合物,选自无机硫或元素硫(S8)、其中1≤n≤8的Li2Sn、有机硫化合物以及碳-硫复合物(C2xSy,其中0≤x≤2和1≤y≤40)或它们中的至少两种的混合物。
作为隔板,使用具有高离子渗透性和机械强度的绝缘薄膜。该隔板通常具有0.01至10μm的孔径和5至300μm的厚度。作为隔板,使用由烯烃类聚合物如聚丙烯制造的片材或无纺织物;或具有耐化学性和疏水性的玻璃纤维或聚乙烯,或牛皮纸。市售隔板的实例包括Celgard系列如和2300(可获自Hoechest Celanese Corp.)、聚丙烯隔板(可获自Ube Industries Ltd.或Pall RAI Co.)和聚乙烯系列(可获自Tonen或Entek)。
在一些情况下,凝胶聚合物电解质可以涂布在隔板上以提高电池稳定性。凝胶聚合物的实例包括但不限于聚环氧乙烷、聚偏二氟乙烯和聚丙烯腈。
当使用固体电解质如聚合物等作为电解质时,该固体电解质也可以充当隔板。
阴极和阳极还可以包括导电材料和粘合剂中的至少一种。
导电材料没有特别限制,只要其具有高导电性和宽表面积即可。导电材料的实例包括石墨如天然或人造石墨;炭黑如炭黑、乙炔黑、科琴黑、槽法炭黑、炉法炭黑、灯黑和热裂炭黑;导电纤维如碳纤维和金属纤维;金属粉末如氟化碳粉末、铝粉末和镍粉末;导电晶须如氧化锌和钛酸钾;导电性金属氧化物如氧化钛;以及聚亚苯基衍生物。
在一个特定实施方案中,导电材料的平均粒径可以为1.0μm以下,比表面积为10m2/g以上。
粘合剂可以是本领域已知的所有粘合剂,特别是选自以下中的一种:氟树脂类粘合剂,如聚偏二氟乙烯(PVdF)和聚四氟乙烯(PTFE),橡胶类粘合剂如苯乙烯-丁二烯橡胶、丙烯腈-丁二烯橡胶和苯乙烯-异戊二烯橡胶,纤维素类粘合剂如羧甲基纤维素(CMC)、淀粉、羟丙基纤维素和再生纤维素,多元醇类粘合剂,聚烯烃类粘合剂如聚乙烯和聚丙烯,聚酰亚胺类粘合剂,聚酯类粘合剂,贻贝粘合剂和硅烷类粘合剂或它们中的至少两种的混合物或共聚物。
根据粘合剂的类型可以选择性使用溶剂,并且溶剂例如是诸如异丙醇、N-甲基吡咯烷酮(NMP)或丙酮等的有机溶剂或水等。
在一个特定实施方案中,可以通过在NMP中分散或溶解PVdF或通过在水中分散或溶解苯乙烯-丁二烯橡胶(SBR)/羧甲基纤维素(CMC)来制备粘合剂溶液。
阳极还可以包含多硫化锂的吸附材料,特别地,多硫化锂的吸附材料可以是氧化铝(Al2O3),但是本发明的实施方案不限于此。
电解质可以是含锂盐的非水电解质,作为非水电解质,可以使用非水电解液、有机固体电解质或无机固体电解质。
锂盐是易溶于非水电解质的物质,其实例包括LiCl、LiBr、LiI、LiClO4、LiBF4、LiB10Cl10、LiPF6、LiCF3SO3、LiCF3CO2、LiAsF6、LiSbF6、LiAlCl4、CH3SO3Li、CF3SO3Li、LiSCN、LiC(CF3SO2)3、(CF3SO2)2NLi、氯硼烷锂、低级脂族羧酸锂、四苯基硼酸锂和亚氨基锂。
