JP7210475B2 - 電気化学セルの不動態化剤 - Google Patents
電気化学セルの不動態化剤 Download PDFInfo
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- JP7210475B2 JP7210475B2 JP2019563875A JP2019563875A JP7210475B2 JP 7210475 B2 JP7210475 B2 JP 7210475B2 JP 2019563875 A JP2019563875 A JP 2019563875A JP 2019563875 A JP2019563875 A JP 2019563875A JP 7210475 B2 JP7210475 B2 JP 7210475B2
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- JP
- Japan
- Prior art keywords
- passivating agent
- electrode
- electrochemical cell
- less
- lithium
- Prior art date
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- 239000003795 chemical substances by application Substances 0.000 claims description 590
- 239000003792 electrolyte Substances 0.000 claims description 259
- 239000010410 layer Substances 0.000 claims description 231
- -1 lithium hexafluoroarsenate Chemical compound 0.000 claims description 172
- 229910052744 lithium Inorganic materials 0.000 claims description 117
- 239000011241 protective layer Substances 0.000 claims description 69
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 61
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical group [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 48
- 150000001875 compounds Chemical class 0.000 claims description 47
- 239000002904 solvent Substances 0.000 claims description 47
- 229920000642 polymer Polymers 0.000 claims description 36
- 238000000034 method Methods 0.000 claims description 35
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims description 34
- IIPYXGDZVMZOAP-UHFFFAOYSA-N lithium nitrate Chemical compound [Li+].[O-][N+]([O-])=O IIPYXGDZVMZOAP-UHFFFAOYSA-N 0.000 claims description 34
- 230000001351 cycling effect Effects 0.000 claims description 30
- 238000000354 decomposition reaction Methods 0.000 claims description 27
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 26
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 claims description 24
- 239000000203 mixture Substances 0.000 claims description 20
- 239000000654 additive Substances 0.000 claims description 17
- 239000000126 substance Substances 0.000 claims description 15
- ZOOODBUHSVUZEM-UHFFFAOYSA-N ethoxymethanedithioic acid Chemical group CCOC(S)=S ZOOODBUHSVUZEM-UHFFFAOYSA-N 0.000 claims description 14
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 13
- DSMUTQTWFHVVGQ-UHFFFAOYSA-N 4,5-difluoro-1,3-dioxolan-2-one Chemical compound FC1OC(=O)OC1F DSMUTQTWFHVVGQ-UHFFFAOYSA-N 0.000 claims description 10
- 230000000996 additive effect Effects 0.000 claims description 10
- 229910003002 lithium salt Inorganic materials 0.000 claims description 10
- 159000000002 lithium salts Chemical class 0.000 claims description 10
- 238000007254 oxidation reaction Methods 0.000 claims description 10
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 9
- 230000003647 oxidation Effects 0.000 claims description 9
- 238000006116 polymerization reaction Methods 0.000 claims description 9
- 238000003780 insertion Methods 0.000 claims description 8
- 230000037431 insertion Effects 0.000 claims description 8
- 229920002635 polyurethane Polymers 0.000 claims description 8
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 6
- SKMLRDJQWWVKDZ-UHFFFAOYSA-M lithium;ethoxymethanedithioate Chemical group [Li+].CCOC([S-])=S SKMLRDJQWWVKDZ-UHFFFAOYSA-M 0.000 claims description 4
- JCBJVAJGLKENNC-UHFFFAOYSA-M potassium ethyl xanthate Chemical compound [K+].CCOC([S-])=S JCBJVAJGLKENNC-UHFFFAOYSA-M 0.000 claims description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 3
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 claims description 3
