JP6262320B2 - 金属ドープされた酸化ニッケル活性材料 - Google Patents
金属ドープされた酸化ニッケル活性材料 Download PDFInfo
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- JP6262320B2 JP6262320B2 JP2016238689A JP2016238689A JP6262320B2 JP 6262320 B2 JP6262320 B2 JP 6262320B2 JP 2016238689 A JP2016238689 A JP 2016238689A JP 2016238689 A JP2016238689 A JP 2016238689A JP 6262320 B2 JP6262320 B2 JP 6262320B2
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- metal
- nickel
- oxide
- doped
- battery
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- 239000002184 metal Substances 0.000 title claims description 85
- 229910052751 metal Inorganic materials 0.000 title claims description 84
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 title description 149
- 229910000480 nickel oxide Inorganic materials 0.000 title description 100
- 239000011149 active material Substances 0.000 title description 20
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 166
- 229910052744 lithium Inorganic materials 0.000 claims description 52
- 229910052782 aluminium Inorganic materials 0.000 claims description 39
- 229910052749 magnesium Inorganic materials 0.000 claims description 33
- 239000002019 doping agent Substances 0.000 claims description 28
- 230000003647 oxidation Effects 0.000 claims description 28
- 238000007254 oxidation reaction Methods 0.000 claims description 28
- 229910052759 nickel Inorganic materials 0.000 claims description 26
- 229910052783 alkali metal Inorganic materials 0.000 claims description 16
- 150000001340 alkali metals Chemical class 0.000 claims description 15
- 229910052791 calcium Inorganic materials 0.000 claims description 14
- 239000003792 electrolyte Substances 0.000 claims description 14
- 229910052748 manganese Inorganic materials 0.000 claims description 11
- 229910052796 boron Inorganic materials 0.000 claims description 9
- 229910052723 transition metal Inorganic materials 0.000 claims description 7
- 150000003624 transition metals Chemical class 0.000 claims description 7
- 150000002739 metals Chemical class 0.000 claims description 6
- 229910052710 silicon Inorganic materials 0.000 claims description 6
- 229910052727 yttrium Inorganic materials 0.000 claims description 6
- 229910052732 germanium Inorganic materials 0.000 claims description 5
- 229910052700 potassium Inorganic materials 0.000 claims description 5
- 229910052708 sodium Inorganic materials 0.000 claims description 4
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 3
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 3
- 229910052792 caesium Inorganic materials 0.000 claims description 3
- 229910052701 rubidium Inorganic materials 0.000 claims description 2
- 239000011777 magnesium Substances 0.000 description 69
- 239000002245 particle Substances 0.000 description 65
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 59
- 230000002950 deficient Effects 0.000 description 58
- 239000000203 mixture Substances 0.000 description 58
- 239000003513 alkali Substances 0.000 description 56
- 239000011701 zinc Substances 0.000 description 56
- 229910052725 zinc Inorganic materials 0.000 description 54
- 239000000843 powder Substances 0.000 description 42
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 38
