JP2022538377A - 再充電可能なバッテリーセル - Google Patents
再充電可能なバッテリーセル Download PDFInfo
- Publication number
- JP2022538377A JP2022538377A JP2021566341A JP2021566341A JP2022538377A JP 2022538377 A JP2022538377 A JP 2022538377A JP 2021566341 A JP2021566341 A JP 2021566341A JP 2021566341 A JP2021566341 A JP 2021566341A JP 2022538377 A JP2022538377 A JP 2022538377A
- Authority
- JP
- Japan
- Prior art keywords
- rechargeable battery
- lithium
- battery cell
- electrolyte
- metal
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000003792 electrolyte Substances 0.000 claims abstract description 163
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 125
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 108
- 229910052751 metal Inorganic materials 0.000 claims abstract description 84
- 239000002184 metal Substances 0.000 claims abstract description 84
- 150000003839 salts Chemical class 0.000 claims abstract description 76
- 150000002739 metals Chemical class 0.000 claims abstract description 20
- 125000001424 substituent group Chemical group 0.000 claims abstract description 9
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 7
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 7
- 230000000737 periodic effect Effects 0.000 claims abstract description 6
- 125000001072 heteroaryl group Chemical group 0.000 claims abstract description 5
- 125000006374 C2-C10 alkenyl group Chemical group 0.000 claims abstract description 4
- 125000005865 C2-C10alkynyl group Chemical group 0.000 claims abstract description 4
- 125000000753 cycloalkyl group Chemical group 0.000 claims abstract description 4
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 claims abstract description 3
- 229910052783 alkali metal Inorganic materials 0.000 claims abstract description 3
- 150000001340 alkali metals Chemical class 0.000 claims abstract description 3
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims abstract description 3
- 150000001342 alkaline earth metals Chemical class 0.000 claims abstract description 3
- 229910052796 boron Inorganic materials 0.000 claims abstract description 3
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 claims description 140
- -1 acyclic sulfonates Chemical class 0.000 claims description 61
- 239000011149 active material Substances 0.000 claims description 52
- 150000001875 compounds Chemical class 0.000 claims description 44
- 239000000203 mixture Substances 0.000 claims description 39
- 125000004122 cyclic group Chemical group 0.000 claims description 26
- 239000011230 binding agent Substances 0.000 claims description 24
- 239000000463 material Substances 0.000 claims description 18
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 17
- 239000000126 substance Substances 0.000 claims description 16
- 238000006243 chemical reaction Methods 0.000 claims description 15
- 239000011572 manganese Substances 0.000 claims description 14
- 239000006262 metallic foam Substances 0.000 claims description 14
- 239000011888 foil Substances 0.000 claims description 13
- 229910019142 PO4 Inorganic materials 0.000 claims description 10
- 238000000151 deposition Methods 0.000 claims description 10
- 238000009830 intercalation Methods 0.000 claims description 10
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 10
- 230000002687 intercalation Effects 0.000 claims description 9
- 229920000642 polymer Polymers 0.000 claims description 9
- 125000002015 acyclic group Chemical group 0.000 claims description 8
- 239000000654 additive Substances 0.000 claims description 8
- 229910052748 manganese Inorganic materials 0.000 claims description 8
- 229910052759 nickel Inorganic materials 0.000 claims description 8
- 235000021317 phosphate Nutrition 0.000 claims description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 7
- 229910052731 fluorine Inorganic materials 0.000 claims description 7
- 150000002736 metal compounds Chemical class 0.000 claims description 7
- 125000006656 (C2-C4) alkenyl group Chemical group 0.000 claims description 6
- 125000006650 (C2-C4) alkynyl group Chemical group 0.000 claims description 6
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 claims description 6
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 claims description 6
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 claims description 6
- 125000003636 chemical group Chemical group 0.000 claims description 6
- 229910001537 lithium tetrachloroaluminate Inorganic materials 0.000 claims description 6
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims description 5
- 230000000996 additive effect Effects 0.000 claims description 5
- 229910052799 carbon Inorganic materials 0.000 claims description 5
- 229910017052 cobalt Inorganic materials 0.000 claims description 5
- 239000010941 cobalt Substances 0.000 claims description 5
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 5
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 claims description 5
- 239000011737 fluorine Substances 0.000 claims description 5
- 125000001153 fluoro group Chemical group F* 0.000 claims description 5
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 claims description 5
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims description 5
- 150000003013 phosphoric acid derivatives Chemical class 0.000 claims description 5
