WO2020171088A1 - リチウムイオン二次電池用正極活物質の製造方法、リチウムイオン二次電池用正極活物質、リチウムイオン二次電池 - Google Patents

リチウムイオン二次電池用正極活物質の製造方法、リチウムイオン二次電池用正極活物質、リチウムイオン二次電池 Download PDF

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Publication number
WO2020171088A1
WO2020171088A1 PCT/JP2020/006360 JP2020006360W WO2020171088A1 WO 2020171088 A1 WO2020171088 A1 WO 2020171088A1 JP 2020006360 W JP2020006360 W JP 2020006360W WO 2020171088 A1 WO2020171088 A1 WO 2020171088A1
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Prior art keywords
lithium
positive electrode
active material
electrode active
composite oxide
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Ceased
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PCT/JP2020/006360
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English (en)
French (fr)
Japanese (ja)
Inventor
鈴木　淳
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Sumitomo Metal Mining Co Ltd
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Sumitomo Metal Mining Co Ltd
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Priority to US17/432,163 priority Critical patent/US12227431B2/en
Priority to CN202080015165.XA priority patent/CN113454813A/zh
Priority to JP2021502048A priority patent/JP7691181B2/ja
Publication of WO2020171088A1 publication Critical patent/WO2020171088A1/ja
Anticipated expiration legal-status Critical
Priority to JP2024101609A priority patent/JP2024123191A/ja
Priority to US19/016,356 priority patent/US20250145491A1/en
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
    • 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
    • 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
    • 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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0471—Processes of manufacture in general involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis
    • 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
    • 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
    • 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
    • C01P2004/01—Particle morphology depicted by an image
    • C01P2004/03—Particle morphology depicted by an image obtained by SEM
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/30—Particle morphology extending in three dimensions
    • C01P2004/45—Aggregated particles or particles with an intergrown morphology
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/40—Electric properties
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/80—Compositional purity
    • C01P2006/82—Compositional purity water content
    • 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
    • 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 element M can be at least one element selected from Mn, V, Mg, Mo, Nb, Ti, Co and Al. Further, the above y is more preferably 0.97 ⁇ y ⁇ 1.15.
  • the lithium nickel composite oxide is preferably a compound having a layered structure, that is, a layered compound.
  • the dissolved tungsten compound may have an amount capable of penetrating to the surface of the primary particles inside the secondary particles of the lithium nickel composite oxide. Therefore, for example, when the tungsten compound is excessively added, after mixing, further, A part may be in a solid state after heating.
  • the temperature for heating in the mixing process is not particularly limited.
  • the mixing temperature in the mixing step is, for example, preferably 30°C or higher and 65°C or lower, more preferably 45°C or higher and 60°C or lower, and further preferably 50°C or higher and 60°C or lower.
  • the atmosphere of the mixing step is preferably exhausted in order to discharge the water generated from the lithium nickel composite oxide.
  • the speed of the exhaust is not particularly limited, the mixed input rate (input amount) of the lithium nickel composite oxide to Step 1 kg / min, mixed with 0.15 m 3 / min or more 0.30 m 3 / min or less speed It is preferable to exhaust the atmosphere.
  • the method of calculating the proportion of segregated particles among the plurality of composite particles included in the positive electrode active material of the present embodiment is not particularly limited, but the positive electrode active material is magnified at a magnification of 10 times or more and 1000 times or less by a scanning electron microscope, for example. By observing from 3 visual fields to 20 visual fields, the ratio of segregated particles in the composite particles in the images obtained can be calculated.
  • the observation conditions of the scanning electron microscope are not particularly limited, but for example, the acceleration voltage is preferably 1 kV or more and 20 kV or less.
  • the particle size of the compound containing tungsten and lithium By setting the particle size of the compound containing tungsten and lithium to 1 nm or more, particularly sufficient lithium ion conductivity can be exhibited. Further, by setting the particle size of the compound containing tungsten and lithium to 300 nm or less, the particles of the compound containing tungsten and lithium can be formed particularly uniformly on the surface of the particles of the lithium nickel composite oxide, and the reaction resistance can be improved. Especially, it can be reduced.
  • the mixing ratio of each material in the positive electrode mixture is a factor that determines the performance of the lithium-ion secondary battery, so it can be adjusted according to the application.
  • the mixing ratio of the materials can be the same as that of the positive electrode of a known lithium ion secondary battery.
  • the positive electrode active material when the total mass of the solid content of the positive electrode mixture excluding the solvent is 100% by mass, the positive electrode active material is It may be contained in an amount of 60% by mass or more and 95% by mass or less, a conductive material in an amount of 1% by mass or more and 20% by mass or less, and a binder in a ratio of 1% by mass or more and 20% by mass or less.
  • the positive electrode active material it is possible to disperse the positive electrode active material, the conductive material, etc., and add a solvent that dissolves the binder to the positive electrode mixture.
  • a solvent specifically, an organic solvent such as N-methyl-2-pyrrolidone can be used.
  • activated carbon may be added to the positive electrode mixture to increase the electric double layer capacity.
  • the electrode 13 includes a positive electrode 13a, a separator 13c, and a negative electrode 13b, which are stacked in this order.
  • the positive electrode 13a contacts the inner surface of the positive electrode can 12a through a current collector 14, and the negative electrode 13b is the negative electrode. It is housed in the case 12 so as to come into contact with the inner surface of the can 12 b via the current collector 14.
  • the current collector 14 is also arranged between the positive electrode 13a and the separator 13c.
  • the amount of tungsten which is the ratio of the number of W atoms to the total number of Ni, Co, and Al atoms, was evaluated using ICP.
  • the amount of tungsten in the obtained positive electrode active material is the same as the amount of W, which is the ratio of the number of W atoms to the total number of atoms of Ni, Co, and Al of the base material in the starting raw material subjected to the mixing step. It has been confirmed that they are equal.
  • Table 1 shows the test conditions and the evaluation results.
  • the composition of the base material was Li 0.97 Ni 0.91 Co 0.04 Al 0.05 O 2 and the moisture content was 4.9 mass %, and W with respect to the total number of atoms of Ni, Co, and Al of the base material WO 3 was added so that the ratio of the number of atoms was 0.18 atom %, the mixing temperature was 30° C., the mixing time was 60 minutes, the heat treatment temperature was 175° C., and the heat treatment time was 150 minutes.
  • decarbonated air was supplied while exhausting the inside of the mixing apparatus.
  • Table 1 shows the test conditions and the evaluation results.
  • Comparative Example 2 Except that WO 3 was added so that the water content was 2.7 mass% and the ratio of the number of W atoms to the total number of Ni, Co, and Al atoms of the base material was 0.15 atom %.
  • a positive electrode active material and a secondary battery were prepared in the same manner as in Example 1 and evaluated.
  • the positive electrode active material of the present embodiment has a high capacity and a high output at a low cost.
  • the evaluation results were good, the productivity was high, and a further large cost reduction can be expected.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
PCT/JP2020/006360 2019-02-21 2020-02-18 リチウムイオン二次電池用正極活物質の製造方法、リチウムイオン二次電池用正極活物質、リチウムイオン二次電池 Ceased WO2020171088A1 (ja)

