WO2021049318A1 - 非水電解質二次電池用正極活物質、及び非水電解質二次電池 - Google Patents

非水電解質二次電池用正極活物質、及び非水電解質二次電池 Download PDF

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WO2021049318A1
WO2021049318A1 PCT/JP2020/032532 JP2020032532W WO2021049318A1 WO 2021049318 A1 WO2021049318 A1 WO 2021049318A1 JP 2020032532 W JP2020032532 W JP 2020032532W WO 2021049318 A1 WO2021049318 A1 WO 2021049318A1
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positive electrode
particles
composite oxide
active material
electrode active
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English (en)
French (fr)
Japanese (ja)
Inventor
なつみ 後藤
貴志 神
鈴木　慎也
史治 新名
翔 鶴田
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Panasonic Corp
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Panasonic Corp
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Priority to CN202080061903.4A priority Critical patent/CN114342116B/zh
Priority to EP25193104.4A priority patent/EP4618192A3/en
Priority to EP20862903.0A priority patent/EP4030508B1/en
Priority to US17/640,249 priority patent/US20220320490A1/en
Priority to JP2021545210A priority patent/JP7608345B2/ja
Publication of WO2021049318A1 publication Critical patent/WO2021049318A1/ja
Anticipated expiration legal-status Critical
Priority to JP2024221414A priority patent/JP7751719B2/ja
Priority to JP2025159924A priority patent/JP2025175191A/ja
Ceased legal-status Critical Current

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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
    • H01M4/364—Composites as mixtures
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G53/00—Compounds of nickel
    • C01G53/80—Compounds containing nickel, with or without oxygen or hydrogen, and containing one or more other elements
    • C01G53/82—Compounds containing nickel, with or without oxygen or hydrogen, and containing two or more other elements
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G53/00—Compounds of nickel
    • C01G53/40—Complex oxides containing nickel and at least one other metal element
    • C01G53/42—Complex oxides containing nickel and at least one other metal element containing alkali metals, e.g. LiNiO2
    • C01G53/44—Complex oxides containing nickel and at least one other metal element containing alkali metals, e.g. LiNiO2 containing manganese
    • C01G53/50—Complex oxides containing nickel and at least one other metal element containing alkali metals, e.g. LiNiO2 containing manganese of the type (MnO2)n-, e.g. Li(NixMn1-x)O2 or Li(MyNixMn1-x-y)O2
    • 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
    • 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
    • H01M4/13—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
    • 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
    • H01M4/52—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
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/50—Solid solutions
    • C01P2002/52—Solid solutions containing elements as dopants
    • C01P2002/54—Solid solutions containing elements as dopants one element only
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/51—Particles with a specific particle size distribution
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/51—Particles with a specific particle size distribution
    • C01P2004/53—Particles with a specific particle size distribution bimodal size distribution
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/60—Particles characterised by their size
    • C01P2004/61—Micrometer sized, i.e. from 1-100 micrometer
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/80—Particles consisting of a mixture of two or more inorganic phases
    • C01P2004/82—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases
    • C01P2004/84—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases one phase coated with the other
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
    • 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
    • H01M4/50—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
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the composite oxide (Z) is a particle having a volume-based median diameter (D50) of, for example, 3 ⁇ m to 30 ⁇ m, preferably 5 ⁇ m to 25 ⁇ m, and particularly preferably 7 ⁇ m to 15 ⁇ m.
  • D50 means a particle size in which the cumulative frequency is 50% from the smallest particle size in the volume-based particle size distribution, and is also called a median diameter.
  • the particle size distribution of the composite oxide (Z) can be measured using water as a dispersion medium using a laser diffraction type particle size distribution measuring device (for example, MT3000II manufactured by Microtrac Bell Co., Ltd.).
  • D70 means a particle size in which the cumulative frequency is 70% from the smallest particle size in the volume-based particle size distribution.
  • D30 means a particle size in which the cumulative frequency is 30% from the smallest particle size in the volume-based particle size distribution.
  • D70 is 9 ⁇ m to 19 ⁇ m and D30 is 3 ⁇ m to 13 ⁇ m.
  • the mole fraction of the metal element present on the particle surface of the composite oxide (Z) is measured by X-ray photoelectron spectroscopy (XPS).
  • B may also be present inside the primary particles and may be solid-solved with a transition metal element such as Ni.
  • the mole fraction of B with respect to the solid-dissolved metal element can be confirmed by energy dispersive X-ray spectroscopy (EDS) in the cross section of the primary particle.
  • EDS energy dispersive X-ray spectroscopy
  • the total number of moles of B in the solid solution state and B in the state of the boron compound existing on the surface is 0.001 to 0.020 with respect to the total number of moles of the metal element excluding Li. Is preferable.
  • the firing temperature in the above step (2) is, for example, 200 ° C. to 500 ° C.
  • the firing temperature of the composite oxides (Y1) and (Y2) is, for example, 200 ° C. to 500 ° C.
  • the surface coverage of B in the composite oxides (Z1) and the composite oxides (Z2) and the thickness of the boron compound can be adjusted.
  • composite oxides (Z1) and (Z2) having a low surface coverage of B on the particle surface can be synthesized.
  • composite oxides (Z1) and (Z2) having a high surface coverage of B on the particle surface can be synthesized.
  • the high temperature is, for example, 350 ° C.
  • a porous sheet having ion permeability and insulating property is used as the separator 13.
  • the porous sheet include a microporous thin film, a woven fabric, and a non-woven fabric.
  • polyolefins such as polyethylene and polypropylene, cellulose and the like are suitable.
  • the separator 13 may have either a single-layer structure or a laminated structure. A heat-resistant layer or the like may be formed on the surface of the separator.
  • lithium hydroxide and nickel-cobalt-manganese composite oxide (X1) having a large average particle size are mixed so that the molar ratio of the total amounts of Li, Ni, Co, and Mn is 1.08: 1, respectively. did.
  • This mixture was calcined at 700 ° C. for 8 hours in an oxygen atmosphere and then pulverized to obtain a lithium composite oxide (X2) having a large average particle size.
  • the obtained lithium composite oxide (X2) was not washed with water.
  • lithium hydroxide and nickel-cobalt-manganese composite oxide (Y1) having a small average particle size are mixed so that the molar ratio of the total amounts of Li, Ni, Co, and Mn is 1.08: 1, respectively. did.
  • This mixture was calcined at 700 ° C. for 8 hours in an oxygen atmosphere and then pulverized to obtain a lithium composite oxide (Y2) having a small average particle size.
  • the obtained lithium composite oxide (Y2) was not washed with water.
  • the total amount of Ni, Co, and Mn of lithium composite oxide (X2) having a large average particle size and boric acid (H 3 BO 3 ) and the molar ratio of B in H 3 BO 3 are 1: 1.
  • the mixture was dry-mixed to 0.005, and the mixture was fired in the air at 300 ° C. for 3 hours and then pulverized to obtain a lithium composite oxide (X3) in which B was present on the particle surface.
  • the composition of the positive electrode active material by ICP As a result of analyzing the composition of the positive electrode active material by ICP, it was Li 1.01 Ni 0.84 Co 0.08 Mn 0.07 B 0.01 O 2 . Therefore, from the result of ICP, the mole fraction of B with respect to the total number of moles of the metal elements (Ni, Co, Mn, B) excluding Li was 1.0%. Further, as a result of analyzing the composition of the lithium composite oxide (X3) and (Y3) by ICP, the mole fraction of B with respect to the total number of moles of the metal elements (Ni, Co, Mn, B) excluding Li was determined. , 0.5% and 1.5%.
  • the positive electrode active material, acetylene black, and polyvinylidene fluoride (PVdF) are mixed at a solid content mass ratio of 96.3: 2.5: 1.2, and an appropriate amount of N-methyl-2-pyrrolidone (NMP) is added. After the addition, this was kneaded to prepare a positive electrode mixture slurry.
  • the positive electrode mixture slurry is applied to both sides of the positive electrode core made of aluminum foil, the coating film is dried, and then the coating film is rolled using a roller and cut to a predetermined electrode size to form the positive electrode core. A positive electrode having a positive electrode mixture layer formed on both sides was obtained. An exposed portion where the surface of the positive electrode core was exposed was provided on a part of the positive electrode.
  • An aluminum lead is attached to the exposed portion of the positive electrode, and a nickel lead is attached to the exposed portion of the negative electrode.
  • the positive electrode and the negative electrode are spirally wound via a polyolefin separator, and then press-molded in the radial direction to form a flat shape.
  • a wound electrode body was produced. This electrode body was housed in an exterior body made of an aluminum laminated sheet, and after injecting the non-aqueous electrolyte, the opening of the exterior body was sealed to obtain a non-aqueous electrolyte secondary battery having a design capacity of 650 mAh. ..
  • Example 2 A non-aqueous electrolyte secondary battery was produced in the same manner as in Example 1 except that each of X2 and Y2 was washed with water.
  • Table 1 shows the mole fraction of B and the surface coverage of B with respect to the total number of moles of the metal element excluding Li in the first particle and the second particle.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Composite Materials (AREA)
  • Manufacturing & Machinery (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Secondary Cells (AREA)
PCT/JP2020/032532 2019-09-09 2020-08-28 非水電解質二次電池用正極活物質、及び非水電解質二次電池 Ceased WO2021049318A1 (ja)

