WO2021141013A1 - 粒子の製造方法 - Google Patents

粒子の製造方法 Download PDF

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Publication number
WO2021141013A1
WO2021141013A1 PCT/JP2021/000054 JP2021000054W WO2021141013A1 WO 2021141013 A1 WO2021141013 A1 WO 2021141013A1 JP 2021000054 W JP2021000054 W JP 2021000054W WO 2021141013 A1 WO2021141013 A1 WO 2021141013A1
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Prior art keywords
dispersion medium
particles
layered compound
producing particles
particles according
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Ceased
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PCT/JP2021/000054
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English (en)
French (fr)
Japanese (ja)
Inventor
拓也 工藤
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Sekisui Chemical Co Ltd
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Sekisui Chemical Co Ltd
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Application filed by Sekisui Chemical Co Ltd filed Critical Sekisui Chemical Co Ltd
Priority to US17/790,878 priority Critical patent/US20230299270A1/en
Priority to JP2021510237A priority patent/JP7813579B2/ja
Priority to KR1020227022432A priority patent/KR20220123651A/ko
Priority to CN202180008588.3A priority patent/CN114981210A/zh
Priority to EP21738703.4A priority patent/EP4089049A4/en
Publication of WO2021141013A1 publication Critical patent/WO2021141013A1/ja
Anticipated expiration legal-status Critical
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
    • H01M4/366—Composites as layered products
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/20—Graphite
    • C01B32/21—After-treatment
    • 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
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B33/00—Silicon; Compounds thereof
    • C01B33/02—Silicon
    • 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
    • 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
    • C01P2004/86—Thin layer coatings, i.e. the coating thickness being less than 0.1 time the particle radius
    • 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
    • C01P2006/10—Solid density
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    • 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
    • H—ELECTRICITY
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    • 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
    • H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • 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
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/387—Tin or alloys based on tin
    • 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
    • H01M4/36—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
    • H01M4/483—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides for non-aqueous cells
    • 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
    • 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
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
    • 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 present invention relates to a method for producing particles, comprising a particle body and a coating layer covering at least a part of the particle body.
  • a compound such as graphene obtained by peeling a layered compound has attracted attention from its conductivity and environmental aspects.
  • Patent Document 1 discloses a battery electrode containing a graphene-encapsulating or graphene-encapsulating electrode active material.
  • Patent Document 1 when producing a graphene-containing or graphene-encapsulated electrode active material, in the first step, a plurality of particles of a graphite material and a plurality of particles of a solid electrode active material are mixed in a collision chamber of an energy collision device. The mixture is formed. At this time, the graphite material has not been intercalated, oxidized, and peeled in advance. In addition, it does not contain a ball mill pulverization medium other than a plurality of particles of the solid electrode active material.
  • the energy collision device is operated to peel the graphene sheet from the particles of the graphite material, move the peeled graphene sheet to the surface of the solid electrode active material particles, and completely enclose or enclose the particles.
  • the energy collision device is operated to peel the graphene sheet from the particles of the graphite material, move the peeled graphene sheet to the surface of the solid electrode active material particles, and completely enclose or enclose the particles.
  • the peeling force of the graphite material is weak, and the surface of the solid electrode active material particles may not be uniformly coated. Therefore, the graphene compound obtained by the production method of Patent Document 1 is still not sufficiently conductive, and when used as an electrode material for a secondary battery, for example, the battery has characteristics such as rate characteristics and cycle characteristics of the secondary battery. There is a problem that the characteristics cannot be sufficiently improved.
  • An object of the present invention is to provide a method for producing particles, which can easily produce particles having excellent conductivity.
  • the method for producing particles according to the present invention is a method for producing particles comprising a particle body and a coating layer covering at least a part of the particle body, wherein the particle body, a layered compound, and a dispersion medium are provided.
  • the viscosity of the dispersion medium at 25 ° C. is 1 mPa ⁇ s or more.
  • the dispersion medium is in the form of a sol, a gel, or a liquid.
  • the dispersion medium contains a dispersion medium having an SP value of 5 or more and 20 or less.