- BAPRMBRFVUJBEI-UHFFFAOYSA-N [O].[O].[Ni] Chemical compound [O].[O].[Ni] BAPRMBRFVUJBEI-UHFFFAOYSA-N 0.000 description 38
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 33
- 239000010410 layer Substances 0.000 description 31
- 238000003860 storage Methods 0.000 description 29
- 150000002500 ions Chemical class 0.000 description 24
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 23
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 23
- 229910017052 cobalt Inorganic materials 0.000 description 22
- 239000010941 cobalt Substances 0.000 description 22
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 22
- -1 alkali metal cation Chemical class 0.000 description 21
- 229910002804 graphite Inorganic materials 0.000 description 21
- 230000014759 maintenance of location Effects 0.000 description 21
- 239000002243 precursor Substances 0.000 description 20
- 239000011575 calcium Substances 0.000 description 19
- 239000010439 graphite Substances 0.000 description 19
- 239000000463 material Substances 0.000 description 19
- 238000000034 method Methods 0.000 description 19
- 229940021013 electrolyte solution Drugs 0.000 description 17
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 16
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 16
- 230000000052 comparative effect Effects 0.000 description 16
- 239000008151 electrolyte solution Substances 0.000 description 16
- 239000007789 gas Substances 0.000 description 16
- 239000011572 manganese Substances 0.000 description 16
- 229910000483 nickel oxide hydroxide Inorganic materials 0.000 description 16
- 150000002641 lithium Chemical class 0.000 description 15
- 239000007787 solid Substances 0.000 description 15
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 13
- 229910052760 oxygen Inorganic materials 0.000 description 13
- 239000001301 oxygen Substances 0.000 description 13
- 229910013716 LiNi Inorganic materials 0.000 description 12
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- 239000006182 cathode active material Substances 0.000 description 12
- 230000008569 process Effects 0.000 description 12
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 11
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 11
- 239000002253 acid Substances 0.000 description 11
- 238000010306 acid treatment Methods 0.000 description 11
- 239000013078 crystal Substances 0.000 description 11
- 229910001882 dioxygen Inorganic materials 0.000 description 11
- 229910001416 lithium ion Inorganic materials 0.000 description 11
- 229910052755 nonmetal Inorganic materials 0.000 description 11
- 238000000634 powder X-ray diffraction Methods 0.000 description 11
- 229910001297 Zn alloy Inorganic materials 0.000 description 9
- ZQQGQJKVMMDIKF-UHFFFAOYSA-N [Ni+4] Chemical compound [Ni+4] ZQQGQJKVMMDIKF-UHFFFAOYSA-N 0.000 description 9
- 238000009826 distribution Methods 0.000 description 9
- 229910021645 metal ion Inorganic materials 0.000 description 9
- 239000000243 solution Substances 0.000 description 9
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 8
- 229910001413 alkali metal ion Inorganic materials 0.000 description 8
- 239000011148 porous material Substances 0.000 description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 8
- 238000004458 analytical method Methods 0.000 description 7