- 229910052698 phosphorus Inorganic materials 0.000 claims description 5
- 239000011574 phosphorus Substances 0.000 claims description 5
- 229910052710 silicon Inorganic materials 0.000 claims description 5
- 238000003860 storage Methods 0.000 claims description 5
- 239000011232 storage material Substances 0.000 claims description 5
- BQCIDUSAKPWEOX-UHFFFAOYSA-N 1,1-Difluoroethene Chemical compound FC(F)=C BQCIDUSAKPWEOX-UHFFFAOYSA-N 0.000 claims description 4
- 239000002033 PVDF binder Substances 0.000 claims description 4
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims description 4
- 150000001735 carboxylic acids Chemical class 0.000 claims description 4
- 229910052742 iron Inorganic materials 0.000 claims description 4
- 229910001092 metal group alloy Inorganic materials 0.000 claims description 4
- 229910044991 metal oxide Inorganic materials 0.000 claims description 4
- 150000004706 metal oxides Chemical class 0.000 claims description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 4
- 229920001897 terpolymer Polymers 0.000 claims description 4
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 claims description 4
- 229910052718 tin Inorganic materials 0.000 claims description 4
- 229920002134 Carboxymethyl cellulose Polymers 0.000 claims description 3
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims description 3
- 239000003513 alkali Substances 0.000 claims description 3
- 150000001339 alkali metal compounds Chemical class 0.000 claims description 3
- 125000000217 alkyl group Chemical group 0.000 claims description 3
- 229910045601 alloy Inorganic materials 0.000 claims description 3
- 239000000956 alloy Substances 0.000 claims description 3
- 150000003863 ammonium salts Chemical class 0.000 claims description 3
- 125000003118 aryl group Chemical group 0.000 claims description 3
- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 claims description 3
- 239000001768 carboxy methyl cellulose Substances 0.000 claims description 3
- 235000010948 carboxy methyl cellulose Nutrition 0.000 claims description 3
- 239000008112 carboxymethyl-cellulose Substances 0.000 claims description 3
- 229910002804 graphite Inorganic materials 0.000 claims description 3
- 239000010439 graphite Substances 0.000 claims description 3
- HCDGVLDPFQMKDK-UHFFFAOYSA-N hexafluoropropylene Chemical group FC(F)=C(F)C(F)(F)F HCDGVLDPFQMKDK-UHFFFAOYSA-N 0.000 claims description 3
- 150000002642 lithium compounds Chemical class 0.000 claims description 3
- SNOOUWRIMMFWNE-UHFFFAOYSA-M sodium;6-[(3,4,5-trimethoxybenzoyl)amino]hexanoate Chemical compound [Na+].COC1=CC(C(=O)NCCCCCC([O-])=O)=CC(OC)=C1OC SNOOUWRIMMFWNE-UHFFFAOYSA-M 0.000 claims description 3
- 229910052596 spinel Inorganic materials 0.000 claims description 3
- 239000011029 spinel Substances 0.000 claims description 3
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical group O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 2
- KGIGUEBEKRSTEW-UHFFFAOYSA-N 2-vinylpyridine Chemical compound C=CC1=CC=CC=N1 KGIGUEBEKRSTEW-UHFFFAOYSA-N 0.000 claims description 2
- BJWMSGRKJIOCNR-UHFFFAOYSA-N 4-ethenyl-1,3-dioxolan-2-one Chemical compound C=CC1COC(=O)O1 BJWMSGRKJIOCNR-UHFFFAOYSA-N 0.000 claims description 2
- KFDVPJUYSDEJTH-UHFFFAOYSA-N 4-ethenylpyridine Chemical compound C=CC1=CC=NC=C1 KFDVPJUYSDEJTH-UHFFFAOYSA-N 0.000 claims description 2
- DJHGAFSJWGLOIV-UHFFFAOYSA-K Arsenate3- Chemical class [O-][As]([O-])([O-])=O DJHGAFSJWGLOIV-UHFFFAOYSA-K 0.000 claims description 2
- 150000004645 aluminates Chemical class 0.000 claims description 2
- 229910000147 aluminium phosphate Inorganic materials 0.000 claims description 2
- 150000001491 aromatic compounds Chemical class 0.000 claims description 2
- 238000009835 boiling Methods 0.000 claims description 2
- 150000001642 boronic acid derivatives Chemical class 0.000 claims description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 claims description 2
- 229910052804 chromium Inorganic materials 0.000 claims description 2
- 239000011651 chromium Substances 0.000 claims description 2
- 229910052802 copper Inorganic materials 0.000 claims description 2
- 150000001924 cycloalkanes Chemical class 0.000 claims description 2
- YNQRWVCLAIUHHI-UHFFFAOYSA-L dilithium;oxalate Chemical compound [Li+].[Li+].[O-]C(=O)C([O-])=O YNQRWVCLAIUHHI-UHFFFAOYSA-L 0.000 claims description 2
- 150000002148 esters Chemical class 0.000 claims description 2
- 229910052732 germanium Inorganic materials 0.000 claims description 2
- 239000011521 glass Substances 0.000 claims description 2
- 150000004820 halides Chemical class 0.000 claims description 2
- 125000000623 heterocyclic group Chemical group 0.000 claims description 2
- 229910001507 metal halide Inorganic materials 0.000 claims description 2
- 150000005309 metal halides Chemical class 0.000 claims description 2
- 229910001463 metal phosphate Inorganic materials 0.000 claims description 2
- 150000007522 mineralic acids Chemical class 0.000 claims description 2
- 150000002895 organic esters Chemical class 0.000 claims description 2
- 150000003891 oxalate salts Chemical class 0.000 claims description 2
- 229920000447 polyanionic polymer Polymers 0.000 claims description 2