例如,非水电解液可以是非质子性有机溶剂,如N-甲基-2-吡咯烷酮、碳酸异丙烯酯、碳酸亚乙酯、碳酸丁烯酯、碳酸二甲酯、碳酸二乙酯、碳酸甲乙酯、γ-丁内酯、1,2-二甲氧基乙烷、1,2-二乙氧基乙烷、四氢呋喃、2-甲基四氢呋喃、二甲亚砜、1,3-二氧戊环、4-甲基-1,3-二噁烯、二乙醚、甲酰胺、二甲基甲酰胺、二氧戊环、乙腈、硝基甲烷、甲酸甲酯、乙酸甲酯、磷酸三酯、三甲氧基甲烷、二氧戊环衍生物、环丁砜、甲基环丁砜、1,3-二甲基-2-咪唑啉酮、碳酸异丙烯酯衍生物、四氢呋喃衍生物、醚、丙酸甲酯或丙酸乙酯。此外,有机溶剂可以是至少两种上面列举的有机溶剂的混合物。
有机固体电解质的实例包括聚乙烯衍生物、聚环氧乙烷衍生物、聚环氧丙烷衍生物、磷酸酯聚合物、聚合的搅拌赖氨酸(poly agitation lysine)、聚酯硫化物、聚乙烯醇、聚偏二氟乙烯和含有离子离解基团的聚合物。
无机固体电解质的实例包括锂(Li)的氮化物、卤化物和硫酸盐,如Li3N、LiI、Li5NI2、Li3N-LiI-LiOH、LiSiO4、LiSiO4-LiI-LiOH、Li2SiS3、Li4SiO4、Li4SiO4-LiI-LiOH和Li3PO4-Li2S-SiS2。
此外,为了改善充电/放电特性和阻燃性,例如,可以向电解质中加入吡啶、亚磷酸三乙酯、三乙醇胺、环醚、乙二胺、正甘醇二甲醚、六磷酰三胺、硝基苯衍生物、硫、醌亚胺染料、N-取代的噁唑烷酮、N,N-取代的咪唑烷、乙二醇二烷基醚、铵盐、吡咯、2-甲氧基乙醇或三氯化铝等。在一些情况下,为了赋予不燃性,电解质还可以包括含卤素的溶剂如四氯化碳和三氟乙烯。此外,为了改善高温储存特性,电解质还可以包括二氧化碳气体、氟代-碳酸亚乙酯(FEC)、丙烯基磺内酯(PRS)或氟代-碳酸异丙烯酯(FPC)等。
阳极和阴极可以使用包括下列工艺的制造方法制造。
制造方法包括通过在溶剂中分散或溶解粘合剂来制备粘合剂溶液;通过混合该粘合剂溶液、电极活性材料和导电材料来制备电极浆料;在集流体上涂布该电极浆料;干燥该电极;将该电极压制到一定厚度。
在一些情况下,制造方法还可以包括干燥所压制的电极。
粘合剂溶液的制备是通过在溶剂中分散或溶解粘合剂来制备粘合剂溶液的工艺。
电极浆料可以通过在粘合剂溶液中混合/分散电极活性材料与导电材料来制备。所制备的电极浆料可以使用储罐运送并在涂布前储存。电极浆料可以在储罐中持续搅拌以防止电极浆料硬化。
电极浆料的涂布是通过穿过涂布头以预定图案将电极浆料涂布到集流体上至一定厚度的工艺。
电极浆料的涂布可以通过使用刮刀等或通过压铸、间歇式涂布或丝网印刷等将电极浆料分配到集流体上并在其上均匀分散电极浆料来进行。在另一实施方案中,电极浆料可以在单独的基底上模制并随后经由压制或层压粘接到集流体上。
对集流体没有特殊限制,只要其不会在制得的电池中引起化学变化并具有高导电性即可。例如,集流体可以由铜、不锈钢、铝、镍、钛、烧结炭,用碳、镍、钛或银等进行表面处理的铜或不锈钢或铝-镉合金等构成。阴极集流体可以在其表面处具有微细的凹凸以提高阴极活性材料与阴极集流体之间的粘附力,并可以以任意多种形式使用,包括膜、片材、箔、网、多孔结构、泡沫和无纺织物。特别地,阴极集流体可以是含有金属如铝的集流体,阳极集流体可以是含有金属如铜的集流体。
电解质的干燥是除去浆料中的溶剂与湿气以便干燥涂布在集流体上的浆料的工艺。在一个特定实施方案中,干燥在真空炉中在50至200℃的温度下进行一天。
制造方法还可以包括在干燥后的冷却过程,该冷却过程可以通过缓慢冷却至室温来进行,以便令人满意地形成粘合剂的再结晶结构。