- 229910001486 lithium perchlorate Inorganic materials 0.000 claims description 3
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 3
- UNYQKQSKNJVANG-UHFFFAOYSA-M potassium;(2-methylpropan-2-yl)oxymethanedithioate Chemical compound [K+].CC(C)(C)OC([S-])=S UNYQKQSKNJVANG-UHFFFAOYSA-M 0.000 claims description 3
- 239000012991 xanthate Substances 0.000 claims description 3
- 229910006095 SO2F Inorganic materials 0.000 claims description 2
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 claims description 2
- 150000004862 dioxolanes Chemical class 0.000 claims description 2
- NSKXNSIBOPUMIM-UHFFFAOYSA-M lithium (2-methylpropan-2-yl)oxymethanedithioate Chemical compound [Li+].CC(C)(C)OC([S-])=S NSKXNSIBOPUMIM-UHFFFAOYSA-M 0.000 claims description 2
- WNDVNPWSLIAORG-UHFFFAOYSA-M lithium 2-methylpropoxymethanedithioate Chemical compound [Li+].CC(C)COC([S-])=S WNDVNPWSLIAORG-UHFFFAOYSA-M 0.000 claims description 2
- MMWITBWRSMPITF-UHFFFAOYSA-M lithium carbamodithioate Chemical compound C(N)([S-])=S.[Li+] MMWITBWRSMPITF-UHFFFAOYSA-M 0.000 claims description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 claims description 2
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 claims description 2
- SKVWXDRVFXUPJX-UHFFFAOYSA-M lithium;carbamate Chemical compound [Li+].NC([O-])=O SKVWXDRVFXUPJX-UHFFFAOYSA-M 0.000 claims description 2
- VGYDTVNNDKLMHX-UHFFFAOYSA-N lithium;manganese;nickel;oxocobalt Chemical compound [Li].[Mn].[Ni].[Co]=O VGYDTVNNDKLMHX-UHFFFAOYSA-N 0.000 claims description 2
- KQDWYPLCKGVLDT-UHFFFAOYSA-M lithium;n,n-diethylcarbamodithioate Chemical compound [Li+].CCN(CC)C([S-])=S KQDWYPLCKGVLDT-UHFFFAOYSA-M 0.000 claims description 2
- CRAXZMAICBMTCW-UHFFFAOYSA-M potassium;2-methylpropoxymethanedithioate Chemical compound [K+].CC(C)COC([S-])=S CRAXZMAICBMTCW-UHFFFAOYSA-M 0.000 claims description 2
- FERZDALKDCSVRX-UHFFFAOYSA-M potassium;carbamate Chemical compound [K+].NC([O-])=O FERZDALKDCSVRX-UHFFFAOYSA-M 0.000 claims description 2
- TZWAQMQVPQXPQA-UHFFFAOYSA-M potassium;dithiocarboxyazanide Chemical compound [K+].NC([S-])=S TZWAQMQVPQXPQA-UHFFFAOYSA-M 0.000 claims description 2
- OFZRVUCVOAUMDT-UHFFFAOYSA-M potassium;n,n-diethylcarbamodithioate Chemical compound [K+].CCN(CC)C([S-])=S OFZRVUCVOAUMDT-UHFFFAOYSA-M 0.000 claims description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 2
- 150000001642 boronic acid derivatives Chemical class 0.000 claims 4
- 125000005587 carbonate group Chemical group 0.000 claims 2
- 230000015556 catabolic process Effects 0.000 claims 1
- 238000006731 degradation reaction Methods 0.000 claims 1
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 claims 1
- MJRXXQVZOMOCLX-UHFFFAOYSA-M lithium;n,n-dimethylcarbamodithioate Chemical compound [Li+].CN(C)C([S-])=S MJRXXQVZOMOCLX-UHFFFAOYSA-M 0.000 claims 1
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 claims 1
- 210000004027 cell Anatomy 0.000 description 392
- 239000002002 slurry Substances 0.000 description 170
- 239000011263 electroactive material Substances 0.000 description 100
- 239000002245 particle Substances 0.000 description 72
- 239000000463 material Substances 0.000 description 67
- 229910000077 silane Inorganic materials 0.000 description 62
- 241000894007 species Species 0.000 description 58
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical group [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 45
- 229910052717 sulfur Inorganic materials 0.000 description 43
- 239000007787 solid Substances 0.000 description 38
- 239000011593 sulfur Substances 0.000 description 38
- 238000002161 passivation Methods 0.000 description 36
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 description 29