- 229920000642 polymer Polymers 0.000 description 7
- OSOVKCSKTAIGGF-UHFFFAOYSA-N [Ni].OOO Chemical compound [Ni].OOO OSOVKCSKTAIGGF-UHFFFAOYSA-N 0.000 description 6
- 238000009792 diffusion process Methods 0.000 description 6
- 239000012528 membrane Substances 0.000 description 6
- 229920000298 Cellophane Polymers 0.000 description 5
- VEQPNABPJHWNSG-UHFFFAOYSA-N Nickel(2+) Chemical group [Ni+2] VEQPNABPJHWNSG-UHFFFAOYSA-N 0.000 description 5
- 239000011230 binding agent Substances 0.000 description 5
- 238000000576 coating method Methods 0.000 description 5
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- 239000011229 interlayer Substances 0.000 description 5
- 238000005259 measurement Methods 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 229910001453 nickel ion Inorganic materials 0.000 description 5
- 230000036961 partial effect Effects 0.000 description 5
- 239000000047 product Substances 0.000 description 5
- 230000002829 reductive effect Effects 0.000 description 5
- 238000001179 sorption measurement Methods 0.000 description 5
- 239000006228 supernatant Substances 0.000 description 5
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 4
- 229920002125 Sokalan® Polymers 0.000 description 4
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 150000008044 alkali metal hydroxides Chemical class 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 4
- 239000006229 carbon black Substances 0.000 description 4
- 239000002134 carbon nanofiber Substances 0.000 description 4
- 239000003575 carbonaceous material Substances 0.000 description 4
- 239000011248 coating agent Substances 0.000 description 4
- 239000008367 deionised water Substances 0.000 description 4
- 229910021641 deionized water Inorganic materials 0.000 description 4
- 238000007323 disproportionation reaction Methods 0.000 description 4
- PQVSTLUFSYVLTO-UHFFFAOYSA-N ethyl n-ethoxycarbonylcarbamate Chemical compound CCOC(=O)NC(=O)OCC PQVSTLUFSYVLTO-UHFFFAOYSA-N 0.000 description 4
- 238000002309 gasification Methods 0.000 description 4
- 238000010438 heat treatment Methods 0.000 description 4
- 238000009616 inductively coupled plasma Methods 0.000 description 4
- 239000003112 inhibitor Substances 0.000 description 4
- 239000010954 inorganic particle Substances 0.000 description 4
- GLXDVVHUTZTUQK-UHFFFAOYSA-M lithium hydroxide monohydrate Substances [Li+].O.[OH-] GLXDVVHUTZTUQK-UHFFFAOYSA-M 0.000 description 4
- 229940040692 lithium hydroxide monohydrate Drugs 0.000 description 4
- 239000000395 magnesium oxide Substances 0.000 description 4
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 4
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 230000001590 oxidative effect Effects 0.000 description 4
- 239000004584 polyacrylic acid Substances 0.000 description 4
- 150000003839 salts Chemical class 0.000 description 4
- 239000011734 sodium Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 238000006467 substitution reaction Methods 0.000 description 4
- 239000011787 zinc oxide Substances 0.000 description 4
- 229910017018 Ni0.8Co0.15Al0.05 Inorganic materials 0.000 description 3
- 239000004743 Polypropylene Substances 0.000 description 3
- 229910052797 bismuth Inorganic materials 0.000 description 3
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 3
