JP2023507023A - 正極材料、その製造方法及びリチウムイオン電池 - Google Patents
正極材料、その製造方法及びリチウムイオン電池 Download PDFInfo
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- 239000010406 cathode material Substances 0.000 title claims abstract description 30
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 25
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 14
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 11
- 238000005245 sintering Methods 0.000 claims abstract description 80
- 239000007774 positive electrode material Substances 0.000 claims abstract description 70
- 239000000463 material Substances 0.000 claims abstract description 63
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 42
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 41
- 239000013078 crystal Substances 0.000 claims abstract description 41
- 239000011572 manganese Substances 0.000 claims abstract description 40
- 239000011248 coating agent Substances 0.000 claims abstract description 37
- 239000002245 particle Substances 0.000 claims abstract description 34
- 238000000576 coating method Methods 0.000 claims abstract description 27
- 238000000034 method Methods 0.000 claims abstract description 27
- 239000002243 precursor Substances 0.000 claims abstract description 26
- 230000008569 process Effects 0.000 claims abstract description 23
- 229910052748 manganese Inorganic materials 0.000 claims abstract description 22
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims abstract description 18
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical group [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 51
- 229910052759 nickel Inorganic materials 0.000 claims description 19
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 claims description 13
- SOXUFMZTHZXOGC-UHFFFAOYSA-N [Li].[Mn].[Co].[Ni] Chemical compound [Li].[Mn].[Co].[Ni] SOXUFMZTHZXOGC-UHFFFAOYSA-N 0.000 claims description 10
- 239000011247 coating layer Substances 0.000 claims description 10
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 claims description 9
- 229910018661 Ni(OH) Inorganic materials 0.000 claims description 8
- 229910052782 aluminium Inorganic materials 0.000 claims description 8
- 229910052796 boron Inorganic materials 0.000 claims description 6
- IIPYXGDZVMZOAP-UHFFFAOYSA-N lithium nitrate Chemical compound [Li+].[O-][N+]([O-])=O IIPYXGDZVMZOAP-UHFFFAOYSA-N 0.000 claims description 6
- 229910052749 magnesium Inorganic materials 0.000 claims description 6
- 229910052758 niobium Inorganic materials 0.000 claims description 6
- 229910052698 phosphorus Inorganic materials 0.000 claims description 6
- 229910052712 strontium Inorganic materials 0.000 claims description 6
- 229910052719 titanium Inorganic materials 0.000 claims description 6
- 229910052721 tungsten Inorganic materials 0.000 claims description 6
- 229910052727 yttrium Inorganic materials 0.000 claims description 6
- 229910052726 zirconium Inorganic materials 0.000 claims description 6
- 150000001875 compounds Chemical class 0.000 claims description 5
