JP2020505739A - リチウムイオン電池用の安定化された活物質 - Google Patents
リチウムイオン電池用の安定化された活物質 Download PDFInfo
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- 239000011149 active material Substances 0.000 title claims description 24
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title description 9
- 229910001416 lithium ion Inorganic materials 0.000 title description 9
- 238000000576 coating method Methods 0.000 claims abstract description 51
- 239000007774 positive electrode material Substances 0.000 claims abstract description 51
- 239000011248 coating agent Substances 0.000 claims abstract description 50
- 239000000463 material Substances 0.000 claims abstract description 50
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 48
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 20
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 20
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 20
- 238000004519 manufacturing process Methods 0.000 claims abstract description 13
- 229910014689 LiMnO Inorganic materials 0.000 claims description 36
- 238000000034 method Methods 0.000 claims description 22
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 claims description 16
- 239000002245 particle Substances 0.000 claims description 15
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 claims description 12
- 230000015572 biosynthetic process Effects 0.000 claims description 8
- 239000007771 core particle Substances 0.000 claims description 7
- 230000001351 cycling effect Effects 0.000 claims description 6
- 239000010420 shell particle Substances 0.000 claims description 6
- 241000156302 Porcine hemagglutinating encephalomyelitis virus Species 0.000 claims description 4
- 239000006182 cathode active material Substances 0.000 claims description 4
- 238000006243 chemical reaction Methods 0.000 claims description 4
- 238000003746 solid phase reaction Methods 0.000 claims description 2
- 239000007787 solid Substances 0.000 claims 1
- 239000000126 substance Substances 0.000 claims 1
- 229910002993 LiMnO2 Inorganic materials 0.000 abstract 1
- 239000011572 manganese Substances 0.000 description 20
- 239000000203 mixture Substances 0.000 description 20
- 239000002904 solvent Substances 0.000 description 11
- 229910001317 nickel manganese cobalt oxide (NMC) Inorganic materials 0.000 description 10
- 239000003792 electrolyte Substances 0.000 description 8
- 229910052748 manganese Inorganic materials 0.000 description 8
- -1 polytetrafluoroethylene Polymers 0.000 description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 229910052596 spinel Inorganic materials 0.000 description 6
- 239000011029 spinel Substances 0.000 description 6
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 5
- 229910052782 aluminium Inorganic materials 0.000 description 5
- 239000007773 negative electrode material Substances 0.000 description 5
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 4
- 239000002033 PVDF binder Substances 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 4
- 239000002184 metal Substances 0.000 description 4
- 239000002114 nanocomposite Substances 0.000 description 4
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- 239000001301 oxygen Substances 0.000 description 4
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- 239000004810 polytetrafluoroethylene Substances 0.000 description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 3
- 239000000654 additive Substances 0.000 description 3
- 239000011230 binding agent Substances 0.000 description 3
- 229910003002 lithium salt Inorganic materials 0.000 description 3
- 159000000002 lithium salts Chemical class 0.000 description 3
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- 238000010532 solid phase synthesis reaction Methods 0.000 description 3
- 239000007858 starting material Substances 0.000 description 3
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 2
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- 229910015118 LiMO Inorganic materials 0.000 description 2
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- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 description 2
- 229910045601 alloy Inorganic materials 0.000 description 2
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- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 2
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- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 238000009830 intercalation Methods 0.000 description 2
- VGYDTVNNDKLMHX-UHFFFAOYSA-N lithium;manganese;nickel;oxocobalt Chemical compound [Li].[Mn].[Ni].[Co]=O VGYDTVNNDKLMHX-UHFFFAOYSA-N 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
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- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229910018068 Li 2 O Inorganic materials 0.000 description 1