- 229910000428 cobalt oxide Inorganic materials 0.000 description 3
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 229910052738 indium Inorganic materials 0.000 description 3
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 3
- 230000007935 neutral effect Effects 0.000 description 3
- 229920001155 polypropylene Polymers 0.000 description 3
- 238000012545 processing Methods 0.000 description 3
- 238000006722 reduction reaction Methods 0.000 description 3
- 238000001878 scanning electron micrograph Methods 0.000 description 3
- 239000002002 slurry Substances 0.000 description 3
- 238000004611 spectroscopical analysis Methods 0.000 description 3
- 238000003786 synthesis reaction Methods 0.000 description 3
- 229910052718 tin Inorganic materials 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 2
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 2
- 229920002134 Carboxymethyl cellulose Chemical class 0.000 description 2
- 229910020599 Co 3 O 4 Inorganic materials 0.000 description 2
- 238000005169 Debye-Scherrer Methods 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- JLVVSXFLKOJNIY-UHFFFAOYSA-N Magnesium ion Chemical compound [Mg+2] JLVVSXFLKOJNIY-UHFFFAOYSA-N 0.000 description 2
- 239000004677 Nylon Substances 0.000 description 2
- 239000004698 Polyethylene Substances 0.000 description 2
- 239000004372 Polyvinyl alcohol Substances 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- 229920002472 Starch Polymers 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 2
- UBSCDTMJJXALAR-UHFFFAOYSA-N [Zn].O(O)O.[Ni] Chemical compound [Zn].O(O)O.[Ni] UBSCDTMJJXALAR-UHFFFAOYSA-N 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 230000000274 adsorptive effect Effects 0.000 description 2
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- 229910001420 alkaline earth metal ion Inorganic materials 0.000 description 2
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- 239000007864 aqueous solution Substances 0.000 description 2
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- 239000001768 carboxy methyl cellulose Chemical class 0.000 description 2
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 2
- 239000008112 carboxymethyl-cellulose Chemical class 0.000 description 2
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- 238000012512 characterization method Methods 0.000 description 2
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- 229910001429 cobalt ion Inorganic materials 0.000 description 2
- XLJKHNWPARRRJB-UHFFFAOYSA-N cobalt(2+) Chemical group [Co+2] XLJKHNWPARRRJB-UHFFFAOYSA-N 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
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- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 description 2
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- 238000000227 grinding Methods 0.000 description 2
- 238000010316 high energy milling Methods 0.000 description 2
- AMWRITDGCCNYAT-UHFFFAOYSA-L hydroxy(oxo)manganese;manganese Chemical compound [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 238000002354 inductively-coupled plasma atomic emission spectroscopy Methods 0.000 description 2
- 229910052500 inorganic mineral Inorganic materials 0.000 description 2
- 238000005342 ion exchange Methods 0.000 description 2