- YNQRWVCLAIUHHI-UHFFFAOYSA-L dilithium;oxalate Chemical compound [Li+].[Li+].[O-]C(=O)C([O-])=O YNQRWVCLAIUHHI-UHFFFAOYSA-L 0.000 claims description 3
- XIXADJRWDQXREU-UHFFFAOYSA-M lithium acetate Chemical compound [Li+].CC([O-])=O XIXADJRWDQXREU-UHFFFAOYSA-M 0.000 claims description 3
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 claims description 3
- 229910052808 lithium carbonate Inorganic materials 0.000 claims description 3
- FUJCRWPEOMXPAD-UHFFFAOYSA-N lithium oxide Chemical compound [Li+].[Li+].[O-2] FUJCRWPEOMXPAD-UHFFFAOYSA-N 0.000 claims description 3
- 229910001947 lithium oxide Inorganic materials 0.000 claims description 3
- 239000000126 substance Substances 0.000 claims description 3
- 229910021585 Nickel(II) bromide Inorganic materials 0.000 claims description 2
- 229910021586 Nickel(II) chloride Inorganic materials 0.000 claims description 2
- 229910021587 Nickel(II) fluoride Inorganic materials 0.000 claims description 2
- 229910021588 Nickel(II) iodide Inorganic materials 0.000 claims description 2
- 239000002131 composite material Substances 0.000 claims description 2
- QMMRZOWCJAIUJA-UHFFFAOYSA-L nickel dichloride Chemical compound Cl[Ni]Cl QMMRZOWCJAIUJA-UHFFFAOYSA-L 0.000 claims description 2
- LGQLOGILCSXPEA-UHFFFAOYSA-L nickel sulfate Chemical compound [Ni+2].[O-]S([O-])(=O)=O LGQLOGILCSXPEA-UHFFFAOYSA-L 0.000 claims description 2
- IPLJNQFXJUCRNH-UHFFFAOYSA-L nickel(2+);dibromide Chemical compound [Ni+2].[Br-].[Br-] IPLJNQFXJUCRNH-UHFFFAOYSA-L 0.000 claims description 2
- 229910000008 nickel(II) carbonate Inorganic materials 0.000 claims description 2
- 229910000363 nickel(II) sulfate Inorganic materials 0.000 claims description 2
- GNMQOUGYKPVJRR-UHFFFAOYSA-N nickel(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Ni+3].[Ni+3] GNMQOUGYKPVJRR-UHFFFAOYSA-N 0.000 claims description 2
- DBJLJFTWODWSOF-UHFFFAOYSA-L nickel(ii) fluoride Chemical compound F[Ni]F DBJLJFTWODWSOF-UHFFFAOYSA-L 0.000 claims description 2
- BFSQJYRFLQUZKX-UHFFFAOYSA-L nickel(ii) iodide Chemical compound I[Ni]I BFSQJYRFLQUZKX-UHFFFAOYSA-L 0.000 claims description 2
- PZFKDUMHDHEBLD-UHFFFAOYSA-N oxo(oxonickeliooxy)nickel Chemical compound O=[Ni]O[Ni]=O PZFKDUMHDHEBLD-UHFFFAOYSA-N 0.000 claims description 2
- 101100513612 Microdochium nivale MnCO gene Proteins 0.000 claims 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 8
- 238000005265 energy consumption Methods 0.000 abstract description 7
- 238000005406 washing Methods 0.000 abstract description 7
- 230000015572 biosynthetic process Effects 0.000 abstract description 6
- 238000003786 synthesis reaction Methods 0.000 abstract description 6
- 230000014759 maintenance of location Effects 0.000 abstract description 5
- 239000003792 electrolyte Substances 0.000 abstract description 4
- 239000011164 primary particle Substances 0.000 abstract description 3
- 238000007086 side reaction Methods 0.000 abstract description 3
- 239000003513 alkali Substances 0.000 description 12
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 9
- 229910001882 dioxygen Inorganic materials 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 7