- 125000004368 propenyl group Chemical group C(=CC)* 0.000 claims description 2
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 2
- 150000008053 sultones Chemical class 0.000 claims description 2
- 229910052719 titanium Inorganic materials 0.000 claims description 2
- 229910000314 transition metal oxide Inorganic materials 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- 229910052725 zinc Inorganic materials 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical group [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 claims 3
- 229910008336 SnCo Inorganic materials 0.000 claims 1
- 229910006898 SnSi Inorganic materials 0.000 claims 1
- 229910021387 carbon allotrope Inorganic materials 0.000 claims 1
- MPDOUGUGIVBSGZ-UHFFFAOYSA-N n-(cyclobutylmethyl)-3-(trifluoromethyl)aniline Chemical compound FC(F)(F)C1=CC=CC(NCC2CCC2)=C1 MPDOUGUGIVBSGZ-UHFFFAOYSA-N 0.000 claims 1
- 125000000008 (C1-C10) alkyl group Chemical group 0.000 abstract 1
- 125000005915 C6-C14 aryl group Chemical group 0.000 abstract 1
- 210000004027 cell Anatomy 0.000 description 209
- 238000012360 testing method Methods 0.000 description 63
- 238000011161 development Methods 0.000 description 30
- 230000018109 developmental process Effects 0.000 description 30
- 238000002474 experimental method Methods 0.000 description 23
- 238000000034 method Methods 0.000 description 16
- 239000002904 solvent Substances 0.000 description 16
- 150000002500 ions Chemical class 0.000 description 14
- 239000003960 organic solvent Substances 0.000 description 13
- 230000008569 process Effects 0.000 description 13
- 239000011247 coating layer Substances 0.000 description 12
- 238000000354 decomposition reaction Methods 0.000 description 9
- 239000011148 porous material Substances 0.000 description 9
- 125000004432 carbon atom Chemical group C* 0.000 description 8
- 230000008021 deposition Effects 0.000 description 8
- 239000011159 matrix material Substances 0.000 description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 8
- 239000004215 Carbon black (E152) Substances 0.000 description 7
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 7
- 229930195733 hydrocarbon Natural products 0.000 description 7
- 150000002430 hydrocarbons Chemical group 0.000 description 7
- 230000002427 irreversible effect Effects 0.000 description 7
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 7
- 229910001416 lithium ion Inorganic materials 0.000 description 7
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 6
- 238000000576 coating method Methods 0.000 description 6
- 239000010410 layer Substances 0.000 description 6
- 238000005259 measurement Methods 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 6
- 230000008901 benefit Effects 0.000 description 5
- 238000007599 discharging Methods 0.000 description 5
- 239000005486 organic electrolyte Substances 0.000 description 5
- 125000001979 organolithium group Chemical group 0.000 description 5
- 239000007774 positive electrode material Substances 0.000 description 5
- 125000004429 atom Chemical group 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 4
- 210000003850 cellular structure Anatomy 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
- 229940125904 compound 1 Drugs 0.000 description 4
- 238000003411 electrode reaction Methods 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- VGYDTVNNDKLMHX-UHFFFAOYSA-N lithium;manganese;nickel;oxocobalt Chemical compound [Li].[Mn].[Ni].[Co]=O VGYDTVNNDKLMHX-UHFFFAOYSA-N 0.000 description 4
- 238000011068 loading method Methods 0.000 description 4
- 239000012528 membrane Substances 0.000 description 4
- 238000002161 passivation Methods 0.000 description 4
- 229930195734 saturated hydrocarbon Natural products 0.000 description 4
- 125000006017 1-propenyl group Chemical group 0.000 description 3
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 3
- 229910013870 LiPF 6 Inorganic materials 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
- 150000001450 anions Chemical class 0.000 description 3
- 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 3
- 210000001787 dendrite Anatomy 0.000 description 3
- 229940021013 electrolyte solution Drugs 0.000 description 3
- 229920000840 ethylene tetrafluoroethylene copolymer Polymers 0.000 description 3
- 239000006260 foam Substances 0.000 description 3
- 239000003365 glass fiber Substances 0.000 description 3
- 229910010272 inorganic material Inorganic materials 0.000 description 3
- 239000011147 inorganic material Substances 0.000 description 3
- 125000001449 isopropyl group Chemical group [H]C([H])([H])C([H])(*)C([H])([H])[H] 0.000 description 3
- INHCSSUBVCNVSK-UHFFFAOYSA-L lithium sulfate Inorganic materials [Li+].[Li+].[O-]S([O-])(=O)=O INHCSSUBVCNVSK-UHFFFAOYSA-L 0.000 description 3
- DVATZODUVBMYHN-UHFFFAOYSA-K lithium;iron(2+);manganese(2+);phosphate Chemical compound [Li+].[Mn+2].[Fe+2].[O-]P([O-])([O-])=O DVATZODUVBMYHN-UHFFFAOYSA-K 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 3
- 230000007935 neutral effect Effects 0.000 description 3
- 239000011368 organic material Substances 0.000 description 3
- 229920000573 polyethylene Polymers 0.000 description 3
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 3