- 239000002563 ionic surfactant Substances 0.000 description 2
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 2
- 229910001425 magnesium ion Inorganic materials 0.000 description 2
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- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Chemical compound [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 description 2
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- WLAMNBDJUVNPJU-UHFFFAOYSA-N 2-methylbutyric acid Chemical compound CCC(C)C(O)=O WLAMNBDJUVNPJU-UHFFFAOYSA-N 0.000 description 1
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- 206010065042 Immune reconstitution inflammatory syndrome Diseases 0.000 description 1
- 229910002995 LiNi0.8Co0.15Al0.05O2 Inorganic materials 0.000 description 1
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- 238000013461 design Methods 0.000 description 1
- JKWMSGQKBLHBQQ-UHFFFAOYSA-N diboron trioxide Chemical compound O=BOB=O JKWMSGQKBLHBQQ-UHFFFAOYSA-N 0.000 description 1
- 239000011262 electrochemically active material Substances 0.000 description 1
- 238000004993 emission spectroscopy Methods 0.000 description 1
- 230000034964 establishment of cell polarity Effects 0.000 description 1
- 238000004880 explosion Methods 0.000 description 1
- IMBKASBLAKCLEM-UHFFFAOYSA-L ferrous ammonium sulfate (anhydrous) Chemical compound [NH4+].[NH4+].[Fe+2].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O IMBKASBLAKCLEM-UHFFFAOYSA-L 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- NBVXSUQYWXRMNV-UHFFFAOYSA-N fluoromethane Chemical compound FC NBVXSUQYWXRMNV-UHFFFAOYSA-N 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 239000013505 freshwater Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 229940119177 germanium dioxide Drugs 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 230000005484 gravity Effects 0.000 description 1
- 239000011874 heated mixture Substances 0.000 description 1
- 229920006158 high molecular weight polymer Polymers 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- RXPAJWPEYBDXOG-UHFFFAOYSA-N hydron;methyl 4-methoxypyridine-2-carboxylate;chloride Chemical compound Cl.COC(=O)C1=CC(OC)=CC=N1 RXPAJWPEYBDXOG-UHFFFAOYSA-N 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 150000002471 indium Chemical class 0.000 description 1
- 229910003437 indium oxide Inorganic materials 0.000 description 1
- 229910000337 indium(III) sulfate Inorganic materials 0.000 description 1
- PSCMQHVBLHHWTO-UHFFFAOYSA-K indium(iii) chloride Chemical compound Cl[In](Cl)Cl PSCMQHVBLHHWTO-UHFFFAOYSA-K 0.000 description 1
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 1
- XGCKLPDYTQRDTR-UHFFFAOYSA-H indium(iii) sulfate Chemical compound [In+3].[In+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O XGCKLPDYTQRDTR-UHFFFAOYSA-H 0.000 description 1
- 150000002484 inorganic compounds Chemical class 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 238000009830 intercalation Methods 0.000 description 1
- 230000002687 intercalation Effects 0.000 description 1
- 230000000670 limiting effect Effects 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- XMWCXZJXESXBBY-UHFFFAOYSA-L manganese(ii) carbonate Chemical compound [Mn+2].[O-]C([O-])=O XMWCXZJXESXBBY-UHFFFAOYSA-L 0.000 description 1