Priority Applications (5)

Application Number Priority Date Filing Date Title
US17/432,163 US12227431B2 (en) 2019-02-21 2020-02-18 Method of manufacturing positive electrode active material for lithium ion secondary battery, positive electrode active material for lithium ion secondary battery, and lithium ion secondary battery
CN202080015165.XA CN113454813A (zh) 2019-02-21 2020-02-18 锂离子二次电池用正极活性物质的制造方法、锂离子二次电池用正极活性物质、锂离子二次电池
JP2021502048A JP7691181B2 (ja) 2019-02-21 2020-02-18 リチウムイオン二次電池用正極活物質の製造方法、リチウムイオン二次電池用正極活物質、リチウムイオン二次電池
JP2024101609A JP2024123191A (ja) 2019-02-21 2024-06-25 リチウムイオン二次電池用正極活物質の製造方法
US19/016,356 US20250145491A1 (en) 2019-02-21 2025-01-10 Positive electrode active material for lithium ion secondary battery and lithium ion secondary battery

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2019029870 2019-02-21
JP2019-029870 2019-02-21

Related Child Applications (2)

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US17/432,163 A-371-Of-International US12227431B2 (en) 2019-02-21 2020-02-18 Method of manufacturing positive electrode active material for lithium ion secondary battery, positive electrode active material for lithium ion secondary battery, and lithium ion secondary battery
US19/016,356 Division US20250145491A1 (en) 2019-02-21 2025-01-10 Positive electrode active material for lithium ion secondary battery and lithium ion secondary battery

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CN113454813A (zh) 2021-09-28
JPWO2020171088A1 (ja) 2021-12-16
US12227431B2 (en) 2025-02-18
JP7691181B2 (ja) 2025-06-11
JP2024123191A (ja) 2024-09-10
TWI822956B (zh) 2023-11-21
TW202044650A (zh) 2020-12-01
US20250145491A1 (en) 2025-05-08

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