为了提高已经在其上完成涂布工艺的电极的容量密度并提高集流体与电极活性材料之间的粘附力,可以通过穿过加热至高温的两个辊将电极压制至所需厚度。该过程称为辊压工艺。
在穿过两个辊之前,电极可以预先加热。预先加热工艺是在引入两个辊之前预热电极以提高电极压制效果的过程。
经辊压的电极可以进行本领域已知的沉积或涂布以形成导电层。
在其上形成有导电层的电极可以在真空炉中在50至200℃下干燥一天。经辊压的电极可以切割至特定尺寸并随后干燥。
在干燥过程后,还可以进行冷却过程,冷却过程可以通过缓慢冷却至室温来进行,以便令人满意地形成粘合剂的再结晶结构。
果酱卷型(jellyroll-type)电极组件可以通过将隔板片材放置在使用上述方法制得的阴极与阳极片材之间并卷绕所得到的结构来制造。
堆叠型电极组件可以通过以下方法制造:将使用上述方法制得的阴极和阳极切割至预定尺寸,在所获得的阴极和阳极板之间插入切割至预定尺寸的隔板(该预定尺寸与阴极与阳极板的尺寸对应),并堆叠所得到的结构。
堆叠/折叠型电极组件可以通过以下方法制造:在隔板片材上排列至少两个阴极板和至少两个阳极板,或在隔板片材上排列至少两个单元电池,每个单元电池包括至少两个阴极板和至少两个阳极板,其间具有隔板,以使得阴极和阳极彼此面对,隔板位于二者之间,并卷绕该隔板片材或折叠该隔板片材至电极板或单元电池的尺寸。
包括该硫-锂离子电池的电池组可以用作电动车辆(EV)、混合动力电动车辆(HEV)、插电式混合动力电动车辆(PHEV)和用于储能的装置的动力源。
具体实施方式
现在,将参照下列实施例更详细地描述本发明。提供这些实施例仅为描述本发明,不应被解释为限制本发明的范围与精神。
<实施例1>
将以95:2.5:2.5的质量比包含LiCoO2、Super-P(可获自Timcal)和PVdF(6020,可获自Solef)的固体与作为溶剂的N-甲基-2-吡咯烷酮(NMP)混合以制备阴极浆料。将该阴极浆料涂布到20微米铝箔上以制造负载量为3mAh/cm2的阴极。
对重量比为20:80的碳粉末和硫的混合物进行湿球磨以获得碳-硫复合物。将包含80.0重量%的碳-硫复合物、10.0重量%的作为导电材料的Super-P和10.0重量%的作为粘合剂的PVdF的阳极混合物添加到作为溶剂的NMP中以制备阳极浆料,并随后将阳极浆料涂布到20微米铝集流体上以制造负载量为3.3mAh/cm2的阳极。
将阴极、阳极、作为电解质的其中溶解1M LiN(CF3SO2)2的四乙二醇二甲醚(TEGDME)和作为隔板的聚烯烃膜组装以制造电池单元。
<对比例1>
对重量比为20:80的碳粉末和硫的混合物进行湿球磨以获得碳-硫复合物。将包含80.0重量%的碳-硫复合物、10.0重量%的作为导电材料的Super-P和10.0重量%的作为粘合剂的PVdF的阴极混合物添加到作为溶剂的NMP中以制备阴极浆料,并随后将阴极浆料涂布到20微米的铝集流体上以制造负载量为3.3mAh/cm2的阴极。
除了使用厚度大约为150微米的锂箔作为阳极外,以与实施例1相同的方式制造电池单元。
<试验实施例1>
比较了根据实施例1和对比例1制造的电池单元随温度改变的循环特性。在下列条件下重复100次电池单元的充电和放电循环:在0.1C下充电并在0.1C下放电。测量了相对于各电池单元初始容量100次循环后的容量保持率(%)。结果显示在下表1中。