- 229910001092 metal group alloy Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 150000001455 metallic ions Chemical class 0.000 description 1
- 238000005272 metallurgy Methods 0.000 description 1
- 239000012982 microporous membrane Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
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- 239000002105 nanoparticle Substances 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- BFDHFSHZJLFAMC-UHFFFAOYSA-L nickel(ii) hydroxide Chemical compound [OH-].[OH-].[Ni+2] BFDHFSHZJLFAMC-UHFFFAOYSA-L 0.000 description 1
- OFKLXPIYUOJPPI-UHFFFAOYSA-N nickel;oxosilver Chemical compound [Ni].[Ag]=O OFKLXPIYUOJPPI-UHFFFAOYSA-N 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000012811 non-conductive material Substances 0.000 description 1
- 239000002736 nonionic surfactant Substances 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- 125000000843 phenylene group Chemical group C1(=C(C=CC=C1)*)* 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 239000006069 physical mixture Substances 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 229920002852 poly(2,6-dimethyl-1,4-phenylene oxide) polymer Polymers 0.000 description 1
- 229920002401 polyacrylamide Polymers 0.000 description 1
- 229920000058 polyacrylate Chemical class 0.000 description 1
- 125000003367 polycyclic group Chemical group 0.000 description 1
- 229920005596 polymer binder Polymers 0.000 description 1
- 239000002491 polymer binding agent Substances 0.000 description 1
- 239000005518 polymer electrolyte Substances 0.000 description 1
- 229920000307 polymer substrate Polymers 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 239000012286 potassium permanganate Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000011085 pressure filtration Methods 0.000 description 1
- 238000001812 pycnometry Methods 0.000 description 1
- 238000004445 quantitative analysis Methods 0.000 description 1
- 239000002964 rayon Substances 0.000 description 1
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- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 238000004626 scanning electron microscopy Methods 0.000 description 1
- 239000011163 secondary particle Substances 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 239000011863 silicon-based powder Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910001923 silver oxide Inorganic materials 0.000 description 1
- 229910000108 silver(I,III) oxide Inorganic materials 0.000 description 1
- 239000002109 single walled nanotube Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000007784 solid electrolyte Substances 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 238000003746 solid phase reaction Methods 0.000 description 1
- 239000012265 solid product Substances 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 238000010671 solid-state reaction Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- 239000012798 spherical particle Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 125000000542 sulfonic acid group Chemical group 0.000 description 1
- 230000003746 surface roughness Effects 0.000 description 1