- 239000004810 polytetrafluoroethylene Substances 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 230000002829 reductive effect Effects 0.000 description 3
- 230000002441 reversible effect Effects 0.000 description 3
- 230000032258 transport Effects 0.000 description 3
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 3
- 125000006039 1-hexenyl group Chemical group 0.000 description 2
- 125000006023 1-pentenyl group Chemical group 0.000 description 2
- 125000000530 1-propynyl group Chemical group [H]C([H])([H])C#C* 0.000 description 2
- 125000003903 2-propenyl group Chemical group [H]C([*])([H])C([H])=C([H])[H] 0.000 description 2
- 125000001494 2-propynyl group Chemical group [H]C#CC([H])([H])* 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 229910003054 Li1.2Mn0.525Ni0.175Co0.1O2 Inorganic materials 0.000 description 2
- 229910010238 LiAlCl 4 Inorganic materials 0.000 description 2
- 229910010082 LiAlH Inorganic materials 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- KLARSDUHONHPRF-UHFFFAOYSA-N [Li].[Mn] Chemical compound [Li].[Mn] KLARSDUHONHPRF-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 2
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 description 2
- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 2
- 229940126214 compound 3 Drugs 0.000 description 2
- 239000013078 crystal Substances 0.000 description 2
- 125000001995 cyclobutyl group Chemical group [H]C1([H])C([H])([H])C([H])(*)C1([H])[H] 0.000 description 2
- 125000001511 cyclopentyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])(*)C1([H])[H] 0.000 description 2
- 125000001559 cyclopropyl group Chemical group [H]C1([H])C([H])([H])C1([H])* 0.000 description 2
- 230000006378 damage Effects 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000008151 electrolyte solution Substances 0.000 description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 2
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 2
- 230000007062 hydrolysis Effects 0.000 description 2
- 238000006460 hydrolysis reaction Methods 0.000 description 2
- 238000003780 insertion Methods 0.000 description 2
- 230000037431 insertion Effects 0.000 description 2
- 125000000959 isobutyl group Chemical group [H]C([H])([H])C([H])(C([H])([H])[H])C([H])([H])* 0.000 description 2
- 125000004491 isohexyl group Chemical group C(CCC(C)C)* 0.000 description 2
- 125000001972 isopentyl group Chemical group [H]C([H])([H])C([H])(C([H])([H])[H])C([H])([H])C([H])([H])* 0.000 description 2
- 229910003473 lithium bis(trifluoromethanesulfonyl)imide Inorganic materials 0.000 description 2
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical compound [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 2
- FRMOHNDAXZZWQI-UHFFFAOYSA-N lithium manganese(2+) nickel(2+) oxygen(2-) Chemical compound [O-2].[Mn+2].[Ni+2].[Li+] FRMOHNDAXZZWQI-UHFFFAOYSA-N 0.000 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 description 2
- 238000001000 micrograph Methods 0.000 description 2
- 125000004108 n-butyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 2
- 125000001280 n-hexyl group Chemical group C(CCCCC)* 0.000 description 2
- 125000000740 n-pentyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 2
- 125000004123 n-propyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])* 0.000 description 2
- 125000001624 naphthyl group Chemical group 0.000 description 2
- 239000007773 negative electrode material Substances 0.000 description 2
- 125000001971 neopentyl group Chemical group [H]C([*])([H])C(C([H])([H])[H])(C([H])([H])[H])C([H])([H])[H] 0.000 description 2
- 229910001317 nickel manganese cobalt oxide (NMC) Inorganic materials 0.000 description 2
- 238000006864 oxidative decomposition reaction Methods 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000004033 plastic Substances 0.000 description 2
- 229920003023 plastic Polymers 0.000 description 2
- 239000002985 plastic film Substances 0.000 description 2
- 229920006255 plastic film Polymers 0.000 description 2
- 229920000098 polyolefin Polymers 0.000 description 2
- 229920001155 polypropylene Polymers 0.000 description 2
- 125000002914 sec-butyl group Chemical group [H]C([H])([H])C([H])([H])C([H])(*)C([H])([H])[H] 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000007784 solid electrolyte Substances 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 125000000999 tert-butyl group Chemical group [H]C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 description 2
- 125000005913 (C3-C6) cycloalkyl group Chemical group 0.000 description 1
- 125000003229 2-methylhexyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])(C([H])([H])[H])C([H])([H])* 0.000 description 1
- 125000000882 C2-C6 alkenyl group Chemical group 0.000 description 1
- 125000003601 C2-C6 alkynyl group Chemical group 0.000 description 1
- 229910021580 Cobalt(II) chloride Inorganic materials 0.000 description 1
- 229910021582 Cobalt(II) fluoride Inorganic materials 0.000 description 1
- 229910021592 Copper(II) chloride Inorganic materials 0.000 description 1
- 229910021594 Copper(II) fluoride Inorganic materials 0.000 description 1
- 229910019573 CozO2 Inorganic materials 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 229910021577 Iron(II) chloride Inorganic materials 0.000 description 1
- 229910021578 Iron(III) chloride Inorganic materials 0.000 description 1