- 230000000052 comparative effect Effects 0.000 description 28
- 239000002356 single layer Substances 0.000 description 28
- 125000000217 alkyl group Chemical group 0.000 description 25
- 239000011230 binding agent Substances 0.000 description 25
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 23
- 238000003860 storage Methods 0.000 description 23
- 125000000524 functional group Chemical group 0.000 description 22
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 19
- 238000006243 chemical reaction Methods 0.000 description 19
- 230000003534 oscillatory effect Effects 0.000 description 19
- 239000002210 silicon-based material Substances 0.000 description 18
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 17
- 230000015572 biosynthetic process Effects 0.000 description 16
- 238000007599 discharging Methods 0.000 description 16
- 239000002243 precursor Substances 0.000 description 16
- 125000003118 aryl group Chemical group 0.000 description 15
- 230000003993 interaction Effects 0.000 description 15
- 125000001072 heteroaryl group Chemical group 0.000 description 14
- 150000004756 silanes Chemical class 0.000 description 14
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical group [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 13
- 239000004615 ingredient Substances 0.000 description 13
- 229910052757 nitrogen Inorganic materials 0.000 description 13
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 13
- 229910052760 oxygen Inorganic materials 0.000 description 13
- 239000001301 oxygen Substances 0.000 description 13
- 125000003545 alkoxy group Chemical group 0.000 description 12
- 229910001416 lithium ion Inorganic materials 0.000 description 12
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 11
- 125000001931 aliphatic group Chemical group 0.000 description 11
- 239000011148 porous material Substances 0.000 description 11
- 150000003839 salts Chemical class 0.000 description 11
- 239000000243 solution Substances 0.000 description 11
- 125000001424 substituent group Chemical group 0.000 description 11
- 125000005842 heteroatom Chemical group 0.000 description 10
- 229910052759 nickel Inorganic materials 0.000 description 10
- 230000009257 reactivity Effects 0.000 description 10
- 229910000733 Li alloy Inorganic materials 0.000 description 9
- 229910001290 LiPF6 Inorganic materials 0.000 description 9
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 9
- 230000009286 beneficial effect Effects 0.000 description 9
- 229910052751 metal Inorganic materials 0.000 description 9
- 239000002184 metal Substances 0.000 description 9
- 150000002826 nitrites Chemical class 0.000 description 9
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 9
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 8
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 8
- 125000004432 carbon atom Chemical group C* 0.000 description 8
- 229920001940 conductive polymer Polymers 0.000 description 8
- 125000004122 cyclic group Chemical group 0.000 description 8
- 239000001989 lithium alloy Substances 0.000 description 8
- 150000002739 metals Chemical class 0.000 description 8
- 230000008569 process Effects 0.000 description 8
- WNXJIVFYUVYPPR-UHFFFAOYSA-N 1,3-dioxolane Chemical compound C1COCO1 WNXJIVFYUVYPPR-UHFFFAOYSA-N 0.000 description 7
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 7
- 239000004642 Polyimide Substances 0.000 description 7
- 125000002252 acyl group Chemical group 0.000 description 7
- 230000008901 benefit Effects 0.000 description 7
- 229910052736 halogen Inorganic materials 0.000 description 7
- 150000002367 halogens Chemical class 0.000 description 7
