JPWO2018207049A1 - 正極活物質粒子 - Google Patents
正極活物質粒子 Download PDFInfo
- Publication number
- JPWO2018207049A1 JPWO2018207049A1 JP2019516737A JP2019516737A JPWO2018207049A1 JP WO2018207049 A1 JPWO2018207049 A1 JP WO2018207049A1 JP 2019516737 A JP2019516737 A JP 2019516737A JP 2019516737 A JP2019516737 A JP 2019516737A JP WO2018207049 A1 JPWO2018207049 A1 JP WO2018207049A1
- Authority
- JP
- Japan
- Prior art keywords
- positive electrode
- active material
- crystal grain
- electrode active
- secondary battery
- 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
- 239000002245 particle Substances 0.000 title claims abstract description 191
- 239000006182 cathode active material Substances 0.000 title description 4
- 239000013078 crystal Substances 0.000 claims abstract description 385
- 239000007774 positive electrode material Substances 0.000 claims abstract description 207
- 239000011777 magnesium Substances 0.000 claims abstract description 168
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims abstract description 136
- 229910052749 magnesium Inorganic materials 0.000 claims abstract description 126
- 150000003624 transition metals Chemical class 0.000 claims abstract description 106
- 229910052723 transition metal Inorganic materials 0.000 claims abstract description 96
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 57
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- 239000001301 oxygen Substances 0.000 claims abstract description 57
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 49
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 44
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 133
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- 239000011737 fluorine Substances 0.000 claims description 118
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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 claims description 30
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- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 description 1
- WBJZTOZJJYAKHQ-UHFFFAOYSA-K iron(3+) phosphate Chemical compound [Fe+3].[O-]P([O-])([O-])=O WBJZTOZJJYAKHQ-UHFFFAOYSA-K 0.000 description 1
- PVFSDGKDKFSOTB-UHFFFAOYSA-K iron(3+);triacetate Chemical compound [Fe+3].CC([O-])=O.CC([O-])=O.CC([O-])=O PVFSDGKDKFSOTB-UHFFFAOYSA-K 0.000 description 1
- GYCHYNMREWYSKH-UHFFFAOYSA-L iron(ii) bromide Chemical compound [Fe+2].[Br-].[Br-] GYCHYNMREWYSKH-UHFFFAOYSA-L 0.000 description 1
- BQZGVMWPHXIKEQ-UHFFFAOYSA-L iron(ii) iodide Chemical compound [Fe+2].[I-].[I-] BQZGVMWPHXIKEQ-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