- 238000001816 cooling Methods 0.000 description 6
- 238000002156 mixing Methods 0.000 description 6
- 238000007873 sieving Methods 0.000 description 6
- 238000010298 pulverizing process Methods 0.000 description 5
- 238000004220 aggregation Methods 0.000 description 4
- 230000002776 aggregation Effects 0.000 description 4
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 3
- 230000001351 cycling effect Effects 0.000 description 3
- 230000006872 improvement Effects 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 238000007796 conventional method Methods 0.000 description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 2
- 238000007580 dry-mixing Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 239000011656 manganese carbonate Substances 0.000 description 2
- 235000006748 manganese carbonate Nutrition 0.000 description 2
- 229910000471 manganese heptoxide Inorganic materials 0.000 description 2
- AMWRITDGCCNYAT-UHFFFAOYSA-L manganese oxide Inorganic materials [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 2
- 229910000016 manganese(II) carbonate Inorganic materials 0.000 description 2
- VASIZKWUTCETSD-UHFFFAOYSA-N manganese(II) oxide Inorganic materials [Mn]=O VASIZKWUTCETSD-UHFFFAOYSA-N 0.000 description 2
- GEYXPJBPASPPLI-UHFFFAOYSA-N manganese(III) oxide Inorganic materials O=[Mn]O[Mn]=O GEYXPJBPASPPLI-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- 241000080590 Niso Species 0.000 description 1
- 240000007594 Oryza sativa Species 0.000 description 1
- 235000007164 Oryza sativa Nutrition 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 230000004931 aggregating effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 239000006257 cathode slurry Substances 0.000 description 1
- 235000013339 cereals Nutrition 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000008151 electrolyte solution Substances 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- -1 lithium hexafluorophosphate Chemical compound 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- CVMIVKAWUQZOBP-UHFFFAOYSA-L manganic acid Chemical group O[Mn](O)(=O)=O CVMIVKAWUQZOBP-UHFFFAOYSA-L 0.000 description 1
- 239000012046 mixed solvent Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 235000009566 rice Nutrition 0.000 description 1
- 238000005096 rolling process Methods 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000012798 spherical particle Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 238000003911 water pollution Methods 0.000 description 1
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Abstract
Description
ニッケル・コバルト・マンガン・リチウム複合酸化物と、ニッケルコバルトマンガンアルミン酸リチウム上に被覆される被覆層とを含み、被覆層はニッケル源材料及び/又はマンガン源材料を焼結して形成したマンガン酸リチウム及び/又はニッケル酸リチウムであり、又は正極材料は、本出願による上記製造方法で製造される。
(1)前駆体Ni0.92Co0.05Mn0.02Al0.01(OH)2とリチウム源を、所定の割合で乾式混合し、前駆体とリチウム源中のLi元素を1:1.05のモル比で混合した後、850℃、酸素ガスの雰囲気下、一次焼結を10h行い、冷却して粉砕し、400メッシュの篩にかけて、一回目の焼結による準単結晶正極材料を得た。
(1)前駆体Ni0.92Co0.05Mn0.02Al0.01(OH)2とリチウム源を、所定の割合で乾式混合し、前駆体とリチウム源中のLi元素を、1:1.05モル比で混合した後、850℃、酸素ガスの雰囲気下、一次焼結を10h行い、冷却して粉砕し、400メッシュの篩にかけて、一回目の焼結による準単結晶正極材料を得た。