- 229910052698 phosphorus Inorganic materials 0.000 description 7
- 239000011574 phosphorus Substances 0.000 description 7
- 229920001721 polyimide Polymers 0.000 description 7
- 239000000047 product Substances 0.000 description 7
- KLLQVNFCMHPYGL-UHFFFAOYSA-N 5h-oxathiole 2,2-dioxide Chemical compound O=S1(=O)OCC=C1 KLLQVNFCMHPYGL-UHFFFAOYSA-N 0.000 description 6
- 229910013553 LiNO Inorganic materials 0.000 description 6
- 239000002033 PVDF binder Substances 0.000 description 6
- 239000004698 Polyethylene Substances 0.000 description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 6
- 125000003342 alkenyl group Chemical group 0.000 description 6
- 125000000304 alkynyl group Chemical group 0.000 description 6
- 239000006182 cathode active material Substances 0.000 description 6
- 229920001577 copolymer Polymers 0.000 description 6
- 239000010949 copper Substances 0.000 description 6
- 238000010586 diagram Methods 0.000 description 6
- 229940052303 ethers for general anesthesia Drugs 0.000 description 6
- 239000007789 gas Substances 0.000 description 6
- 239000000178 monomer Substances 0.000 description 6
- 150000002823 nitrates Chemical class 0.000 description 6
- 229920000570 polyether Polymers 0.000 description 6
- 229920000573 polyethylene Polymers 0.000 description 6
- 150000008117 polysulfides Polymers 0.000 description 6
- 239000000758 substrate Substances 0.000 description 6
- ZUHZGEOKBKGPSW-UHFFFAOYSA-N tetraglyme Chemical compound COCCOCCOCCOCCOC ZUHZGEOKBKGPSW-UHFFFAOYSA-N 0.000 description 6
- UUEWCQRISZBELL-UHFFFAOYSA-N 3-trimethoxysilylpropane-1-thiol Chemical compound CO[Si](OC)(OC)CCCS UUEWCQRISZBELL-UHFFFAOYSA-N 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 5
- 229910002651 NO3 Inorganic materials 0.000 description 5
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 5
- 239000004952 Polyamide Substances 0.000 description 5
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical group [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 5
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 description 5
- 125000002015 acyclic group Chemical group 0.000 description 5
- 229910052782 aluminium Inorganic materials 0.000 description 5
- 125000003277 amino group Chemical group 0.000 description 5
- 150000001768 cations Chemical class 0.000 description 5
- 239000000919 ceramic Substances 0.000 description 5
- SBZXBUIDTXKZTM-UHFFFAOYSA-N diglyme Chemical compound COCCOCCOC SBZXBUIDTXKZTM-UHFFFAOYSA-N 0.000 description 5
- 125000005843 halogen group Chemical group 0.000 description 5
- 229910001959 inorganic nitrate Inorganic materials 0.000 description 5
- 238000009830 intercalation Methods 0.000 description 5
- 230000000670 limiting effect Effects 0.000 description 5
- 239000011572 manganese Substances 0.000 description 5
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 5
- 230000001483 mobilizing effect Effects 0.000 description 5
- 150000002894 organic compounds Chemical class 0.000 description 5
- 229940082615 organic nitrates used in cardiac disease Drugs 0.000 description 5
- 229920002647 polyamide Polymers 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 229910052710 silicon Inorganic materials 0.000 description 5
- YFNKIDBQEZZDLK-UHFFFAOYSA-N triglyme Chemical compound COCCOCCOCCOC YFNKIDBQEZZDLK-UHFFFAOYSA-N 0.000 description 5
- 229920002554 vinyl polymer Polymers 0.000 description 5
- DHKHKXVYLBGOIT-UHFFFAOYSA-N 1,1-Diethoxyethane Chemical compound CCOC(C)OCC DHKHKXVYLBGOIT-UHFFFAOYSA-N 0.000 description 4
- 229920002302 Nylon 6,6 Polymers 0.000 description 4
- 239000004696 Poly ether ether ketone Substances 0.000 description 4