- 229910008555 Li1.2Mn0.6Ni0.2O2 Inorganic materials 0.000 description 1
- 229910008626 Li1.2Ni0.13Co0.13Mn0.54O2 Inorganic materials 0.000 description 1
- 229910001216 Li2S Inorganic materials 0.000 description 1
- 229910002986 Li4Ti5O12 Inorganic materials 0.000 description 1
- 229910010092 LiAlO2 Inorganic materials 0.000 description 1
- 229910013075 LiBF Inorganic materials 0.000 description 1
- 229910013063 LiBF 4 Inorganic materials 0.000 description 1
- 229910013178 LiBO2 Inorganic materials 0.000 description 1
- 229910013188 LiBOB Inorganic materials 0.000 description 1
- 229910000552 LiCF3SO3 Inorganic materials 0.000 description 1
- 229910012808 LiCoMnO4 Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
- 229910012488 LiNi0.55Mn0.30Co0.15O2 Inorganic materials 0.000 description 1
- 229910012748 LiNi0.5Mn0.3Co0.2O2 Inorganic materials 0.000 description 1
- 229910002099 LiNi0.5Mn1.5O4 Inorganic materials 0.000 description 1
- 229910011322 LiNi0.6Mn0.2Co0.2O2 Inorganic materials 0.000 description 1
- 229910011732 LiNi0.7Mn0.2Co0.1O2 Inorganic materials 0.000 description 1
- 229910015965 LiNi0.8Mn0.1Co0.1O2 Inorganic materials 0.000 description 1
- 229910014422 LiNi1/3Mn1/3Co1/3O2 Inorganic materials 0.000 description 1
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- 229910012513 LiSbF 6 Inorganic materials 0.000 description 1
- 229910021586 Nickel(II) chloride Inorganic materials 0.000 description 1
- 229910021587 Nickel(II) fluoride Inorganic materials 0.000 description 1
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- 239000004952 Polyamide Substances 0.000 description 1
- LMFMZUUUIFGRHQ-UHFFFAOYSA-K S(=O)(=O)([O-])F.[Fe+2].[Li+].S(=O)(=O)([O-])F.S(=O)(=O)([O-])F Chemical compound S(=O)(=O)([O-])F.[Fe+2].[Li+].S(=O)(=O)([O-])F.S(=O)(=O)([O-])F LMFMZUUUIFGRHQ-UHFFFAOYSA-K 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 229910021607 Silver chloride Inorganic materials 0.000 description 1
- 229910006854 SnOx Inorganic materials 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- SGYOHBMMKNRZRP-UHFFFAOYSA-M [Li+].[O-]S(Cl)(=O)=O Chemical compound [Li+].[O-]S(Cl)(=O)=O SGYOHBMMKNRZRP-UHFFFAOYSA-M 0.000 description 1
- IDSMHEZTLOUMLM-UHFFFAOYSA-N [Li].[O].[Co] Chemical class [Li].[O].[Co] IDSMHEZTLOUMLM-UHFFFAOYSA-N 0.000 description 1
- ZYXUQEDFWHDILZ-UHFFFAOYSA-N [Ni].[Mn].[Li] Chemical compound [Ni].[Mn].[Li] ZYXUQEDFWHDILZ-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
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- 150000001768 cations Chemical class 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 229940125782 compound 2 Drugs 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 description 1
- GWFAVIIMQDUCRA-UHFFFAOYSA-L copper(ii) fluoride Chemical compound [F-].[F-].[Cu+2] GWFAVIIMQDUCRA-UHFFFAOYSA-L 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 230000001351 cycling effect Effects 0.000 description 1
- 125000000582 cycloheptyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])([H])C([H])(*)C([H])([H])C1([H])[H] 0.000 description 1
- 125000006547 cyclononyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])(*)C([H])([H])C([H])([H])C1([H])[H] 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 229920002313 fluoropolymer Polymers 0.000 description 1
- 239000004811 fluoropolymer Substances 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 125000002541 furyl group Chemical group 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 229910052740 iodine Inorganic materials 0.000 description 1
- 230000037427 ion transport Effects 0.000 description 1
- 239000002608 ionic liquid Substances 0.000 description 1
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 description 1
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 1
- FZGIHSNZYGFUGM-UHFFFAOYSA-L iron(ii) fluoride Chemical compound [F-].[F-].[Fe+2] FZGIHSNZYGFUGM-UHFFFAOYSA-L 0.000 description 1
- SHXXPRJOPFJRHA-UHFFFAOYSA-K iron(iii) fluoride Chemical compound F[Fe](F)F SHXXPRJOPFJRHA-UHFFFAOYSA-K 0.000 description 1
- 238000005184 irreversible process Methods 0.000 description 1
- YQNQTEBHHUSESQ-UHFFFAOYSA-N lithium aluminate Chemical compound [Li+].[O-][Al]=O YQNQTEBHHUSESQ-UHFFFAOYSA-N 0.000 description 1
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- BVPMZCWLVVIHKO-UHFFFAOYSA-N lithium cobalt(2+) manganese(2+) oxygen(2-) Chemical compound [O-2].[Mn+2].[Co+2].[Li+] BVPMZCWLVVIHKO-UHFFFAOYSA-N 0.000 description 1
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical compound [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 description 1
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 description 1
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 1
- HZRMTWQRDMYLNW-UHFFFAOYSA-N lithium metaborate Chemical compound [Li+].[O-]B=O HZRMTWQRDMYLNW-UHFFFAOYSA-N 0.000 description 1
- 229910003002 lithium salt Inorganic materials 0.000 description 1
- 159000000002 lithium salts Chemical group 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000000691 measurement method Methods 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 125000003136 n-heptyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- QMMRZOWCJAIUJA-UHFFFAOYSA-L nickel dichloride Chemical compound Cl[Ni]Cl QMMRZOWCJAIUJA-UHFFFAOYSA-L 0.000 description 1