- 239000004094 surface-active agent Substances 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical compound [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 238000004448 titration Methods 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 229910001428 transition metal ion Inorganic materials 0.000 description 1
- 238000003828 vacuum filtration Methods 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- GFDKELMFCRQUSG-UHFFFAOYSA-N yttrium;trihydrate Chemical compound O.O.O.[Y] GFDKELMFCRQUSG-UHFFFAOYSA-N 0.000 description 1
- 229910006279 γ-NiOOH Inorganic materials 0.000 description 1
Images
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- C01G51/40—Cobaltates
- C01G51/42—Cobaltates containing alkali metals, e.g. LiCoO2
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- C01G51/44—Cobaltates containing alkali metals, e.g. LiCoO2 containing manganese
- C01G51/50—Cobaltates containing alkali metals, e.g. LiCoO2 containing manganese of the type [MnO2]n-, e.g. Li(CoxMn1-x)O2, Li(MyCoxMn1-x-y)O2
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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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- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
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- H—ELECTRICITY
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Description
W.B.Meldrun(Quantitative Analysis,Boston:Heath,1955,408〜9)に説明される硫酸アンモニウム第一鉄及び標準化された過マンガン酸カリウム溶液を用いて化学的滴定法により決定され得る。遷移金属の平均酸化状態はまた、金属ドープされたリチウム欠損酸化ニッケルをカソード活性材料として含み、Li金属をアノード活性材料として含み、また非水電解質溶液を含むコインセルに関して観察される比の重力測定的容量から、間接的に決定され得る。
1200e)により測定され得る。真密度は、例えば、British Standards Instituteによって、開放孔及び閉鎖孔を除く、その体積で除した粒子の質量として定義される。
LixNi(IV)1−xNi(III)xO2+H2O→Ni(II)(OH)2+x Li++1/2 O2 (1)
2LiNi+3O2+4H+→Ni+4O2+Ni+2+2Li++2H2O (2)
LiNi+3O2+H2O→HxLi(1−x)Ni+3O2+xLiOH (3)
観察されるパターンは、様々な組成物を有する他の科学的に脱リチウム化された積層酸化ニッケルに関して、例えば、H.Arai et al.(例えば、J.Solid State Chem.,2002,163,340〜9)及びまたL.Croguennec et al.(例えば、J.Mater.Chem.,2001,11,131〜41)により以前に報告されたものと一致し得る。実験的パターンは、脱リチウム化された酸化ニッケルの比較試料に関してT.Ohzuku et al.(例えば、J.Electrochem.Soc.,1993,140,1862)によって報告されたものと一致し得る。
アノードは、例えば、重量で約0.05重量%〜2重量%の間、又は約0.1重量%〜1重量%の間のゲル化剤を含み得る。
化学量論的ニッケル酸リチウムLiNiO2を、93.91gの商用の球状β−オキシ水酸化ニッケル粉末(例えば、β−NiOOH、Kansai Catalyst Co.)及び42.97gの一水化水酸化リチウム(LiOH・H2O,Aldrich Chemical)を配合し、混合物を酸素ガス流下で、チューブ炉内において約210℃で約20時間、加熱することによって合成した。加熱した混合物を、周囲室温まで炉冷させ、すり鉢とすりこぎとで挽き、酸素ガス流下で更に48時間800℃にて再加熱した。
最終反応生成物のX線粉末回析パターンは、例えば、米国特許第5,720,932号、J.Maruta et al.(Journal of Power Sources,2000,90,89〜94)、及びY.Sun et al.(Solid State Ionics,2006,177,1173〜7)に説明されるような、化学量論的LiNiO2(例えば、ICDD PDF No.09−0063)に関して報告されたものに厳密に対応した。
実施例1のニッケル酸リチウムを、本明細書にその全体が援用される米国出願番号第12/722,669号の実施例1に開示されるプロセスと同様の低温酸処理プロセスによって、脱リチウム化した。具体的には、およそ100gのLiNiO2を、1.5Lの急速に撹拌した水性の6M H2SO4溶液に添加し、0〜5℃の間まで冷却した。得られたスラリーを、攪拌し、約2℃で約20時間(実施例2a)か又は40時間(実施例2b)かのいずれかで維持する。次に、懸濁した固体を沈殿させ、上澄み液をデカンテーションによって除去し、上澄みのpHがほぼ中性(即ち、pH約6〜7)になるまで、固体を脱イオン水のアリコートで洗浄した。固体を、加圧濾過かまたは真空濾過かのいずれかによって収集し、約80℃で約24時間、空気乾燥した。乾燥させた脱リチウム化されたLixNiO2生成物の残留リチウム含量は、ICP分光法によって、x=0.31に相当する2.2重量% Li未満(実施例2a)、及びx=0.06に相当する0.4重量%
Li超(実施例2b)と決定された。脱リチウム化された生成物のX線粉末回析パターンは、より高い2θ角度への回析ピーク位置の予想された移動を伴う、化学量論的LiNiO2のパターンに類似した。脱リチウム化されたLixNiO2粉末の平均粒径は、約1〜8μmの範囲であり、B.E.T.比表面積は、約1.36m2/gであった。LixNiO2粉末の真密度は、Heピクノメータによって4.70g/cm3と測定された。
追加のKOH電解質溶液をセパレータに添加して、電解質溶液が完全にセパレータを貫通し、下のカソードを湿潤することを確実にした。ポリマー絶縁シールを、アノード缶の縁部に定置した。亜鉛合金粒子を含有する約2.6gのアノードスラリー、電解質溶液、及びゲル化剤を、アノード缶に添加した。次に、ポリマーシールを有するアノード缶をカソード缶の上部に位置付け、2つの缶を合わせて機械的に圧着して、セルを密封した。