Priority Applications (7)

Application Number Priority Date Filing Date Title
CN202080061903.4A CN114342116B (zh) 2019-09-09 2020-08-28 非水电解质二次电池用正极活性物质和非水电解质二次电池
EP25193104.4A EP4618192A3 (en) 2019-09-09 2020-08-28 Positive electrode active material for nonaqueous electrolyte secondary battery, and nonaqueous electrolyte secondary battery
EP20862903.0A EP4030508B1 (en) 2019-09-09 2020-08-28 Positive electrode active material for nonaqueous electrolyte secondary battery, and nonaqueous electrolyte secondary battery
US17/640,249 US20220320490A1 (en) 2019-09-09 2020-08-28 Positive electrode active material for nonaqueous electrolyte secondary battery, and nonaqueous electrolyte secondary battery
JP2021545210A JP7608345B2 (ja) 2019-09-09 2020-08-28 非水電解質二次電池用正極活物質、及び非水電解質二次電池
JP2024221414A JP7751719B2 (ja) 2019-09-09 2024-12-18 非水電解質二次電池用正極活物質、及び非水電解質二次電池
JP2025159924A JP2025175191A (ja) 2019-09-09 2025-09-26 非水電解質二次電池用正極活物質の製造方法

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JP2019163571 2019-09-09
JP2019-163571 2019-09-09

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US (1) US20220320490A1 (https=)
EP (2) EP4030508B1 (https=)
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WO (1) WO2021049318A1 (https=)

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US20220320490A1 (en) 2022-10-06
CN114342116B (zh) 2024-06-25
JP7608345B2 (ja) 2025-01-06
EP4618192A2 (en) 2025-09-17
JP7751719B2 (ja) 2025-10-08
EP4030508A4 (en) 2022-11-09
EP4030508A1 (en) 2022-07-20
JP2025028269A (ja) 2025-02-28
JP2025175191A (ja) 2025-11-28
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