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 150000001412 amines Chemical class 0.000 description 4
- 125000001769 aryl amino group Chemical group 0.000 description 4
- 125000004104 aryloxy group Chemical group 0.000 description 4
- IWOUKMZUPDVPGQ-UHFFFAOYSA-N barium nitrate Chemical compound [Ba+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O IWOUKMZUPDVPGQ-UHFFFAOYSA-N 0.000 description 4
- NLSCHDZTHVNDCP-UHFFFAOYSA-N caesium nitrate Chemical compound [Cs+].[O-][N+]([O-])=O NLSCHDZTHVNDCP-UHFFFAOYSA-N 0.000 description 4
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 description 4
- 230000003197 catalytic effect Effects 0.000 description 4
- IJOOHPMOJXWVHK-UHFFFAOYSA-N chlorotrimethylsilane Chemical compound C[Si](C)(C)Cl IJOOHPMOJXWVHK-UHFFFAOYSA-N 0.000 description 4
- 229910052802 copper Inorganic materials 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000000945 filler Substances 0.000 description 4
- FFUAGWLWBBFQJT-UHFFFAOYSA-N hexamethyldisilazane Chemical compound C[Si](C)(C)N[Si](C)(C)C FFUAGWLWBBFQJT-UHFFFAOYSA-N 0.000 description 4
- 238000001095 inductively coupled plasma mass spectrometry Methods 0.000 description 4
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 description 4
- 239000011777 magnesium Substances 0.000 description 4
- 150000002828 nitro derivatives Chemical class 0.000 description 4
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 4
- 229920002627 poly(phosphazenes) Polymers 0.000 description 4
- 229920002401 polyacrylamide Polymers 0.000 description 4
- 229920002530 polyetherether ketone Polymers 0.000 description 4
- 229920001451 polypropylene glycol Polymers 0.000 description 4
- FGIUAXJPYTZDNR-UHFFFAOYSA-N potassium nitrate Chemical compound [K+].[O-][N+]([O-])=O FGIUAXJPYTZDNR-UHFFFAOYSA-N 0.000 description 4
- 230000009467 reduction Effects 0.000 description 4
- 239000010703 silicon Substances 0.000 description 4
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Chemical compound [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 description 4
- LPXPTNMVRIOKMN-UHFFFAOYSA-M sodium nitrite Chemical compound [Na+].[O-]N=O LPXPTNMVRIOKMN-UHFFFAOYSA-M 0.000 description 4
- 238000006467 substitution reaction Methods 0.000 description 4
- 239000000725 suspension Substances 0.000 description 4
- 229910052723 transition metal Inorganic materials 0.000 description 4
- 229910000319 transition metal phosphate Inorganic materials 0.000 description 4
- PYOKUURKVVELLB-UHFFFAOYSA-N trimethyl orthoformate Chemical compound COC(OC)OC PYOKUURKVVELLB-UHFFFAOYSA-N 0.000 description 4
- RYHBNJHYFVUHQT-UHFFFAOYSA-N 1,4-Dioxane Chemical compound C1COCCO1 RYHBNJHYFVUHQT-UHFFFAOYSA-N 0.000 description 3
- DURPTKYDGMDSBL-UHFFFAOYSA-N 1-butoxybutane Chemical compound CCCCOCCCC DURPTKYDGMDSBL-UHFFFAOYSA-N 0.000 description 3
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
- KXDHJXZQYSOELW-UHFFFAOYSA-N Carbamic acid Chemical group NC(O)=O KXDHJXZQYSOELW-UHFFFAOYSA-N 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- 229910013733 LiCo Inorganic materials 0.000 description 3
- 229910052493 LiFePO4 Inorganic materials 0.000 description 3
- 229910013870 LiPF 6 Inorganic materials 0.000 description 3
- 229910019142 PO4 Inorganic materials 0.000 description 3
- 239000007983 Tris buffer Substances 0.000 description 3
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- 150000007513 acids Chemical class 0.000 description 3
- 239000011149 active material Substances 0.000 description 3
- 125000003282 alkyl amino group Chemical group 0.000 description 3
- 125000004429 atom Chemical group 0.000 description 3