  • the dispersion medium contains a solvent having a molecular weight of 40 or more.
  • the layered compound comprises graphite or graphite oxide.
  • the layered compound comprises boron nitride or a graphite-like layered compound.
  • the average particle size of the particle body is 20 ⁇ m or less.
  • the true density of the particle body is 0.8 g / cm 3 or more.
  • the particle body is a metal or a metal compound.
  • the shearing force is applied by at least one method selected from the group consisting of ball mills, agitation, ultrasonic waves, high pressure release, and planetary agitation. ..
  • the layered compound is peeled off and the layered compound is peeled off by applying the shearing force in a state where the mixture is cooled to increase the viscosity. Is coated on the particle body.
  • a step of removing the dispersion medium is further provided after the step of forming the coating layer.
  • the dispersion medium in the step of removing the dispersion medium, is removed by solid-liquid separation or volatilization by heating or reduced pressure.
  • a step of carbonizing the dispersion medium by heating is further provided after the step of forming the coating layer.
  • a step of removing the carbonized dispersion medium is further provided.
  • FIG. 1A to 1C are schematic views for explaining an example of a method for producing particles according to the present invention.
  • FIG. 2 is a schematic cross-sectional view showing an example of particles produced by the method for producing particles according to the present invention.
  • FIG. 3 is a diagram showing the results of thermogravimetric analysis and measurement of particles before removing amorphous carbon in Example 1.
  • FIG. 4 is a diagram showing the results of thermogravimetric analysis and measurement of particles before removing amorphous carbon in Example 2.
  • FIG. 5 is a diagram showing the results of thermogravimetric analysis and measurement of particles before removing amorphous carbon in Example 3.
  • FIG. 6 is a diagram showing the results of thermogravimetric analysis and measurement of particles before removing amorphous carbon in Example 4.
  • FIG. 1A to 1C are schematic views for explaining an example of a method for producing particles according to the present invention.
  • FIG. 2 is a schematic cross-sectional view showing an example of particles produced by the method for producing particles according to the present invention.
  • FIG. 7 is a diagram showing the results of thermogravimetric analysis and measurement of particles after removing amorphous carbon in Example 1.
  • FIG. 8 is a diagram showing the results of thermogravimetric analysis and measurement of particles after removing amorphous carbon in Example 2.
  • FIG. 9 is a diagram showing the results of thermogravimetric analysis and measurement of particles after removing amorphous carbon in Example 3.
  • FIG. 10 is a diagram showing the results of thermogravimetric analysis and measurement of particles after removing amorphous carbon in Example 4.
  • FIG. 11 is a diagram showing the results of thermogravimetric analysis measurement of the particles of Comparative Example 1.
  • FIG. 12 is a diagram showing the results of thermogravimetric analysis measurement of the particles of Comparative Example 2.
  • FIG. 12 is a diagram showing the results of thermogravimetric analysis measurement of the particles of Comparative Example 2.
  • FIG. 13 is a diagram showing the results of thermogravimetric analysis measurement of the particles of Comparative Example 3.
  • FIG. 14 is a diagram showing the results of thermogravimetric analysis measurement of the particles of Comparative Example 4.
  • FIG. 15 is a diagram showing a transmission electron micrograph of the particles obtained in Example 4 before removing amorphous carbon.
  • FIG. 16 is a diagram showing a transmission electron micrograph of the particles obtained in Example 4 after removing amorphous carbon.
  • particles are produced, comprising a particle body and a coating layer covering at least a part of the particle body.
  • the particles of the present invention can be obtained by peeling off the layered compound and coating the particle body with the layered compound to form a coating layer.
  • the viscosity of the dispersion medium at 25 ° C. is 1 mPa ⁇ s or more.
  • water has a viscosity of 0.88 mPa ⁇ s at 25 ° C.
  • the viscosity of the dispersion medium is 1 mPa ⁇ s or more
  • the layered compound can be easily peeled off by simply applying a shearing force to the mixture, and the layered compound can be used as the particle body. Can be coated on. Therefore, the particles of the present invention can be easily produced without requiring complicated steps.