図2の三成分組成図に示される金属ドープされたLi(Ni1−y−zCoyAlz)O2及びLi(Ni1−y−zCoyMgz)O2系を、合成し、脱リチウム化し、対応する脱リチウム化された(即ち、リチウム欠損)金属ドープされた酸化ニッケル活性材料の性能に関して、酸素ガス発生、初期開路電圧(OCV)、出来立て時(即ち、24時間)放電容量、並びに周囲温度及び高温で保管した後の容量保持率について評価した。
対照的に、20時間の酸処理後の残留Liレベルの量は、概して40時間に対するものの3倍超であった(例えば、>2重量%)。
実施例3a〜nの金属ドープされたニッケル酸リチウムLiNi1−y−zCoyMa zO2(M=Mg、Al)のそれぞれ10.0g部分を、別々の6M H2SO4溶液の150mLアリコート中で同時に攪拌し、約0℃(例えば、2〜5℃)で20時間、別の部分をそれぞれ40時間保った。脱リチウム化された固体を、濾過によって収集し、洗浄液が公称の中性pHを有するまで脱イオン水で洗浄し、80℃で空気乾燥させた。実施例4a〜nの脱リチウム化された粉末は、次の公称のNi:Co:M金属原子比を有する:実施例4a 0.96:0.04:0;4b 0.92:0.08:0;4c 0.88:0.12:0;4d−1(M=Mg)、4d−2(M=Al)0.98:0:0.2;4e−1(M=Mg)、4e−2(M=Al)0.96:0:0.04;4f−1(M=Mg)、4f−2(M=Al)0.92:0:0.08;4g−1(M=Mg)、4g−2(M=Al)0.96:0.02:0.02;4h−1(M=Mg)、4h−2(M=Al)0.92:0.06:0.02;4i−1(M=Mg)、4i−2(M=Al)0.92:0.04:0.04;4j−1(M=Mg)、4j−2(M=Al)0.92:0.02:0.06;4k−1(M=Mg)、4k−2(M=Al)0.88:0.10:0.02;4l−1(M=Mg)、4l−2(M=Al)0.88:0.08:0.04;4m−1(M=Mg)、4m−2(M=Al)0.88:0.06:0.06;4n−1(M=Mg)、4n−2(M=Al)0.88:0.04:0.08。乾燥させた固体のX線粉末回析パターンを、Cu Kα線を用いて測定した。実施例4a〜nの選択された脱リチウム化された粉末の試料の熱安定性を、DSCによって決定した。残留リチウムの量を、実施例4a〜n選択された脱リチウム化された粉末の試料に関してICP−EAによって決定し、表1に示す。
球状オキシ水酸化コバルトでコーティングされたβ−オキシ水酸化ニッケル粉末の試料を、例えば、米国特許第8,043,748号に開示されるような一般的な方法によって開示される通り、商用の球状β−水酸化ニッケル(例えば、Kansai Catalyst Co.,Ltd.,Osaka、日本)から調製した。
公称組成LiNi0.8Co0.15Al0.05O2及びLi(Ni0.8Co0.15Al0.05)0.99B0.01O2(即ち、LiNi0.792Co0.149Al0.049B0.01O2)を有する商用のリチウムニッケルコバルトアルミニウム酸化物粉末(Toda America Inc.,Battle Creek,MI)の試料を、上述の実施例2の酸処理プロセスによって脱リチウム化して、それぞれ比較例2a及び2bの脱リチウム化された金属置換された酸化Ni(IV)を形成した。ボタンセルを、実施例2の一般的な方法によって製造した。比較例2のセルを、製造後24時間以内に試験した。OCV値は、約1.83〜1.85Vの範囲であった。セルを、0.8Vカットオフ電圧に対して公称C/30速度に対応する約10mA/gの一定電流にて低速で放電した。図10に、比較例2aの脱リチウム化された、コバルト及びアルミニウム置換された酸化ニッケル、及び比較例2bのコバルト、アルミニウム、及びホウ素ドープされた酸化ニッケルを含有するセルに関する放電曲線を、実施例2bの脱リチウム化されたLixNiO2を含有するセル、及び商用の電池グレードEMDに関するものと比較する。比較例2a及び2bの脱リチウム化されたコバルト/アルミニウム/ホウ素ドープされた酸化ニッケルを含有するセルに関する平均放電容量は、それぞれ325mAh/g及び335mAh/gであった。
公称化学組成物LiNi0.9Co0.2O2及びLiNi0.8Co0.1O2を有する商用のリチウムニッケルコバルト酸化物粉末(例えば、NEI Corp.,Somerset,NJ)の試料を、上述の実施例2の酸処理プロセスによって脱リチウム化して、それぞれ比較例3a及び3bの脱リチウム化された金属ドープされた酸化ニッケル(IV)を形成した。ボタンセルを、実施例2の一般的な方法によって製造した。比較例3のセルを、製造後24時間以内に試験した。OCV値は、典型的に約1.81Vであった。セルを、0.8Vカットオフ電圧に対して公称C/30速度に対応する約10mA/gの一定電流にて低速で放電した。比較例3a及び3bの脱リチウム化されたコバルトドープされた酸化ニッケルを含有するセルに関する平均放電容量は、それぞれ355mAh/g及び335mAh/gであった。
Claims (12)
- 電池であって、
式AxNi1−y−z−wCoyMa zMb wO2を有する酸化物を含むカソードと、 アノードと、
前記カソードと前記アノードとの間のセパレータと、
水性アルカリ電解質と、を含み、
式中、
Aが、アルカリ金属であり、
Maが、遷移金属、アルカリ土類金属、主族金属、およびそれらの組み合わせからなる群から選択される金属ドーパントであり、
Mbが、B、Si、Ge、又はそれらの組み合わせからなる群から選択される非金属ドーパントであり、
0≦x≦0.08であり、
0≦w≦0.02であり、かつ
0.02≦y+z≦0.25である、電池。 - 0.02≦y≦0.15、請求項1に記載の電池。
- yが、0である、請求項1に記載の電池。
- 0.02≦z≦0.08である、請求項1に記載の電池。
- zが、0である、請求項1に記載の電池。
- wが、0である、請求項1に記載の電池。
- 前記アルカリ金属が、Li、Na、K、Cs、Rb、及び任意のそれらの組み合わせからなる群から選択される、請求項1に記載の電池。
- Maが、Ca、Mg、Al、Y、Mn、及び任意のそれらの組み合わせからなる群から選択される、請求項1に記載の電池。
- 前記酸化物が、陽子を更に含む、請求項1に記載の電池。
- 前記酸化物が、ニッケル及び金属ドーパントの合計に対して0.02〜0.2の間の化学量論的比にて陽子を更に含む、請求項1に記載の電池。
- 前記酸化物が、LixNi1−yCoyO2、LixNi1−zCazO2、LixNi1−y−zCoyCazO2、LixNi1−zMgzO2、LixNi1−y−zCoyMgzO2、LixNi1−zAlzO2、及びLixNi1−y−zCoyAlzO2、LixNi1−z(Mg,Al)zO2、LixNi1−y−zCoy(Mg,Al)zO2、LixNi1−zYzO2、LixNi1−y−zCoyYzO2、LixNi1−zMnzO2、及びLixNi1−y−zCoyMnzO2からなる群から選択される、請求項1に記載の電池。
- Niが、+3.25を超える平均酸化状態を有する、請求項1に記載の電池。
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