<表1>
从表1中所示结果可以看出,本发明的电池在解决现有锂-硫电池的循环特性问题方面表现出优异的效果。
工业实用性
本发明的硫-锂离子电池包括作为阳极活性材料的含硫化合物,并由此与常规锂-硫电池不同,不会发生充电过程中锂的沉积,因此,该硫-锂离子电池表现出提高的安全性。
此外,与常规锂-硫电池不同,充电过程中不会发生根据多硫化锂的还原进行的活性硫的还原,由此该硫-锂离子电池表现出增强的循环特性。
Claims (18)
1.一种电极组件,包括:
阴极,该阴极包含作为阴极活性材料的含锂化合物,所述含锂化合物是层状化合物并且是选自用一种或多种过渡金属取代的锂钴氧化物LiCoO2和用一种或多种过渡金属取代的锂镍氧化物LiNiO2;具有式Li1+yMn2-yO4的锂锰氧化物,其中0<y≤0.33;锂铜氧化物Li2CuO2;式LiNi1-yMyO2的Ni位型锂镍氧化物,其中M=Co、Mn、Al、Cu、Fe、Mg、B或Ga,并且0.01≤y≤0.3;式LiMn2-yMyO2的锂锰复合氧化物,其中M=Co、Ni、Fe、Cr、Zn或Ta,并且0.01≤y≤0.1,或式Li2Mn3MO8的锂锰复合氧化物,其中M=Fe、Co、Ni、Cu或Zn;其中一部分Li原子被碱土金属离子取代的LiMn2O4中的至少一种;
阳极,该阳极包含作为阳极活性材料的含硫物质,所述含硫物质是选自元素硫S8、其中1≤n≤8的Li2Sn、有机硫化合物以及其中0≤x≤2和1≤y≤40的碳-硫复合物C2xSy或它们的至少两种的混合物中的硫类化合物;和
设置在阴极与阳极之间的隔板,
其中,所述阳极还包含多硫化锂的吸附材料。
2.根据权利要求1所述的电极组件,其中所述阴极和阳极还包含导电材料和粘合剂中的至少一种。
3.根据权利要求2所述的电极组件,其中所述导电材料的平均粒径为1.0μm以下,比表面积为10m2/g以上。
4.根据权利要求1所述的电极组件,其中所述多硫化锂的吸附材料是氧化铝。
5.一种硫-锂离子电池,包括:根据权利要求1至4中任一项所述的电极组件、电解质、和电池外壳。
6.根据权利要求5所述的硫-锂离子电池,其中在0.1C的电流和20℃下重复100次充电和放电循环时,相对于初始容量,100次循环的容量保持率为80%以上。
7.根据权利要求5所述的硫-锂离子电池,其中在0.1C的电流和35℃下重复100次充电和放电循环时,相对于初始容量,100次循环的容量保持率为80%以上。
8.根据权利要求5所述的硫-锂离子电池,其中在0.1C的电流和60℃下重复100次充电和放电循环时,相对于初始容量,100次循环的容量保持率为80%以上。
9.根据权利要求5所述的硫-锂离子电池,其中所述电解质是包含锂盐和有机溶剂的非水电解质、有机固体电解质或无机固体电解质。
10.根据权利要求9所述的硫-锂离子电池,其中所述锂盐是选自LiCl、LiBr、LiI、LiClO4、LiBF4、LiB10Cl10、LiPF6、LiCF3SO3、LiCF3CO2、LiAsF6、LiSbF6、LiAlCl4、CH3SO3Li、CF3SO3Li、LiSCN、LiC(CF3SO2)3、(CF3SO2)2NLi、氯硼烷锂、低级脂族羧酸锂、四苯基硼酸锂和亚氨基锂中的至少一种。