  • the above-mentioned manufacturing process can be performed in a non-oxidizing environment, the conductivity of the obtained particles can be enhanced.
  • the particles obtained by the production method of the present invention are excellent in conductivity as described above, they can be suitably used as an electrode material for a power storage device or the like. Among them, it can be suitably used as a positive electrode active material or a negative electrode active material constituting an electrode of a power storage device.
  • the particles obtained by the production method of the present invention as an electrode material of a power storage device, characteristics such as cycle characteristics due to charging and discharging can be improved.
  • the shape of the particle body is not particularly limited, and for example, a spherical shape, a substantially spherical shape, a scaly shape, a planar shape, an elliptical shape, a substantially elliptical shape, or the like can be used. Further, in addition to the above shape, a structure having a hollow or porous structure inside can also be used. Of these, a spherical shape or a substantially spherical shape is preferable.
  • the average particle size of the particle body is not particularly limited. However, the average particle size of the particle body is preferably 10 nm or more, more preferably 50 nm or more, preferably 20 ⁇ m or less, more preferably 10 ⁇ m or less, still more preferably 5 ⁇ m or less. When the average particle size of the particle body is within the above range, the layered compound can be more easily peeled off and the layered compound can be more reliably coated on the particle body.
  • the average particle size refers to a value calculated by a volume reference distribution using a particle size distribution measuring device by a dynamic light scattering method or a particle size distribution measuring device by a laser diffraction method.
  • the true density of the particle body is not particularly limited, but is preferably 0.8 g / cm 3 or more, and more preferably 2 g / cm 3 or more. In this case, the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the upper limit of the true density of the particle body is not particularly limited, but may be, for example, 20 g / cm 3 .
  • the particle body is not particularly limited, and examples thereof include a metal or a metal compound, a semiconductor or a semiconductor compound, and a sulfur or a sulfur compound.
  • the particle body is a particle capable of storing and releasing an alkali metal ion or an alkaline earth metal ion.
  • the alkali metal ion include lithium ion, sodium ion, and potassium ion.
  • alkaline earth metals include calcium ions and magnesium ions.
  • metal or metal compound examples include Mg, Al, Ca, Sc, Ti, V, Mn, Fe, Co, Ni, Cu, Zn, Ga, Sr, Y, Zr, Nb, Mo, Tc, Ru, Pd. , Ag, Cd, In, Sn, Ba, Hf, Ta, W, Re, Os, Ir, Pt, Au, Hg, Tl, Pb, or compounds thereof.
  • As the semiconductor or semiconductor compound for example, Si, P, Ge, As, Se, Sb, Te, Bi, Po, or a compound thereof can be used.
  • examples of the particle body include Si, Si compounds, Sn, Sn compounds and the like.
  • examples of the Si compound include alloys of Si and other metals, Si oxides such as SiO and SiO 2.
  • examples of the Sn compound include alloys of Sn and other metals, Sn oxides such as SnO and SnO 2, and the like. In this case, characteristics such as the capacity of the power storage device can be further enhanced.
  • One type of these metals or metal compounds may be used alone, or a plurality of types may be used in combination.
  • the particles When the particles are used as the positive electrode active material (LiB positive electrode active material) of the lithium ion secondary battery, examples of the particle body include lithium metal oxide, lithium sulfide, nickel compound, sulfur and the like. ..
  • lithium metal oxide examples include a layered rock salt type compound, a spinel type structure compound, an olivine type structure compound, or a mixture thereof.
  • Examples of the compound having a layered rock salt structure include lithium cobalt oxide and lithium nickel oxide.
  • Examples of the compound having a spinel-type structure include lithium manganate and the like.
  • Examples of the compound having an olivine type structure include lithium iron phosphate and the like.
  • the particle body is preferably lithium cobalt oxide.
  • the particle body may be a granulated body in which a plurality of particles are bonded.
  • the granulated body for example, nickel, manganese, and cobalt ternary Li (NiMnCo) O 2 (NMC) can be used.
  • the content of the particle body in the mixture is preferably 1% by weight or more and 50% by weight or less.