- 239000011575 calcium Substances 0.000 description 3
- 125000002837 carbocyclic group Chemical group 0.000 description 3
- 239000010406 cathode material Substances 0.000 description 3
- 230000022131 cell cycle Effects 0.000 description 3
- 210000003850 cellular structure Anatomy 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 239000004020 conductor Substances 0.000 description 3
- 150000004292 cyclic ethers Chemical class 0.000 description 3
- 238000002484 cyclic voltammetry Methods 0.000 description 3
- 150000002148 esters Chemical class 0.000 description 3
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 3
- 239000012530 fluid Substances 0.000 description 3
- 239000011888 foil Substances 0.000 description 3
- 230000006870 function Effects 0.000 description 3
- 238000004868 gas analysis Methods 0.000 description 3
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 3
- 238000010348 incorporation Methods 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 3
- 239000011244 liquid electrolyte Substances 0.000 description 3
- IDNHOWMYUQKKTI-UHFFFAOYSA-M lithium nitrite Chemical compound [Li+].[O-]N=O IDNHOWMYUQKKTI-UHFFFAOYSA-M 0.000 description 3
- CAIZIGKCPQJNCW-UHFFFAOYSA-N nitric acid;pyridine Chemical compound O[N+]([O-])=O.C1=CC=NC=C1 CAIZIGKCPQJNCW-UHFFFAOYSA-N 0.000 description 3
- 125000000449 nitro group Chemical group [O-][N+](*)=O 0.000 description 3
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 3
- 239000010452 phosphate Substances 0.000 description 3
- 235000021317 phosphate Nutrition 0.000 description 3
- 125000002467 phosphate group Chemical group [H]OP(=O)(O[H])O[*] 0.000 description 3
- 229920001197 polyacetylene Polymers 0.000 description 3
- 229920002239 polyacrylonitrile Polymers 0.000 description 3
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- 125000003785 benzimidazolyl group Chemical group N1=C(NC2=C1C=CC=C2)* 0.000 description 1
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- 238000000576 coating method Methods 0.000 description 1
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- 125000001995 cyclobutyl group Chemical group [H]C1([H])C([H])([H])C([H])(*)C1([H])[H] 0.000 description 1
- 125000000113 cyclohexyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])(*)C([H])([H])C1([H])[H] 0.000 description 1
- 125000001511 cyclopentyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])(*)C1([H])[H] 0.000 description 1
- 125000001559 cyclopropyl group Chemical group [H]C1([H])C([H])([H])C1([H])* 0.000 description 1
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- 150000002334 glycols Chemical class 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- NDEMNVPZDAFUKN-UHFFFAOYSA-N guanidine;nitric acid Chemical compound NC(N)=N.O[N+]([O-])=O.O[N+]([O-])=O NDEMNVPZDAFUKN-UHFFFAOYSA-N 0.000 description 1
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- 125000001188 haloalkyl group Chemical group 0.000 description 1
- 125000004446 heteroarylalkyl group Chemical group 0.000 description 1
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- 150000002430 hydrocarbons Chemical class 0.000 description 1
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
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- 125000004857 imidazopyridinyl group Chemical group N1C(=NC2=C1C=CC=N2)* 0.000 description 1
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- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000011147 inorganic material Substances 0.000 description 1
- 229920000592 inorganic polymer Polymers 0.000 description 1
- 230000002687 intercalation Effects 0.000 description 1