- 229910013063 LiBF 4 Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910013716 LiNi Inorganic materials 0.000 description 1
- 229910002992 LiNi0.33Mn0.33Co0.33O2 Inorganic materials 0.000 description 1
- 229910012578 LiNi0.4Mn0.3Co0.3O2 Inorganic materials 0.000 description 1
- 229910012748 LiNi0.5Mn0.3Co0.2O2 Inorganic materials 0.000 description 1
- 229910011322 LiNi0.6Mn0.2Co0.2O2 Inorganic materials 0.000 description 1
- 229910002995 LiNi0.8Co0.15Al0.05O2 Inorganic materials 0.000 description 1
- 229910015965 LiNi0.8Mn0.1Co0.1O2 Inorganic materials 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- 239000002174 Styrene-butadiene Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- NDPGDHBNXZOBJS-UHFFFAOYSA-N aluminum lithium cobalt(2+) nickel(2+) oxygen(2-) Chemical compound [Li+].[O--].[O--].[O--].[O--].[Al+3].[Co++].[Ni++] NDPGDHBNXZOBJS-UHFFFAOYSA-N 0.000 description 1
- 229910021417 amorphous silicon Inorganic materials 0.000 description 1
- 150000001722 carbon compounds Chemical class 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
- CXULZQWIHKYPTP-UHFFFAOYSA-N cobalt(2+) manganese(2+) nickel(2+) oxygen(2-) Chemical compound [O--].[O--].[O--].[Mn++].[Co++].[Ni++] CXULZQWIHKYPTP-UHFFFAOYSA-N 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
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- 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
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- H—ELECTRICITY
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M4/00—Electrodes
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- H01M4/04—Processes of manufacture in general
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
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- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- 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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- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
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Abstract
Description
電気エネルギーの貯蔵は、ここ数十年でよりいっそう大きな重要性を得ている。電気エネルギーは、電池を用いて貯蔵可能である。電池は、化学反応エネルギーを電気エネルギーに変換する。この場合、一次電池と二次電池は区別される。一次電池は、一回だけ機能する能力があるが、蓄電池ともいわれる二次電池は、再充電可能である。電池は、この場合、1つ以上の電池セルを含む。
リチウムとニッケルとを含む少なくとも1つの混合酸化物(以後混合酸化物ともいう)を含み、この混合酸化物の表面の少なくとも一部に、LiMnO2を含む被覆材料が塗布されている、電気化学セルの正極用の正極活物質が提案される。
記載された、LiMnO2を含む被覆材料を含む正極活物質は、被覆材料を簡単な固相合成により低コストの出発物質から製造することができ、かつこの被覆材料はその層状構造に基づき、同様に層状構造で存在する被覆されるべき混合酸化物と極めて良好に適合することにより優れている。この正極活物質を使用する電池セルの出力を損なう界面損傷効果は起こらない。さらに、被覆は、ニッケル含有混合酸化物を、正極活物質からのニッケル原子の損失、およびそれと関連する容量損失から保護する。マンガン富有LiMnO2は、熱的に安定である。電池セルの化成および/またはサイクルの間のLiMnO2からLiMn2O4への変換により、混合酸化物の表面の少なくとも一部にスピネル構造を有する被覆が得られ、この被覆は安定化作用を有するばかりか、同時にそれ自体正極活物質としてエネルギー貯蔵にも関与する。混合酸化物と被覆材料との構造の密接な噛み合いにより、極端に安定な複合材料が生じる。
本発明の実施形態を、図面および次の記載に基づいて詳細に説明する。
図1には、コア/シェル粒子の形で存在する活物質粒子1の概略図を示す。活物質粒子1のコア52は、ニッケルを含む混合酸化物、ことにリチウム過剰高エネルギーニッケル−コバルト−マンガン酸化物(HE−NMC)から形成されている。ここでは、例えばLi1.17Ni0.17Co0.1Mn0.56O2が使用される。混合酸化物の粒子は、好ましくは1nm〜100nm、ここでは約10nmの平均粒子サイズを有する。混合酸化物粒子の表面上に、LiMnO2を含む被覆が塗布され、これはコア/シェル粒子のシェル62を形成する。これは、例えば0.1〜2nmの平均層厚で混合酸化物からなるコア52を完全に取り囲む。被覆のLiMnO2を含む材料は、固相合成法でMn2O3およびLiOH・H2Oから製造され、ここでこの方法は、混合酸化物粒子の存在で実施されるので、LiMnO2の合成および混合酸化物粒子の被覆は、1つの方法工程で達成される。得られた複合材料を、引き続き正極22の製造のために使用することができる。
Claims (12)
- リチウムとニッケルとを含む混合酸化物を含み、前記混合酸化物の表面の少なくとも一部に、LiMnO2を含む被覆材料が塗布されている、電気化学セルの正極(22)用の正極活物質(42)。
- 前記正極活物質(42)は、コア/シェル粒子の形で存在し、前記コア(52)は少なくとも1つの混合酸化物を含み、かつ前記シェル(62)はLiMnO2を含む前記被覆材料により形成される、活物質粒子(1)を含む、請求項1記載の正極活物質(42)。
- 電気化学セルの正極(22)用の正極活物質(42)の製造方法において、前記正極活物質(42)は、リチウムとニッケルとを含む混合酸化物を含み、前記混合酸化物の表面の少なくとも一部に、LiMnO2を含む被覆材料が塗布されていて、かつ前記LiMnO2は、Mn2O3とLiOH・H2Oとの固相反応から得られる、正極活物質(42)の製造方法。
- 電気化学セルの正極(22)用の正極活物質(42)の製造方法において、前記正極活物質(42)は、リチウムとニッケルとを含む混合酸化物を含み、前記混合酸化物の表面の少なくとも一部に、LiMnO2を含む被覆材料が塗布されていて、かつ前記方法は、まず、LiMnO2を含む被覆材料を前記混合酸化物の表面に塗布する工程を含む、正極活物質(42)の製造方法。
- LiMnO2を含む前記被覆材料は、Mn2O3とLiOH・H2Oとの固相反応から得られる、請求項4記載の正極活物質(42)の製造方法。
- 前記方法は、前記活物質の化成および/またはサイクルを含む、請求項4または5記載の正極活物質(42)の製造方法。
- 前記化成および/またはサイクルを電気化学セル中で行う、請求項6記載の正極活物質(42)の製造方法。
- 請求項3から7までのいずれか1項記載の方法により得られる、混合酸化物の表面の少なくとも一部に、LiMn2O4を含む被覆材料が塗布されている、混合酸化物を含む正極活物質(42)。
- 電気化学セルまたはバッテリーの正極(22)の製造のための、請求項1、2または8記載の正極活物質(42)の使用。
- 請求項1、2または8記載の正極活物質(42)を含む、正極(22)。
- 請求項10記載の少なくとも1つの正極(22)を含む電池セル(2)。
- 電気自動車(EV)における、ハイブリッド自動車(HEV)における、プラグインハイブリッド自動車(PHEV)における、工具における、またはコンシューマーエレクトロニクス製品における、請求項11記載の電池セル(2)の使用。
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US11495796B2 (en) | 2018-11-14 | 2022-11-08 | Samsung Sdi Co., Ltd. | Positive active material for rechargeable lithium battery, method of preparing the same and rechargeable lithium battery including the same |
US11757092B2 (en) | 2018-11-15 | 2023-09-12 | Samsung Sdi Co., Ltd. | Positive active material for rechargeable lithium battery, method of preparing the same and rechargeable lithium battery including the same |
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