  • the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the layered compound is not particularly limited, and for example, graphite, graphite oxide, boron nitride, graphite-like layered compound (BC2N) and the like can be used. These layered compounds may be used alone or in combination of two or more. Among them, when the layered compound is used in a secondary battery such as a lithium ion secondary battery (LiB), it preferably contains graphite, and more preferably graphite. In this case, the conductivity of the obtained particles can be further increased. On the other hand, it is preferable to use an insulating layered compound such as boron nitride for applications such as heat conductive sheets that require insulating properties.
  • a secondary battery such as a lithium ion secondary battery (LiB)
  • LiB lithium ion secondary battery
  • it preferably contains graphite, and more preferably graphite. In this case, the conductivity of the obtained particles can be further increased.
  • an insulating layered compound such as boron n
  • Graphite is a laminate of multiple graphene sheets.
  • the number of laminated graphene sheets of graphite is usually about 100,000 to 1,000,000.
  • As the graphite for example, natural graphite, artificial graphite, expanded graphite or the like can be used.
  • a laminated body of a sheet-like material can be used as the layered compound.
  • the content of the layered compound in the mixture is preferably 0.01% by weight or more and 30% by weight or less.
  • the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the viscosity of the dispersion medium at 25 ° C. is 1 mPa ⁇ s or more, preferably 1.5 mPa ⁇ s or more, and more preferably 10 mPa ⁇ s or more.
  • the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the upper limit of the viscosity of the dispersion medium at 25 ° C. can be, for example, 10,000,000 mPa ⁇ s.
  • the viscosity of the dispersion medium can be measured under the condition of 25 ° C. using, for example, an E-type viscometer (TV-25 Type-H viscometer manufactured by Toki Sangyo Co., Ltd.).
  • the form of the dispersion medium may be any of a sol form, a gel form, and a liquid form.
  • the dispersion medium is not particularly limited, but for example, polyethylene glycol, polypropylene glycol, sucrose, polyvinyl alcohol, vinyl acetate, polystyrene, polyamine, silicon oil, carboxymethyl cellulose, water, ethanol, methanol, propanol, dimethylformamide and the like may be used. Can be done.
  • One of these dispersion media may be used alone, or a plurality of types may be used in combination. Further, these dispersion media may be in the state of a solution in which the solute is dissolved in a solvent such as water. In this case, the viscosity of the dispersion medium indicates the viscosity of the solution.
  • an aqueous sucrose solution can be used as the dispersion medium
  • the viscosity of the 20% sucrose aqueous solution at 25 ° C. is 1.68 mPa ⁇ s
  • the viscosity of the 50% sucrose aqueous solution at 25 ° C. is 12. It is .98 mPa ⁇ s.
  • the SP value of the dispersion medium is not particularly limited, but is preferably 5 or more, more preferably 8 or more, preferably 20 or less, and more preferably 18 or less.
  • the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the SP value is a measure of affinity between substances.
  • the SP value can be obtained based on Hidebrand's theory of regular solution.
  • the unit of the SP value is (cal / cm 3 ) 0.5 .
  • the Fedors method is described in the Journal of the Japan Adhesive Society, Vol. 22, 1986, p. 566.
  • the molecular weight of the dispersion medium is not particularly limited, but is preferably 20 or more, more preferably 40 or more. As a result, the viscosity of the dispersion medium is increased, the layered compound can be more easily peeled off, and the layered compound can be more reliably coated on the particle body.
  • the upper limit of the molecular weight of the dispersion medium is not particularly limited, but may be, for example, 10,000.
  • the dispersion medium is a mixed solvent of a plurality of solvents or a solution in which a solute is dissolved in the solvent, the molecular weight is weighted and averaged by the compounding ratio.
  • the content of the dispersion medium in the mixture is not particularly limited, but is preferably 100 parts by weight or more with respect to 100 parts by weight of the charged weight of the layered compound because it is used when peeling the layered compound. As a result, the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the content of the dispersion medium in the mixture is preferably 500 parts by weight or less with respect to 100 parts by weight of the charged weight of the particle body. In this case, wasteful use of the dispersion medium can be reduced, and coated particles can be obtained more efficiently.