- 230000037427 ion transport Effects 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- 125000000959 isobutyl group Chemical group [H]C([H])([H])C([H])(C([H])([H])[H])C([H])([H])* 0.000 description 1
- 125000001449 isopropyl group Chemical group [H]C([H])([H])C([H])(*)C([H])([H])[H] 0.000 description 1
- GAPFWGOSHOCNBM-UHFFFAOYSA-N isopropyl nitrate Chemical compound CC(C)O[N+]([O-])=O GAPFWGOSHOCNBM-UHFFFAOYSA-N 0.000 description 1
- SKRDXYBATCVEMS-UHFFFAOYSA-N isopropyl nitrite Chemical compound CC(C)ON=O SKRDXYBATCVEMS-UHFFFAOYSA-N 0.000 description 1
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- YQNQTEBHHUSESQ-UHFFFAOYSA-N lithium aluminate Chemical compound [Li+].[O-][Al]=O YQNQTEBHHUSESQ-UHFFFAOYSA-N 0.000 description 1
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- PAZHGORSDKKUPI-UHFFFAOYSA-N lithium metasilicate Chemical compound [Li+].[Li+].[O-][Si]([O-])=O PAZHGORSDKKUPI-UHFFFAOYSA-N 0.000 description 1
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Images
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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
-
- 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
- H01M4/0402—Methods of deposition of the material
- H01M4/0407—Methods of deposition of the material by coating on an electrolyte layer
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
- C25B11/095—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds at least one of the compounds being organic
-
- 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
- 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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
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Description
例1~3および比較例1~7では、特に明記しない限り、電気化学セルは次の方法で調製した。第一電極(アノード)は、ポリエチレンテレフタレート(PET)基板上に配置された厚さ200nmCu集電体に配置された真空蒸着Li(厚さ15または25μm)であった。多孔質セパレーターは厚さ25μmのポリオレフィンフィルム(Celgard2325)で、第二電極(カソード)は、活性カソード材料(ACM)が集電体の両側に約19.3mg/cm2の量で厚さ20μmのアルミニウム基板集電体にコーティングされたニッケルマンガンコバルト(BASF NCM622)である。上記の構成要素は、アノード/セパレーター/カソード/セパレーター/アノードの積層構造に組み立てられた。カソードの総表面積は100cm2であった。フォイルポーチでセルコンポーネントを密封した後、適切な量の電解質を追加した(通常、25μmリチウムセルには0.55mLを使用し、15μmリチウムセルには0.6mLを使用した)。次に、セルパッケージを真空密封した。これらのセルは、24時間電解液に無制限に浸された。
例4:粉末状の約37gのニッケルマンガンコバルトカソード(NCM523、BASFから入手)を125℃の真空オーブンで一晩乾燥させた。この乾燥粉末17gを、炭酸ジメチル(DMC)中の0.5Mテトラエチルオルトシリケート(TEOS)100mLで攪拌し、35℃で一晩保持した。このステップの後、溶液を数時間沈降させ、上清をデカントした。残りの粉末をDMCですすぎ、125℃の真空オーブンで一晩乾燥させた。次に、粉末を使用して、カソードスラリーを形成した。スラリーは流体のような特性を示し、6時間後にゲルを形成しなかった。
例8-13では、特に明記しない限り、電気化学セルは以下の方法で調製された。第一電極(負極)はPET基板上に配置された厚さ200nmのCu集電体上に配置された(厚さ14μm)を真空蒸着したLiである。多孔質セパレーターは、厚さ9μmのポリオレフィンフィルム(Entek EP)で、第二電極(カソード)は、活性カソード材料(ACM)で厚さ20μmのアルミニウム基板集電体にコーティングされたニッケルマンガンコバルト(BASF NCM721)である。集電体の両側に約20.1mg/cm2の負荷。上記のコンポーネントは、アノード/セパレーター/カソード/セパレーター/アノードの積層構造に組み立てられた。カソードの総表面積は100cm2であった。フォイルポーチでセルコンポーネントを密封した後、0.5mLの電解質を加えた。次に、セルパッケージを真空密封した。これらのセルは、24時間電解液に無制限に浸された。
セルを電解液に浸した後、10kg/cm2の圧力をセルに加え、この圧力でセルを循環させた。充放電サイクルは、次の条件下で実行された。30mAで4.4Vまで充電し、その後4.4Vで10mAまでテーパーし、120mAで3.2Vまで放電の3回のサイクル。75mAでさらに4.4Vに充電し、4.4Vで10mAまでテーパーし、次に300Vで3.2Vに放電する。表5に示すように、電解質にVC、LiBOB、及びFECを含むバッテリー(例12)はFECとVCまたはLiBOBのいずれかのみを含む、またはFECとVCとLiBOBのいずれも含まない電池よりもサイクル寿命が大幅に改善された(例8-10)。また、表5に示すように、電解質にPES、LiBOB、及びFECを含むバッテリー(例13)は、FECとPESとLiBOBのいずれかのみ、またはFECとPESとLiBOBのいずれも含まないバッテリーよりもサイクル寿命が大幅に改善された(例8、9、および11)。ただし、VC、PES、LiBOB、およびFECの一つ以上が不足しているバッテリーも、相当のサイクル寿命を示した。
Claims (41)
- 以下を含む電気化学セル:
リチウムを含む第一電極(ここで第一電極は第一表面を含む)
第二電極(ここで第二電極は第二表面を含む)
電解質;
第一不動態化剤(ここで第一不動態化剤はキサンテート基を含む種を含む)
第二不動態化剤(ここで第二不動態化剤は(オキサラト)ボレート基を含む種を含み、第二不動態化剤は、電解質中に0.2wt%以上で存在する)。 - 以下を含む電気化学セル:
リチウムを含む第一電極(ここで第一電極は第一表面を含む)
第二電極(ここで第二電極は第二表面を含む)
電解質;
第一不動態化剤(ここで第一不動態化剤はキサンテート基を含む種を含む)
第二不動態化剤(ここで第二不動態化剤は、リチウムジフルオロ(オキサラト)ボレート、セルサイクル中にカソード上に層を形成するために重合を受けることができる種、およびビニル基を含まないが電気化学セルサイクル時にビニル基を発生させることができる種の一以上を含む)。 - 以下を含む電気化学セル:
リチウムを含む第一電極(ここで第一電極は第一表面を含む)
第二電極(ここで第二電極は第二表面を含む)
電解質;
第一不動態化剤(ここで第一不動態化剤はN-O化合物を含む)
第二不動態化剤(ここで第二不動態化剤は、セルサイクル中にカソード上に層を形成するために重合を受けることができる種を含む)
(ここで第二電極は、リチウムに対して2.8V以上4.5V以下の電圧を有する)。 - 以下を含む電気化学セル:
リチウムを含む第一電極(ここで第一電極は第一表面を含む)
第二電極(ここで第二電極は第二表面を含む)
電解質;
第一不動態化剤(ここで第一不動態化剤はカリウムtert-ブチルキサンテートを含む)
第二不動態化剤(ここで第二不動態化剤は、(オキサラト)ボレート基を含む種、セルサイクル中にカソード上に層を形成するために重合を受けることができる種、ビニル基を含む種、およびビニル基を含まないが電気化学セルサイクル時にビニル基を発生させることができる種の一以上を含む)。 - (オキサラト)ボレート塩を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- (オキサラト)ボレート塩がリチウムビス(オキサラト)ボレートを含む、請求項5に記載の電気化学セル。
- (オキサラト)ボレート塩がリチウムジフルオロ(オキサラト)ボレートを含む、請求項5に記載の電気化学セル。
- 第二不動態化剤がフルオロエチレンカーボネートを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二不動態化剤がジフルオロエチレンカーボネートを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が硝酸リチウムを含み、第二不動態化剤がさらにリチウムジフルオロ(オキサラト)ボレートを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が硝酸リチウムを含み、第二不動態化剤がリチウムビス(オキサラト)ボレートとフルオロエチレンカーボネートの両方を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が硝酸リチウムを含み、第二不動態化剤がリチウムビス(オキサラト)ボレート、フルオロエチレンカーボネート、およびジフルオロエチレンカーボネートのそれぞれを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が硝酸リチウムを含み、第二不動態化剤がリチウムジフルオロ(オキサラト)ボレート、フルオロエチレンカーボネート、およびジフルオロエチレンカーボネートのそれぞれを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が溶媒である、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が非溶媒である、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が電解質に可溶性または混和性の添加剤である、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤がリチウム塩を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤がキサントゲン酸リチウム、エチルキサントゲン酸リチウム、イソブチルキサントゲン酸リチウム、tert-ブチルキサントゲン酸リチウム、キサントゲン酸カリウム、エチルキサントゲン酸カリウム、イソブチルキサントゲン酸カリウム、tert-ブチルキサントゲン酸カリウム、および/またはキサンテート官能基を含むポリマーの一以上を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤がカルバミン酸リチウム、ジチオカルバミン酸リチウム、ポリカルバメート、ジエチルジチオカルバミン酸リチウム、N、N-ジメチルジチオカルバミン酸リチウム、カルバミン酸カリウム、ジチオカルバミン酸カリウム、および/または、ジエチルジチオカルバミン酸カリウムを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二電極がリチウムに対して2.8V以上4.5V以下の電圧を有する、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二電極がリチウム挿入電極である、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二電極がリチウムニッケルマンガンコバルト酸化物を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二電極がリチウムニッケルコバルトアルミニウム酸化物を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二電極がコバルト酸リチウムを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二電極がリン酸鉄リチウムを含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 電解質が溶媒を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 溶媒がカーボネート基を含む、請求項26に記載の電気化学セル。
- 電解質がジメチルカーボネート、ジエチルカーボネート、エチルメチルカーボネート、プロピレンカーボネート、ジオキソラン類、ジメトキシエタン、およびエチレンカーボネートの一以上を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 溶媒がジメチルカーボネートとエチレンカーボネートの混合物を含む、請求項26に記載の電気化学セル。
- 電解質がリチウム塩を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 電解質が過塩素酸リチウム、ヘキサフルオロヒ酸リチウム、テトラフルオロホウ酸リチウム、トリフルオロメタンスルホン酸リチウム、およびリチウムビス(トリフルオロメタンスルホニル)イミド、ヘキサフルオロリン酸リチウム、およびLiN(SO2F)2の一以上を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第一不動態化剤が第一表面を不動態化するように構成および配置されている、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二不動態化剤が第二電極の第二表面上の第一不動態化剤の分解を低減するように構成及び配置されている、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二不動態化剤が第二電極の第二表面上の電解質成分の分解を低減するように構成及び配置されている、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二不動態化剤が電解質成分の酸化を低減するように構成及び配置されている、請求項1~4のいずれか一項に記載の電気化学セル。
- 保護層をさらに含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 保護層が第一電極上に配置される、請求項36に記載の電気化学セル。
- 保護層が多孔質である、請求項36に記載の電気化学セル。
- 保護層が約25%以上約80%以下の多孔度を有する、請求項36に記載の電気化学セル。
- 第二不動態化剤がフルオロエチレンカーボネートを含み、第二電極がリチウム挿入電極であり、電解質がカーボネート基を含む溶媒を含む、請求項1~4のいずれか一項に記載の電気化学セル。
- 第二不動態化剤がリチウムビス(オキサラト)ボレートを含む(オキサラト)ボレート塩を含み、電解質がジメチルカーボネートとエチレンカーボネートの混合物を含む溶媒を含む、請求項1~4のいずれか一項に記載の電気化学セル。
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