- DBJLJFTWODWSOF-UHFFFAOYSA-L nickel(ii) fluoride Chemical compound F[Ni]F DBJLJFTWODWSOF-UHFFFAOYSA-L 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910052755 nonmetal Inorganic materials 0.000 description 1
- 150000002843 nonmetals Chemical class 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000000075 oxide glass Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 229920002492 poly(sulfone) Polymers 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- XIUFWXXRTPHHDQ-UHFFFAOYSA-N prop-1-ene;1,1,2,2-tetrafluoroethene Chemical group CC=C.FC(F)=C(F)F XIUFWXXRTPHHDQ-UHFFFAOYSA-N 0.000 description 1
- 125000004309 pyranyl group Chemical group O1C(C=CC=C1)* 0.000 description 1
- 125000004076 pyridyl group Chemical group 0.000 description 1
- 125000000168 pyrrolyl group Chemical group 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 238000001953 recrystallisation Methods 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- FZHAPNGMFPVSLP-UHFFFAOYSA-N silanamine Chemical class [SiH3]N FZHAPNGMFPVSLP-UHFFFAOYSA-N 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 229910052814 silicon oxide Inorganic materials 0.000 description 1
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 201000009032 substance abuse Diseases 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 125000004434 sulfur atom Chemical group 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- RBTVSNLYYIMMKS-UHFFFAOYSA-N tert-butyl 3-aminoazetidine-1-carboxylate;hydrochloride Chemical compound Cl.CC(C)(C)OC(=O)N1CC(N)C1 RBTVSNLYYIMMKS-UHFFFAOYSA-N 0.000 description 1
- 125000001544 thienyl group Chemical group 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- VRSRNLHMYUACMN-UHFFFAOYSA-H trilithium;hexafluoroaluminum(3-) Chemical compound [Li+].[Li+].[Li+].[F-].[F-].[F-].[F-].[F-].[F-].[Al+3] VRSRNLHMYUACMN-UHFFFAOYSA-H 0.000 description 1
- 230000004222 uncontrolled growth Effects 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
Images
Classifications
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- C01G53/50—Nickelates containing alkali metals, e.g. LiNiO2 containing manganese of the type [MnO2]n-, e.g. Li(NixMn1-x)O2, Li(MyNixMn1-x-y)O2
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- C—CHEMISTRY; METALLURGY
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- C01G53/54—Nickelates containing alkali metals, e.g. LiNiO2 containing manganese of the type [Mn2O4]-, e.g. Li(NixMn2-x)O4, Li(MyNixMn2-x-y)O4
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- C07F—ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM
- C07F5/00—Compounds containing elements of Groups 3 or 13 of the Periodic Table
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Abstract
Description
-電気的性能が向上し、特にエネルギー密度が高い。
-負電極に安定したコーティング層を有し、それによってコーティング層の容量が低くなり、さらなる動作中に負電極でさらなる還元性電解質の分解が起こらない。
-SO2ベースの電解質を含み、これにより金属リチウムの堆積が可能な限り均一になる。
-導電性塩類の溶解度が高く、イオン伝導性と電子絶縁性に優れているため、イオン輸送を促進し、自己放電を最小限に抑えることができるSO2ベースの電解質を備える。
-セパレータ、電極材料、セルパック材料など、再充電可能なバッテリーセルの他の構成要素に対しても不活性であるSO2ベースの電解質を備える。
-電気的、機械的、熱的などの様々な誤使用に対して耐性がある。
-SO2ベースの電解質で構成されており、再充電可能なバッテリーセルのセル構成要素に含まれる残留水分量に対する安定性が向上している。
-広い電気化学的ウィンドウ(electrochemical window)を有するため、正電極での酸化的な電解質の分解が起こらない。
-過充電や深放電が改善され、自己放電が少ない。
-耐用年数の向上、特に使用可能な充放電サイクル数の増加を示す。
負電極の活物質は、金属リチウムである。つまり、リチウムは、再充電可能なバッテリーの活性金属でもある。前記リチウムは、前記再充電可能なバッテリーセルが充電されると、前記負電極の放電素子に堆積する。これは、負電極が金属リチウムに加えて、放電素子も有していることを意味する。この放電素子は、負電極の活物質の必要な電子伝導性接続を可能にする役割を果たす。このため、放電素子は、負電極の電極反応に関与する活物質と接触している。再充電可能なバッテリーセルが放電されると、金属リチウムはリチウムイオンに変換され、リチウムイオンは負電極から正電極に移動する。前記正電極がインターカレーション電極として設計されている場合、バッテリーセルの非充電状態におけるリチウムイオンは、少なくとも部分的に、正のインターカレーション電極の活物質のホストマトリックスに位置している。
SO2ベースの電解質に関する再充電可能なバッテリーセルの有利な発展形を以下に記載する。
-好ましくはC2-C4アルキルからの、特に好ましくはアルキル基2-プロピル、メチルおよびエチルからの、C1-C6アルキル;
-好ましくはC2-C4アルケニルからの、特に好ましくはアルケニル基のエテニルおよびプロペニルからの、C2-C6アルケニル;
-好ましくはC2-C4アルキニルからの、C2-C6アルキニル;
-C3-C6シクロアルキル;
-フェニル;および
-C5-C7ヘテロアリール
によって形成される群から選択される。
(i)5~99.4重量%の二酸化硫黄、
(ii)0.6~95重量%の第1導電性塩、
(iii)0~25重量%の第2導電性塩、および
(iv)0~10重量%の添加剤
の組成を有する。
(i)5~99.4重量%の二酸化硫黄、
(ii)0.6~95重量%の第1導電性塩、
(iii)0~25重量%の第2導電性塩、
(iv)0~10重量%の添加剤、および
(v)0~50重量%の有機溶媒
の組成を有する。
正電極に関する本発明による再充電可能なバッテリーセルの有利な発展形を、以下に説明する。
-M’は、Ti、V、Cr、Mn、Fe、Co、Ni、CuおよびZnからなる群から選択される少なくとも1つの金属である;
-M”は、元素周期表の第2族、第3族、第4族、第5族、第6族、第7族、第8族、第9族、第10族、第11族、第12族、第13族、第14族、第15族および第16族の元素により形成される群から選択される少なくとも1つの元素である;
-xおよびyは、互いに独立して、0より大きい数である;
-zは、0以上の数である;そして
-aは、0より大きい数字である。
mLi2MnO3・(1-m)LiM’O2、0<m<1で表される。
このような化合物の例としては、Li1.2Mn0.525Ni0.175Co0.1O2、Li1.2Mn0.6Ni0.2O2、またはLi1.2Ni0.13Co0.13Mn0.54O2が挙げられる。
タイプA:MXz←→+yLi M+ zLi(y/z)X
タイプB:X←→+yLi LiyX
本発明による再充電可能なバッテリーセルの有利な発展形は、その構造に関して以下に説明される。
後述する実施例で使用する参照電解質は、欧州特許第2954588号明細書(以下、[V3]とする)に記載されている方法で調製した。まず、塩化リチウム(LiCl)を120℃で3日間、真空下で乾燥させた。また、アルミニウム粒子(Al)を450℃で2日間、真空下で乾燥させた。LiCl、塩化アルミニウム(AlCl3)、およびAlを、AlCl3:LiCl:Alのモル比が1:1.06:0.35となるように、ガス抜き用の開口部を有するガラス瓶に入れて混合した。その後、このブレンド物を段階的に熱処理して溶融塩を生成した。冷却後、形成された塩の溶融物をろ過し、次に室温まで冷却し、最後に、LiAlCl4に対するSO2の所望のモル比が形成されるまで、SO2を加えた。このようにして形成された参照電解質は、LiAlCl4 *xSO2という組成を有し、ここでxは供給されたSO2の量に依存する。
以下に説明する実験のために、SO2ベースの電解質の4つの実施形態1,2,3および4を調製した(以下、電解質1,2,3および4と称する)。この目的のために、まず、以下の文献[V4],[V5]および[V6]に記載されている製造方法を用いて、式(I)による4種類の異なる第1導電性塩を調製した。
[V4]“I.Krossing,Chem.Eur.J.2001,7,490;
[V5]S.M.Ivanova et al, Chem.Eur.J.2001,7,503;
[V6]Tsujioka et al, J.Electrochem.Soc.,2004,151,A1418”
1)ライザーパイプ付きの圧力ピストンにおけるそれぞれの化合物1,2,3および4の受け入れ、