  • the coating layer forming step a shearing force is applied to the mixture obtained in the above-mentioned mixing preparation step. Thereby, the layered compound is peeled off, and the layered compound is coated on the particle body to form a coating layer.
  • the peeled product obtained by peeling the layered compound may be coated on the particle body, or the layered compound coated on the particle body may be peeled off. Alternatively, both may be used. By either method, a coating layer containing a stripped product of the layered compound can be formed. Further, the coating layer may contain a layered compound before peeling.
  • the method of applying a shearing force to the mixture is not particularly limited, but for example, a method such as a ball mill, stirring, ultrasonic waves, high pressure release, or planetary stirring can be used. Of these, planetary agitation is preferable. In this case, the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • a method such as a ball mill, stirring, ultrasonic waves, high pressure release, or planetary stirring can be used.
  • planetary stirring is preferable.
  • the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • one kind of method may be used alone, or a plurality of kinds of methods may be used in combination.
  • the viscosity of the dispersion medium When applying a shearing force to the mixture, the viscosity of the dispersion medium may be increased while cooling, and the shearing force may be applied. In this case, even if a dispersion medium having a low viscosity at room temperature is used, the layered compound can be easily peeled off and the layered compound can be more reliably coated on the particle body, and the dispersion medium is removed in a later step. At that time, it becomes easier to remove the dispersion medium. Further, when applying a shearing force to the mixture, the viscosity of the dispersion medium may be lowered while heating, and the shearing force may be applied.
  • a highly viscous dispersion medium can be used at room temperature, the layered compound can be more easily peeled off, and the layered compound can be more reliably coated on the particle body.
  • the temperature at the time of cooling or heating depends on the type of the dispersion medium, but can be, for example, ⁇ 30 ° C. or higher and 200 ° C. or lower.
  • the viscosity of the dispersion medium at the temperature at the time of cooling or heating is preferably 1 mPa ⁇ s or more, more preferably 1.5 mPa ⁇ s or more, and particularly preferably 10 mPa ⁇ s. That is all.
  • the layered compound can be peeled off more easily, and the layered compound can be more reliably coated on the particle body.
  • the viscosity of the dispersion medium at the temperature at the time of cooling or heating is preferably 10,000,000 mPa ⁇ s or less, more preferably 1,000,000 mPa ⁇ s. It is as follows. In this case, it becomes easier to apply a shearing force to the mixture.
  • the dispersion medium may be removed after the particle body is coated with the layered compound.
  • the dispersion medium can be removed by, for example, solid-liquid separation or volatilization by heating or reduced pressure.
  • the heating may be performed in the atmosphere or in an atmosphere of an inert gas such as nitrogen gas.
  • the dispersion medium may be carbonized by heating after the particle body is coated with the layered compound.
  • a coating layer containing a stripped product of amorphous carbon and a layered compound may be used.
  • the heating temperature can be, for example, 200 ° C. or higher and 600 ° C. or lower.
  • the heating time can be 20 minutes or more and 480 minutes or less.
  • the heating may be performed in the atmosphere or in an atmosphere of an inert gas such as nitrogen gas.
  • the carbonized dispersion medium may be further removed by heating. Thereby, the conductivity of the obtained particles can be further increased.
  • the heating temperature can be, for example, 300 ° C. or higher and 800 ° C. or lower.
  • the heating time can be 10 minutes or more and 300 minutes or less. It is preferable that the heating is performed under the condition that the carbonized dispersion medium (amorphous carbon) is burnt and the exfoliated material of the layered compound is not burned. For example, it may be carried out in the atmosphere under conditions such as 500 ° C. and 30 minutes.
  • 1 (a) to 1 (c) are schematic views for explaining an example of the method for producing particles according to the present invention.
  • the particle body 2, the layered compound 11, and the dispersion medium 12 are added to the container 10 to prepare a mixture.
  • the layered compound 11 may be used as it is, or may be pulverized and classified by a ball mill, a feather mill, ultrasonic waves, a pulverizing classifier, a sieve or the like.
  • the mixture is rotated and revolved together with the balls 13 shown in FIG. 1 (b) to rotate and mix.