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- DEUISMFZZMAAOJ-UHFFFAOYSA-N lithium dihydrogen borate oxalic acid Chemical compound B([O-])(O)O.C(C(=O)O)(=O)O.C(C(=O)O)(=O)O.[Li+] DEUISMFZZMAAOJ-UHFFFAOYSA-N 0.000 description 1
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- 230000007704 transition Effects 0.000 description 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 1
- ZMQDTYVODWKHNT-UHFFFAOYSA-N tris(2,2,2-trifluoroethyl) phosphate Chemical compound FC(F)(F)COP(=O)(OCC(F)(F)F)OCC(F)(F)F ZMQDTYVODWKHNT-UHFFFAOYSA-N 0.000 description 1
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 description 1
- VLOPEOIIELCUML-UHFFFAOYSA-L vanadium(2+);sulfate Chemical compound [V+2].[O-]S([O-])(=O)=O VLOPEOIIELCUML-UHFFFAOYSA-L 0.000 description 1
- 238000001947 vapour-phase growth Methods 0.000 description 1
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- UGZADUVQMDAIAO-UHFFFAOYSA-L zinc hydroxide Chemical compound [OH-].[OH-].[Zn+2] UGZADUVQMDAIAO-UHFFFAOYSA-L 0.000 description 1
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Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—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
- H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/364—Composites as mixtures
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G51/00—Compounds of cobalt
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G53/00—Compounds of nickel
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/04—Hybrid capacitors
- H01G11/06—Hybrid capacitors with one of the electrodes allowing ions to be reversibly doped thereinto, e.g. lithium ion capacitors [LIC]
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/30—Electrodes characterised by their material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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Abstract
Description
[正極活物質の構造]
本発明の一態様である正極活物質粒子100について、図1(A)乃至図1(C)、図2(A)乃至図2(C)を用いて説明する。
本発明の一態様である正極活物質粒子100が有する結晶粒界103は、マグネシウム及び酸素を有する。結晶粒界103は酸化マグネシウムを有する。また、結晶粒界103はさらにフッ素を有すると好ましい。酸化マグネシウムが有する一部の酸素がフッ素で置換されていてもよい。酸化マグネシウムが部分的にフッ素で置換されることにより、例えばリチウムの拡散性を高めることができ、充放電を妨げない。結晶粒界103はフッ素を有することで、フッ酸に溶けにくい場合がある。
本発明の一態様である正極活物質粒子100が有する結晶粒101は、リチウム、遷移金属及び酸素を含む。例えば、結晶粒101は、リチウム、遷移金属及び酸素を含む複合酸化物を有する。また、遷移金属として、鉄、コバルト、ニッケル、マンガン、クロム、チタン、バナジウム、ニオブ等の一以上を用いることができる。
結晶粒101及び結晶粒界103を有する正極活物質粒子100の作製方法を、図3を用いて説明する。結晶粒101は、リチウム、遷移金属(M)及び酸素を含む複合酸化物を有する。結晶粒界103はマグネシウム、フッ素及び酸素を有する。
本実施の形態では、先の実施の形態で説明した正極活物質粒子100を有する二次電池に用いることのできる材料の例について説明する。本実施の形態では、正極、負極および電解液が、外装体に包まれている二次電池を例にとって説明する。
正極は、正極活物質層および正極集電体を有する。
正極活物質層は、正極活物質粒子を有する。また、正極活物質層は、導電助剤およびバインダを有していてもよい。