2)圧力ピストンの排気、
3)液体SO2の流入、および
4)目標量のSO2が添加されるまで、ステップ2+3を繰り返す。
後述する実験で用いた試験用フルセルは、セパレータで隔てられた2つの負電極と1つの正電極を有する再充電可能なバッテリーセルである。正電極には、活物質、導電性媒介剤、バインダーが含まれていた。正電極の活物質については、それぞれの実験で命名している。負電極は活物質として金属リチウムを含み、これは負電極の放電素子上に堆積させたもの、または既に存在していたものであった。正電極と負電極の放電素子はニッケル製であった。試験用フルセルには、それぞれ実験に必要な電解質、すなわち参照電解質、または電解質1,2,3もしくは4が充填されていた。
コーティング層の容量:
最初のサイクルで負電極にコーティング層を形成するために消費される容量は、バッテリーセルの品質の重要な基準となる。このコーティング層は、試験用フルセルが初めて充電されたときに負電極上に形成される。このコーティング層の形成のためにリチウムイオンが不可逆的に消費されるため(コーティング層容量)、試験用フルセルでは、後続のサイクルで使用できるサイクル容量が少なくなる。コーティング層容量(%)は、負電極にコーティング層を形成するために使用された理論の%であり、以下の式に従って算出される。
試験用フルセルでの測定では、例えば放電容量をサイクル数から求める。この目的のために、試験用フルセルは、一定の充電電流強度で、一定の上限電位まで充電される。対応する上限電位は、充電電流が、一定の値まで低下するまで保持される。その後、一定の放電電位まで、一定の放電電流強度で放電を行う。この充電方法は、いわゆるI/U充電である。このプロセスは、所望のサイクル数に応じて繰り返される。
負電極の活物質として金属リチウムを用いて、実施例3による試験用フルセルの実験を行った。試験用フルセルには、実施例2で説明した電解質1を充填した。正電極は、リチウムニッケルマンガンコバルト酸化物を活物質として含有した。2回の充電/放電サイクルを行い、放電容量を測定した。2回の充電/放電サイクルは、第1試験用フルセルで直接行った。2回の充電/放電サイクルの前に、第2試験用フルセルを用いて初期化サイクルを行った。金属リチウムは、12mAで3分間堆積させ、さらに0.1mA/cm2で充電終了まで堆積させた。この後、放電を行った。その後、2回の充電/放電サイクルを開始した。3つ目の試験用フルセルを用いて、外圧の影響を調べた。この目的のために、テスト用フルセルのハウジングを外側から約50N/cm2の圧力で規定通りに押し付けた。次に、第2試験用フルセルで説明したように初期化サイクルを行い、その後、2回の充電および放電サイクルを行った。試験用フルセルは、0.1mA/cm2の電流で4.4ボルトの電位まで、8mAh/cm2の充電容量に達するまで充電された。その後、2.9ボルトの電位に達するまで0.1mA/cm2の電流で放電を行った。
実験1の第2試験用フルセルを数サイクル後に解体し、堆積した金属リチウムの形態を判別した。図9は、均一でコンパクトなリチウムの体積が確認できる、この負電極を示す。リチウムが点状に堆積することはなく、電極全体が均一に覆われていることがわかる。このようにリチウムが良好に堆積していることから、使用した電解質1におけるリチウムのサイクル安定性が良好であることがわかる。
さらに、より高い電流での充電および放電を調べるために、実験1と同様に2つの試験用フルセルを作製した。最初の試験用フルセルでは、0.5mA/cm2の充電および放電電流で2回の充電および放電サイクルが行われた。第2試験用フルセルでは、充電および放電電流は1.0mA/cm2であった。前記セルは、21回充電および放電された。充電/放電サイクルの前に、両方の試験用フルセルに対して初期化サイクルが実行された。試験用フルセルは、0.5 mA/cm2または1.0 mA/cm2の電流で4.4ボルトの電位まで、8 mAh/cm2の充電容量に達するまで充電された。その後、2.9ボルトの電位に達するまで0.5mA/cm2または1.0mA/cm2の電流で放電させた。
電解質1を用いた試験用フルセルと参照電解質を用いた試験用フルセルのサイクル効率を比較するために、まず、参照電解質を用いた試験用フルセルを作製した。試験用セルは、正電極の活物質としてリン酸鉄リチウムを、負電極の活物質として金属リチウムを含んでいた。この試験用セルは、組成LiAlCl4x6SO2の参照電解質を含んでいた。
リチウムの腐食、すなわち電解質中の損失を防ぐために、急速充電および放電レートは7.5mAh/cm2を選択した。この速度で試験用フルセルを3.6Vの電位まで充電し、2.5Vの電位まで放電させた。
導電率を測定するために、化合物1,3および4の濃度を変えて電解質1,3および4を調製した。電解質の導電率は、各化合物の濃度ごとに導電率測定法を用いて測定した。温度調整後、2電極センサーを溶液中に接触させ、0~50mS/cmの測定範囲で測定した。測定中、センサーがSO2を含む電解質溶液と反応する可能性があることがわかった。
Claims (29)
- 活性金属と、放電素子(26)を有する少なくとも1つの正電極(4,23,44)と、放電素子(27)を有する少なくとも1つの負電極(5,22,45)と、ハウジング(1,28)と、電解質とを備える再充電可能なバッテリーセル(2,20,40)であって、
前記負電極(5,22,45)が、少なくとも前記再充電可能なバッテリーセルの充電状態において活物質として金属リチウムを有しており、
前記電解質が、SO2をベースとし、式(I)を有する少なくとも1つの第1導電性塩を含む、再充電可能なバッテリーセル(2,20,40)。
-Mは、アルカリ金属、アルカリ土類金属、元素周期表第12族の金属およびアルミニウムにより形成される群から選択される金属であり、
-xは、1から3の整数であり、
-置換基R1,R2,R3およびR4は、C1~C10アルキル、C2~C10アルケニル、C2~C10アルキニル、C3~C10シクロアルキル、C6~C14アリールおよびC5~C14ヘテロアリールからなる群から、互いに独立して選択され;そして
-Zは、アルミニウムまたはホウ素である) - 前記金属リチウムが、前記再充電可能なバッテリーセルの充電時に前記負電極(5,22,45)の前記放電素子(27)上に堆積可能である、請求項1に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記金属リチウムが、前記再充電可能なバッテリーセルの充電状態において、前記負電極(5、22、45)の前記放電素子(27)上に位置している、請求項1または2に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記金属リチウムが、前記再充電可能なバッテリーセルの第1の充電が行われる前に、前記負電極(5、22、45)の放電素子(27)上に既に配置されている、請求項1~3の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記負電極(5、22、45)の前記放電素子(27)が、
-金属板または金属箔の形態において、平面的に、または
-多孔質金属構造の形態で三次元的に、特に発泡金属(18)の形態において
設計されている、請求項1~4の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - 前記負電極(5、22、45)の前記放電素子(27)が、
-特に炭素同素体グラファイトの形態における、炭素、
-リチウムと合金を形成する物質、
-炭素を含まないリチウムインターカレーション物質、特にチタン酸リチウム(例えば、Li4Ti5O12)、および
-変換物質、特に遷移金属酸化物
によって形成される群から選択されるリチウム貯蔵物質から、少なくとも部分的に形成される、請求項1~5の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - リチウムと活性な合金を形成する前記物質が、
-リチウム貯蔵金属および金属合金、好ましくはSi、Ge、Sn、SnCoxCyおよびSnSixによって形成される群から、または
-リチウム貯蔵金属および金属合金の酸化物、好ましくはSnOx、SiOx、ならびにSnおよびSiの酸化ガラスによって形成される群から
選択される、請求項6に記載の再充電可能なバッテリーセル(2,20,40)。 - 前記正電極(4,23,44)が活物質として少なくとも1つの化合物を含有し、前記化合物が、好ましくはLixM’yM”zOaの組成を有し、式中、
-M’は、Ti、V、Cr、Mn、Fe、Co、Ni、CuおよびZnにより形成される群から選択される少なくとも1つの金属であり、
-M”は、元素周期表の第2族、第3族、第4族、第5族、第6族、第7族、第8族、第9族、第10族、第11族、第12族、第13族、第14族、第15族および第16族の元素により形成される群から選択される少なくとも1つの元素であり、
-xおよびyは、互いに独立して、0より大きい数であり、
-zは、0以上の数であり、そして
-aは、0より大きい数である、請求項1~7の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - 前記化合物が、LixM’yM”zOaの組成を有し、式中、M’はマンガンであり、M”はコバルトであり、x、yおよびzが好ましくは1に等しく、aが好ましくは4に等しい、請求項8に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記化合物が、LixM’yM”zOaの組成を有し、M’がニッケルおよびマンガンを含み、M”がコバルトであり、LixNiy1Mny2CozOaの組成を有する、請求項8または9に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記化合物が、LixM’yM”1 z1M”2 z2O4の組成を有し、式中、M”2はリンであり、z2は値1を有する、請求項8に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記化合物が、LixM’yM”1 z1PO4の組成を有し、式中、M’は鉄であり、M”はマンガンであり、前記化合物は、好ましくはLi(Fe0.3Mn0.7)PO4の組成を有する、請求項11に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記第1導電性塩の置換基R1,R2,R3およびR4が、互いに独立して、
-好ましくはC2-C4アルキルからの、特に好ましくはアルキル基2-プロピル、メチルおよびエチルからの、C1-C6アルキル;
-好ましくはC2-C4アルケニルからの、特に好ましくはアルケニル基のエテニルおよびプロペニルからの、C2-C6アルケニル;
-好ましくはC2-C4アルキニルからの、C2-C6アルキニル;
-C3-C6シクロアルキル;
-フェニル;および
-C5-C7ヘテロアリール