  • the balls 13 apply a shearing force to the mixture.
  • the layered compound 11a and the dispersion medium 12 are attached to the surface of the particle body 2 while the layered compound 11 is peeled off.
  • a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") can be used.
  • the rotation speed can be, for example, 400 rpm or more and 2000 rpm or less.
  • the rotation time can be, for example, 5 minutes or more and 600 minutes or less.
  • a seramic ball can be used as the ball 13.
  • a zirconia ball is used as the ball 13.
  • the particle body 2 to which the stripped material 11a of the layered compound and the dispersion medium 12 are attached is taken out from the container 10. Subsequently, the particle body 2 on which the stripped material 11a of the layered compound and the dispersion medium 12 adhered to the surface is heated at a temperature of 200 ° C. or higher and 600 ° C. or lower in a nitrogen atmosphere to carbonize the dispersion medium 12 and form amorphous carbon. To form. Thereby, particles having a coating layer containing a stripped product 11a of the layered compound and amorphous carbon can be obtained.
  • the amorphous carbon in the coating layer may be removed by further heating the obtained particles at a temperature of 300 ° C. or higher and 800 ° C. or lower in an air atmosphere. Thereby, the conductivity of the particles can be further increased.
  • the layered compound is peeled off by mechanical treatment. Therefore, it does not include an oxidation step of the layered compound as in the case where the layered compound is peeled off by a chemical treatment. Therefore, particles having excellent conductivity can be obtained.
  • FIG. 2 is a schematic cross-sectional view showing an example of particles produced by the method for producing particles according to the present invention.
  • the particle 1 includes a particle body 2 and a coating layer 3.
  • a coating layer 3 is provided so as to cover the surface 2a of the particles 2.
  • the coating layer 3 may cover the entire surface 2a of the particle body 2 or a part of the surface 2a as in the present embodiment.
  • the coating layer 3 covers at least a part of the surface 2a of the particle body 2.
  • the coating layer 3 preferably covers 20% or more of the surface 2a of the particle body 2, more preferably 90% or more, further preferably 95% or more, and 98% or more. It is particularly preferable to cover the particles, and it is most preferable to completely cover the particles. In this case, the conductivity of the particles can be further improved.
  • whether or not the surface of the particle body is covered with the coating layer can be confirmed by a scanning electron microscope (SEM), a transmission electron microscope (TEM), or the like.
  • SEM scanning electron microscope
  • TEM transmission electron microscope
  • energy dispersive X-ray spectroscopy SEM-EDX, TEM-EDX
  • C element carbon element
  • the particle body is a particle such as Si particle that reacts with oxygen to form an oxide
  • the thermal weight analysis of the particle is performed under the conditions of an air atmosphere and a heating rate of 10 ° C./min.
  • the presence or absence of coating depends on whether or not the weight increase start temperature, which is an index of the temperature at which oxidation starts when Si, which is the main body of the particle reacts with oxygen in the air, which is the measurement gas, shifts to 600 ° C or higher. You may check.
  • thermogravimetric analysis can be measured using a thermogravimetric / calorific value simultaneous measuring device (manufactured by Hitachi High-Tech Science Corporation, product number "TGDTA6300").
  • the thermogravimetric analysis is measured under the following conditions.
  • Atmosphere Air atmosphere Temperature rise rate: 10 ° C / min Temperature range: 40 ° C to 1000 ° C
  • the weight increase start temperature of the obtained particles is preferably 600 ° C. or higher, more preferably 700 ° C. or higher, and preferably 900 ° C. or lower.
  • the coating layer can be used for more uniform coating, and the conductivity of the particles can be further increased.
  • the weight increase start temperature of the particles is not more than the upper limit value, the thickness of the coating layer is unlikely to increase. Therefore, when used as an electrode material for a power storage device, ions such as lithium ions can be occluded and released more smoothly, and characteristics such as cycle characteristics due to charging and discharging can be further improved.
  • the thickness of the coating layer is preferably 0.1 nm or more, more preferably 1 nm or more, preferably 20 nm or less, and more preferably 10 nm or less.