正極集電体としては、ステンレス、金、白金、アルミニウム、チタン等の金属、及びこれらの合金など、導電性が高い材料をもちいることができる。また正極集電体に用いる材料は、正極の電位で溶出しないことが好ましい。また、シリコン、チタン、ネオジム、スカンジウム、モリブデンなどの耐熱性を向上させる元素が添加されたアルミニウム合金を用いることができる。また、シリコンと反応してシリサイドを形成する金属元素で形成してもよい。シリコンと反応してシリサイドを形成する金属元素としては、ジルコニウム、チタン、ハフニウム、バナジウム、ニオブ、タンタル、クロム、モリブデン、タングステン、コバルト、ニッケル等がある。集電体は、箔状、板状(シート状)、網状、パンチングメタル状、エキスパンドメタル状等の形状を適宜用いることができる。集電体は、厚みが5μm以上30μm以下のものを用いるとよい。
負極は、負極活物質層および負極集電体を有する。また、負極活物質層は、導電助剤およびバインダを有していてもよい。
負極活物質としては、例えば合金系材料や炭素系材料等を用いることができる。
負極集電体には、正極集電体と同様の材料を用いることができる。なお負極集電体は、リチウム等のキャリアイオンと合金化しない材料を用いることが好ましい。
電解液は、溶媒と電解質を有する。電解液の溶媒としては、非プロトン性有機溶媒が好ましく、例えば、エチレンカーボネート(EC)、プロピレンカーボネート(PC)、ブチレンカーボネート、クロロエチレンカーボネート、ビニレンカーボネート、γ−ブチロラクトン、γ−バレロラクトン、ジメチルカーボネート(DMC)、ジエチルカーボネート(DEC)、エチルメチルカーボネート(EMC)、ギ酸メチル、酢酸メチル、酢酸エチル、プロピオン酸メチル、プロピオン酸エチル、プロピオン酸プロピル、酪酸メチル、1,3−ジオキサン、1,4−ジオキサン、ジメトキシエタン(DME)、ジメチルスルホキシド、ジエチルエーテル、メチルジグライム、アセトニトリル、ベンゾニトリル、テトラヒドロフラン、スルホラン、スルトン等の1種、又はこれらのうちの2種以上を任意の組み合わせおよび比率で用いることができる。
また二次電池は、セパレータを有することが好ましい。セパレータとしては、例えば、紙をはじめとするセルロースを有する繊維、不織布、ガラス繊維、セラミックス、或いはナイロン(ポリアミド)、ビニロン(ポリビニルアルコール系繊維)、ポリエステル、アクリル、ポリオレフィン、ポリウレタンを用いた合成繊維等で形成されたものを用いることができる。セパレータは袋状に加工し、正極または負極のいずれか一方を包むように配置することが好ましい。
本実施の形態では、先の実施の形態で説明した正極活物質粒子100を有する二次電池の形状の例について説明する。本実施の形態で説明する二次電池に用いる材料は、先の実施の形態の記載を参酌することができる。
まずコイン型の二次電池の一例について説明する。図5(A)はコイン型(単層偏平型)の二次電池の外観図であり、図5(B)は、その断面図である。
円筒型の二次電池の例について図6(A)乃至図6(D)を参照して説明する。円筒型の二次電池600は、図6(A)に示す円筒型の二次電池600は、図6(B)の断面模式図に示すように、上面に正極キャップ(電池蓋)601を有し、側面および底面に電池缶(外装缶)602を有している。これら正極キャップと電池缶(外装缶)602とは、ガスケット(絶縁パッキン)610によって絶縁されている。
蓄電装置の別の構造例について、図7乃至図11を用いて説明する。
次に、ラミネート型の二次電池の例について、図12乃至図17を参照して説明する。ラミネート型の二次電池は、可撓性を有する構成とすれば、可撓性を有する部位を少なくとも一部有する電子機器に実装すれば、電子機器の変形に合わせて二次電池も曲げることもできる。
ここで、図14に外観図を示すラミネート型二次電池の作製方法の一例について、図16(B)及び図16(C)を用いて説明する。
次に、曲げることのできる二次電池の例について図17及び図18を参照して説明する。
本実施の形態では、本発明の一態様である二次電池を電子機器に実装する例について説明する。
本実施の形態では、車両に本発明の一態様である二次電池を搭載する例を示す。
試料Aの作製について説明する。
次に、試料Aを集束イオンビーム(FIB:Focused Ion Beam)により薄片化し、試料Aの断面をTEM及びSTEMで観察した。また、試料Aの断面を、EDX測定で組成分析を行った。TEM、STEM観察及びEDX測定には、日本電子社製JEM−ARM200Fを用い、加速電圧は200kV、ビーム径は約0.1nmφとした。
試料Bの作製について説明する。
次に、試料Bを集束イオンビーム(FIB)により薄片化し、試料Bの断面をTEM及びSTEMで観察した。また、試料Bの断面を、EDX測定で組成分析を行った。TEM、STEM観察及びEDX測定の詳細は試料Aの記載を参照できるため、説明を省略する。
Claims (5)
- 第1の結晶粒と、第2の結晶粒と、前記第1の結晶粒及び前記第2の結晶粒の間に位置する結晶粒界と、を有し、
前記第1の結晶粒及び前記第2の結晶粒は、リチウムと、遷移金属と、酸素と、を有し、
前記結晶粒界は、マグネシウムと、酸素と、を有し、
前記結晶粒界は、前記第1の結晶粒及び前記第2の結晶粒よりマグネシウム濃度が高い領域を有する、正極活物質粒子。 - 請求項1において、
前記遷移金属の原子濃度に対する、前記マグネシウムの原子濃度の比が、0.010以上0.50以下の領域を有する正極活物質粒子。 - 請求項1又は請求項2において、
前記結晶粒界はさらにフッ素を有し、
前記結晶粒界は、前記第1の結晶粒及び前記第2の結晶粒よりフッ素濃度が高い領域を有する、正極活物質粒子。 - 請求項3において、
前記遷移金属の原子濃度に対する、前記フッ素の原子濃度の比が、0.020以上1.00以下の領域を有する正極活物質粒子。 - 請求項1又は請求項2において、
前記遷移金属として、鉄、コバルト、ニッケル、マンガン、クロム、チタン、バナジウム及びニオブのいずれか一以上を有する、正極活物質粒子。
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