(1)前駆体Ni0.92Co0.05Mn0.02Al0.01(OH)2とリチウム源を、所定の割合で乾式混合し、前駆体とリチウム源中のLi元素を1:1.05のモル比で混合した後、850℃、酸素ガスの雰囲気下、一次焼結を10h行い、冷却して粉砕し、篩にかけて、一回目の焼結による準単結晶正極材料を得た。
実施例2との区別として、一回目の焼結による準単結晶正極材料と、被覆剤Ni(OH)2中のNi元素とを、1:0.0015の質量比で均一に乾式混合した。
実施例2との区別として、一回目の焼結による準単結晶正極材料と、被覆剤Ni(OH)2中のNi元素とを、1:0.0025の質量比で均一に乾式混合した。
実施例2との区別として、正極前駆体材料とリチウム源材料中のリチウム元素とのモル比は1:1.35であった。
実施例2との区別として、正極前駆体材料とリチウム源材料中のリチウム元素とのモル比は1:0.8であった。
実施例2との区別として、正極前駆体材料とリチウム源材料中のリチウム元素とのモル比は1:1.6であった。
実施例2との区別として、一回目の焼結の温度は950℃であった。
実施例2との区別として、一回目の焼結の温度は1050℃であった。
実施例2との区別として、二回目の焼結の温度は150℃であった。
実施例2との区別として、二回目の焼結の温度は250℃であった。
実施例2との区別として、二回目の焼結の温度は300℃であった。
実施例2との区別として、第1の焙焼後、破砕して選別し、200メッシュの篩にかけて、第2の焙焼を直接行った。
実施例2との区別として、第1の焙焼後、破砕して選別し、200メッシュの篩にかけて、第2の焙焼後、破砕選別を行わなかった。
(1)前駆体Ni0.92Co0.05Mn0.02Al0.01(OH)2とリチウム源を、所定の割合で乾式混合し、前駆体とリチウム源中のLi元素を1:1.05のモル比で混合した後、850℃、酸素ガスの雰囲気下、一次焼結を10h行い、冷却して粉砕し、篩にかけて、一回目の焼結による準単結晶正極材料を得た。
(1)前駆体Ni0.92Co0.05Mn0.02Al0.01(OH)2とリチウム源を、所定の割合で乾式混合し、前駆体とリチウム源中のLi元素を1:1.05のモル比で混合した後、850℃、酸素ガスの雰囲気下、一次焼結を10h行い、冷却して粉砕し、篩にかけて、一回目の焼結による準単結晶正極材料を得た。
Claims (10)
- リチウム源材料と正極前駆体材料に対して第1の焼結処理を行って、第1の焼結生成物を得るステップと、
前記第1の焼結生成物の表面にニッケル源材料及び/又はマンガン源材料である被覆剤を被覆し、その後、第2の焼結処理を行って、前記正極材料を得るステップとを含む、ことを特徴とする正極材料の製造方法。 - 前記マンガン源材料はMn(OH)2、MnO、MnO2、Mn2O3、Mn3O4、Mn2O7、及びMnCO3からなる群から選ばれる1種又は複数種であり、前記ニッケル源材料はNi(OH)2、NiSO4、NiCO3、NiF2、NiCl2、NiBr2、NiI2、及びNi2O3からなる群から選ばれる1種又は複数種である、ことを特徴とする請求項1に記載の製造方法。
- 前記第1の焼結生成物の重量と、前記被覆剤中のニッケル元素及びマンガン元素の総重量との比が、1:(0.0008~0.0015)である、ことを特徴とする請求項1又は2に記載の製造方法。
- 前記第2の焼結処理は、温度150~250℃、処理時間4~8hである、ことを特徴とする請求項3の製造方法。
- 前記第1の焼結処理は、温度700~1000℃、焼結時間8~20hであり、
好ましくは、前記第1の焼結処理の温度は800~950℃である、ことを特徴とする請求項1~4のいずれか1項に記載の製造方法。 - 前記リチウム源材料は、水酸化リチウム、炭酸リチウム、酢酸リチウム、酸化リチウム、硝酸リチウム、及びシュウ酸リチウムからなる群のうちの1種又は複数種であり、前記正極前駆体材料は、NiaCobMncAldMy(OH)2で示される化合物であり、MはY、Sr、Mo、La、Al、Zr、Ti、Mg、B、Nb、Ba、Si、P、W元素のうちの1種又は複数種であり、且つaは0.5~0.92、bは0.02~0.06、cは0.01~0.03、dは0.01~0.03、yは0.00~0.01である、ことを特徴とする請求項1に記載の製造方法。
- 複数の単結晶粒子で形成される準単結晶正極材料であり、前記単結晶粒子の粒子径が0.10~2μm、前記準単結晶正極材料の粒子径D50が2~7.5μmであり、
ニッケル・コバルト・マンガン・リチウム複合酸化物と、前記ニッケルコバルトマンガンアルミン酸リチウム上に被覆される被覆層とを含み、前記被覆層はニッケル源材料及び/又はマンガン源材料を焼結して形成したマンガン酸リチウム及び/又はニッケル酸リチウムであり、又は、前記正極材料は請求項1~6のいずれか1項に記載の製造方法で製造される、ことを特徴とする正極材料。 - 前記正極材料の化学一般式はLixNiaCobMncAldMyRzO2であり、式中、1.00≦x≦1.35、0<y≦0.01、0<z≦0.01、0<a≦0.92、0<b≦0.06、0<c≦0.03、0<d≦0.03、a+b+c+d+z=1であり、MはY、Sr、Mo、La、Al、Zr、Ti、Mg、B、Nb、Ba、Si、P、W元素のうちの1種又は複数種であり、RはNi元素及び/又はMn元素である、ことを特徴とする請求項7に記載の正極材料。
- 前記ニッケルコバルトマンガンアルミン酸リチウムの粒子径D50は2~7.5μmであり、前記被覆層中の粒子物の粒子径は0.01~0.45μmである、ことを特徴とする請求項7に記載の正極材料。
- 正極材料を含むリチウムイオン電池であって、
前記正極材料は請求項7~9のいずれか1項に記載の正極材料を含むことを特徴とするリチウムイオン電池。
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- 2020-10-28 EP EP20942519.8A patent/EP4002520A4/en active Pending
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CN111628157B (zh) | 2024-03-26 |
WO2022000889A1 (zh) | 2022-01-06 |
EP4002520A1 (en) | 2022-05-25 |
KR20220127277A (ko) | 2022-09-19 |
EP4002520A4 (en) | 2023-09-13 |
JP7416956B2 (ja) | 2024-01-17 |
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US20230327082A1 (en) | 2023-10-12 |
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