  • the conductivity of the particles can be further increased.
  • the film thickness of the coating layer is not more than the above upper limit value, ions such as lithium ions can be occluded and released more smoothly when used as an electrode material of a power storage device, and a cycle by charging and discharging can be performed. Characteristics such as characteristics can be further improved.
  • the thickness of the coating layer can be obtained from the average value of the thickness of the coating layer of any three particles observed by a transmission electron micrograph (TEM photograph).
  • the coating layer contains exfoliated material of the layered compound. Therefore, the particles are particles coated with exfoliated material of the layered compound.
  • the exfoliated product of the layered compound may be flaky graphite.
  • the flaky graphite is obtained by exfoliating the original graphite, and refers to a graphene sheet laminate thinner than the original graphite.
  • the number of graphene sheets laminated in the flaky graphite may be smaller than that of the original graphite.
  • the number of laminated sheets such as graphene sheets is not particularly limited, but is preferably 1 layer or more, more preferably 3 layers or more, preferably 100 layers or less, and more preferably 10 layers or less.
  • the conductivity of the particles can be further increased.
  • the number of laminated sheets is less than or equal to the above upper limit, ions such as lithium ions can be occluded and released more smoothly when used as an electrode material for a power storage device, and cycle characteristics due to charge and discharge can be obtained. The characteristics can be further improved.
  • the content of the exfoliated material of the layered compound in the coating layer is preferably 0.01% by weight or more, more preferably 0.1% by weight or more, preferably 30% by weight, based on 100% by weight of the material constituting the coating layer. Hereinafter, it is more preferably 5% by weight or less.
  • the conductivity of the particles can be further improved.
  • the coating layer may further contain a layered compound as a raw material.
  • the content of the layered compound in the coating layer can be, for example, 0.01% by weight or more and 10% by weight or less with respect to 100% by weight of the material constituting the coating layer.
  • the coating layer may further contain amorphous carbon.
  • the surface of the particle body can be coated even more uniformly.
  • the content of amorphous carbon in the coating layer can be, for example, 1% by weight or more and 30% by weight or less with respect to 100% by weight of the material constituting the coating layer.
  • the particles obtained by the method for producing particles according to the present invention are uniformly coated with a stripped material of a layered compound having excellent conductivity, and therefore, for example, when used as a negative electrode active material of a secondary battery.
  • the volume change due to charging and discharging can be reduced, and the negative electrode active material can be prevented from cracking or peeling off from the electrode.
  • the coating layer in the particles obtained by the production method of the present invention contains a stripped product of the layered compound. Therefore, the thickness of the coating layer does not become too thick, and ions such as lithium ions can be smoothly occluded and released. Therefore, the particles obtained in the present invention can improve characteristics such as cycle characteristics when used as an electrode material for a power storage device.
  • Example 1 1.2 g of graphite as a layered compound (manufactured by Toyo Carbon Co., Ltd., product number "PF8”), polyethylene glycol as a dispersion medium (manufactured by Sanyo Kasei Co., Ltd., product number "PEG600", viscosity: 106 mPa ⁇ s (25 ° C.), molecular weight: 600, SP value: 9.4) 23.4 g and water (viscosity: 0.88 mPa ⁇ s (25 ° C.), molecular weight: 18, SP value: 23.4) were dispersed in a mixed solvent of 23.0 g.
  • the prepared mixture was placed in a zirconia container of a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") together with 2 mm zirconia balls (2.5 g), and the mixture was mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. It was. After mixing, the removed particles were heated at 420 ° C. for 1 hour in a nitrogen atmosphere. As a result, particles in which the surface of Si particles was coated with flaky graphite and amorphous carbon were obtained.
  • the obtained particles were heated at 500 ° C. for 10 minutes in an air atmosphere. As a result, amorphous carbon was removed to obtain particles in which the surface of Si particles was coated with flaky graphite.