11.根据权利要求9所述的硫-锂离子电池,其中所述有机溶剂是非质子性有机溶剂。
12.根据权利要求11所述的硫-锂离子电池,其中所述非质子性有机溶剂是选自N-甲基-2-吡咯烷酮、碳酸异丙烯酯、碳酸亚乙酯、碳酸丁烯酯、碳酸二甲酯、碳酸二乙酯、碳酸甲乙酯、γ-丁内酯、1,2-二甲氧基乙烷、1,2-二乙氧基乙烷、四氢呋喃、2-甲基四氢呋喃、二甲亚砜、1,3-二氧戊环、4-甲基-1,3-二噁烯、二乙醚、甲酰胺、二甲基甲酰胺、二氧戊环、乙腈、硝基甲烷、甲酸甲酯、乙酸甲酯、磷酸三酯、三甲氧基甲烷、二氧戊环衍生物、环丁砜、甲基环丁砜、1,3-二甲基-2-咪唑啉酮、碳酸异丙烯酯衍生物、四氢呋喃衍生物、醚、丙酸甲酯和丙酸乙酯中的至少一种。
13.根据权利要求9所述的硫-锂离子电池,其中所述有机固体电解质是选自聚乙烯衍生物、聚环氧乙烷衍生物、聚环氧丙烷衍生物、磷酸酯聚合物、聚合的搅拌赖氨酸、聚酯硫化物、聚乙烯醇、聚偏二氟乙烯和含有离子离解基团的聚合物中的至少一种。
14.根据权利要求9所述的硫-锂离子电池,其中所述无机固体电解质是选自锂的氮化物、卤化物和硫酸盐中的至少一种。
15.根据权利要求14所述的硫-锂离子电池,其中所述无机固体电解质是选自Li3N、LiI、Li5NI2、Li3N-LiI-LiOH、LiSiO4、LiSiO4-LiI-LiOH、Li2SiS3、Li4SiO4、Li4SiO4-LiI-LiOH和Li3PO4-Li2S-SiS2中的至少一种。
16.一种制造权利要求1所述的电极组件的方法,该方法包括通过将隔板片材放置在阴极片材与阳极片材之间并卷绕该阴极片材、阳极片材和隔板片材来制造果酱卷型电极组件。
17.一种制造权利要求1所述的电极组件的方法,该方法包括通过以下方法制造堆叠型电极组件:顺序堆叠阴极板、隔板和阳极板,使得隔板设置在阴极板与阳极板之间。
18.一种制造权利要求1所述的电极组件的方法,该方法包括通过以下方法制造堆叠/折叠型电极组件:在隔板片材上排列至少两个阴极板和至少两个阳极板,或在隔板片材上排列至少两个单元电池,每个单元电池包括至少两个阴极板和至少两个阳极板,其间具有隔板,使得阴极和阳极彼此面对,其间具有隔板片材,并卷绕该隔板片材或折叠该隔板片材至所述阴极板和阳极板或所述单元电池的尺寸。
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JP7216073B2 (ja) * | 2018-03-13 | 2023-01-31 | 株式会社Adeka | 非水電解質二次電池 |
JP7017123B2 (ja) * | 2018-06-01 | 2022-02-08 | トヨタ自動車株式会社 | 正極合材、全固体電池および正極合材の製造方法 |
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EP2892104B1 (en) | 2017-10-18 |
US20160093887A1 (en) | 2016-03-31 |
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