により形成される群から選択される、請求項1~12の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - 前記第1導電性塩の置換基R1,R2,R3およびR4のうちの少なくとも1つが、少なくとも1つのフッ素原子および/または少なくとも1つの化学基によって置換されており、前記化学基が、C1~C4アルキル、C2~C4アルケニル、C2~C4アルキニル、フェニルおよびベンジルによって形成される群から選択される、請求項1~13の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記第1導電性塩の置換基R1,R2,R3およびR4のうち少なくとも1つが、CF3基またはOSO2CF3基である、請求項1~14の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質が、式(I)による第1導電性塩とは異なる少なくとも1つの第2導電性塩を含む、請求項1~16の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質の前記第2導電性塩が、アルミン酸塩、ハロゲン化物、シュウ酸塩、ホウ酸塩、リン酸塩、ヒ酸塩および没食子酸塩により形成される群から選択される、アルカリ金属化合物、特にリチウム化合物である、請求項17に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質の前記第2導電性塩が、テトラハロアルミン酸リチウム、特にテトラクロロアルミン酸リチウムである、請求項17または18に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質が、少なくとも1つの添加剤を含む、請求項1~19の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質の前記添加剤が、ビニレンカーボネートおよびその誘導体、ビニルエチレンカーボネートおよびその誘導体、メチルエチレンカーボネートおよびその誘導体、(ビスオキサラト)ホウ酸リチウム、ジフルオロ(オキサラト)ホウ酸リチウム、テトラフルオロ(オキサラト)リン酸リチウム、シュウ酸リチウム、2-ビニルピリジン、4-ビニルピリジン、環状のエキソメチレンカーボネート類、スルトン類、環状および非環状のスルホン酸塩類、非環状の亜硫酸塩類、環状および非環状のスルフィン酸塩類、有機エステル類、無機酸類、1バールで少なくとも36℃の沸点を有する非環状および環状のアルカン類、芳香族化合物類、ハロゲン化された環状および非環状スルホニルイミド類、ハロゲン化された環状および非環状リン酸エステル類、ハロゲン化された環状および非環状ホスフィン類、ハロゲン化された環状および非環状ホスファイト類、ハロゲン化された環状および非環状のホスファゼン類、ハロゲン化された環状および非環状のシリルアミン類、ハロゲン化された環状および非環状のハロゲン化エステル類、ハロゲン化された環状および非環状のアミド類、ハロゲン化された環状および非環状の無水物類、ならびにハロゲン化された有機複素環類により形成される群から選択される、請求項20に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質が、電解質組成物の総重量に基づいて、
(i)5~99.4重量%の二酸化硫黄、
(ii)0.6~95重量%の第1導電性塩、
(iii)0~25重量%の第2導電性塩、および
(iv)0~10重量%の添加剤
の組成を有する、請求項1~21の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - 前記第1導電性塩のモル濃度が、前記電解質の全体積を基準にして、0.01mol/L~10mol/L、好ましくは0.05mol/L~10mol/L、より好ましくは0.1mol/L~6mol/L、最も好ましくは0.2mol/L~3.5mol/Lの範囲内である、請求項1~22の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記電解質が、導電性塩1mol当たり、少なくとも0.1molのSO2、好ましくは少なくとも1molのSO2、より好ましくは少なくとも5molのSO2、より好ましくは少なくとも10molのSO2、最も好ましくは少なくとも20molのSO2を含む、請求項1~23の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記正電極(4,23,44)が、金属酸化物、金属ハロゲン化物および金属リン酸塩によって形成される群から選択される少なくとも1つの金属化合物を含み、ここで前記金属化合物の金属が、好ましくは、元素の周期表の原子番号22から28の遷移金属、特にコバルト、ニッケル、マンガンまたは鉄である、請求項1~24の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 前記正電極(4,23,44)が、スピネル、層状酸化物、変換化合物またはポリアニオン化合物の化学構造を有する少なくとも1つの金属化合物を含む、請求項1~25の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
- 正電極(4,23,44)が、
-金属板または金属箔の形態において、平面的に、または、
-多孔質金属構造の形で三次元的に、特に発泡金属(18)の形態において
好ましくは形成されている放電素子(34)を有する、請求項1~26の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - 正電極(4,23,44)および/または負電極(5)が、少なくとも1つのバインダー、好ましくはフッ素系バインダー、特にポリフッ化ビニリデン、ならびに/またはテトラフルオロエチレン、ヘキサフルオロプロピレンおよびフッ化ビニリデンから作製されるターポリマー、または
共役カルボン酸のモノマー構造単位、または前記共役カルボン酸のアルカリ塩、アルカリ土類塩、アンモニウム塩、またはこれらの組み合わせから構成されるポリマーからなるバインダー、または
モノマースチレンおよびブタジエン構造単位をベースとするポリマーからなるバインダー、またはカルボキシメチルセルロースの群からのバインダー、を含み、
ここで、前記バインダーが、総正電極重量に基づいて、好ましくは最大で20重量%、より好ましくは最大で15重量%、より好ましくは最大で10重量%、より好ましくは最大で7重量%、より好ましくは最大で5重量%、最も好ましくは最大で2重量%の濃度で存在する、請求項1~27の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。 - ハウジング(1,28)内に交互に積層された複数の負電極(5,22,45)および複数の正電極(4,23,44)を備え、前記正電極および前記負電極(5,22,45)が、好ましくは、セパレータ(11,13,21)によってそれぞれ互いに電気的に分離されている、請求項1~28の何れか1項に記載の再充電可能なバッテリーセル(2,20,40)。
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DE102021131511A1 (de) * | 2021-12-01 | 2023-06-01 | Bayerische Motoren Werke Aktiengesellschaft | Kathode mit einem fluorhaltigen Polymer sowie eine Festkörperbatterie mit der Kathode |
DE102021132742A1 (de) | 2021-12-10 | 2023-06-15 | Bayerische Motoren Werke Aktiengesellschaft | Batteriespeicher mit einer Sicherheitsvorrichtung sowie Verfahren zum Auslösen der Sicherheitsvorrichtung |
DE102021132739A1 (de) | 2021-12-10 | 2023-06-15 | Bayerische Motoren Werke Aktiengesellschaft | Batteriespeicher mit einer Sicherheitsvorrichtung und ein Verfahren zum Auslösen der Sicherheitsvorrichtung |
DE102021132747A1 (de) | 2021-12-10 | 2023-06-15 | Bayerische Motoren Werke Aktiengesellschaft | Batteriezelle sowie Batteriespeicher mit der Batteriezelle |
DE102021132746A1 (de) | 2021-12-10 | 2023-06-15 | Bayerische Motoren Werke Aktiengesellschaft | Batteriespeicher mit einer Sicherheitsvorrichtung sowie Verfahren zum Auslösen der Sicherheitsvorrichtung |
DE102021132740A1 (de) | 2021-12-10 | 2023-06-15 | Bayerische Motoren Werke Aktiengesellschaft | Batteriespeicher mit einer Filtervorrichtung |
DE102021132745A1 (de) | 2021-12-10 | 2023-06-15 | Bayerische Motoren Werke Aktiengesellschaft | Batteriespeicher mit einer Sicherheitsvorrichtung sowie Verfahren zum Auslösen der Sicherheitsvorrichtung |
EP4199149A1 (de) | 2021-12-17 | 2023-06-21 | Innolith Technology AG | Wiederaufladbare batteriezelle |
EP4199150A1 (de) * | 2021-12-17 | 2023-06-21 | Innolith Technology AG | Wiederaufladbare batteriezelle |
CN117096447A (zh) * | 2022-05-12 | 2023-11-21 | 珠海冠宇电池股份有限公司 | 一种电池 |
WO2024012973A1 (de) | 2022-07-13 | 2024-01-18 | Bayerische Motoren Werke Aktiengesellschaft | Flüssige elektrolytzusammensetzung mit einem salz, elektrochemische zelle mit der elektrolytzusammensetzung, salz sowie verwendung des salzes in der elektrochemischen zelle |
WO2024012974A1 (de) | 2022-07-13 | 2024-01-18 | Bayerische Motoren Werke Aktiengesellschaft | Flüssige elektrolytzusammensetzung mit einem salz, elektrochemische zelle mit der elektrolytzusammensetzung, salz sowie verwendung des salzes in der elektrochemischen zelle |
CN115367816B (zh) * | 2022-10-27 | 2023-02-03 | 宜宾锂宝新材料有限公司 | 一种镍锰酸锂正极材料、其制备方法及锂离子电池 |
CN116053591B (zh) * | 2023-03-30 | 2023-06-27 | 宁德新能源科技有限公司 | 一种二次电池的电解液、二次电池及电子装置 |
CN116404238A (zh) * | 2023-06-08 | 2023-07-07 | 广州天赐高新材料股份有限公司 | 一种含有含硫无机成分的电解液和包括该电解液的锂离子电池 |
CN117586294B (zh) * | 2024-01-18 | 2024-05-28 | 山东海化集团有限公司 | 一种四(六氟异丙氧基)硼酸钠的制备方法及其在钠电中的应用 |
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