  • Example 2 1 g of graphite as a layered compound (manufactured by Toyo Carbon Co., Ltd., product number "PF8"), 20 wt% sucrose water as a dispersion medium (manufactured by Fuji Film Wako Pure Chemical Industries, Ltd., prepared by dissolving a predetermined amount of reagent special grade sucrose in water) 234 g
  • a mixture of graphite and a dispersion medium was obtained by dispersing the mixture in the mixture and stirring the mixture with a stirrer (“PRIMIX2” manufactured by Primix) under the conditions of a rotation speed of 11000 rpm and a stirring time of 30 minutes.
  • the viscosity of the dispersion medium was measured at 25 ° C. using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd., trade name "TV-25 Type-H", spindle No. 1) and 1.68 mPa. ⁇ It was s.
  • the prepared mixture was placed in a container of a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") together with 2 mm zirconia balls (2.5 g), and the mixture was mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. After mixing, the removed particles were heated at 250 ° C. for 1 hour in a nitrogen atmosphere. As a result, particles in which the surface of Si particles was coated with flaky graphite and amorphous carbon were obtained.
  • the obtained particles were heated at 550 ° C. for 10 minutes in an air atmosphere. As a result, amorphous carbon was removed to obtain particles in which the surface of Si particles was coated with flaky graphite.
  • Example 3 1 g of graphite (manufactured by Toyo Tanso Co., Ltd., product number "PF8") as a layered compound in 50 wt% sucrose water as a dispersion medium (manufactured by Fuji Film Wako Pure Chemical Industries, Ltd., prepared by dissolving a predetermined amount of reagent special grade sucrose in water)
  • a mixture of graphite and a dispersion medium was obtained by dispersing in 234 g and stirring with a stirrer (“PRIMIX 2” manufactured by Primix) under the conditions of a rotation speed of 11000 rpm and a stirring time of 30 minutes.
  • the viscosity of the dispersion medium was measured at 25 ° C. using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd., trade name "TV-25 Type-H", spindle No. 1), and was 12.98 mPa. ⁇ It was s.
  • the prepared mixture was placed in a container of a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") together with 2 mm zirconia balls (2.5 g), and the mixture was mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. After mixing, the removed particles were heated at 250 ° C. for 1 hour in a nitrogen atmosphere. As a result, particles in which the surface of Si particles was coated with flaky graphite and amorphous carbon were obtained.
  • the obtained particles were heated at 600 ° C. for 10 minutes in an air atmosphere. As a result, amorphous carbon was removed to obtain particles in which the surface of Si particles was coated with flaky graphite.
  • Example 4 1 g of graphite as a layered compound (manufactured by Toyo Tanso Co., Ltd., product number "PF8”), polyethylene glycol as a dispersion medium (manufactured by Sanyo Kasei Co., Ltd., product number "PEG600", viscosity: 106 mPa ⁇ s (25 ° C.), molecular weight: 600, SP value: 9.4) Disperse in 234 g and stir with a stirrer (“PRIMIX2” manufactured by Primix Co., Ltd.) under the conditions of a rotation speed of 11000 rpm and a stirring time of 30 minutes to obtain a mixture of graphite and PEG600 as a dispersion medium.
  • PF8 polyethylene glycol as a dispersion medium
  • the viscosity of the dispersion medium was measured at 25 ° C. using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd., trade name “TV-25 Type-H”, spindle No. 1).
  • the prepared mixture was placed in a zirconia container of a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") together with 2 mm zirconia balls (2.5 g), and the mixture was mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. It was. After mixing, the removed particles were heated at 420 ° C. for 1 hour in a nitrogen atmosphere. As a result, particles in which the surface of Si particles was coated with flaky graphite and amorphous carbon were obtained.
  • the obtained particles were heated at 500 ° C. for 10 minutes in an air atmosphere. As a result, amorphous carbon was removed to obtain particles in which the surface of Si particles was coated with flaky graphite.
  • the prepared mixture was placed in a zirconia container of a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") together with 2 mm zirconia balls (2.5 g), and the mixture was mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. It was. The obtained mixture was taken out into a glass petri dish and vacuum dried at 120 ° C. for 24 hours to remove water to obtain particles.
  • a planetary ball mill manufactured by Shinky Co., Ltd., product number "NP-100”
  • the prepared mixture was placed in a container of a planetary ball mill (manufactured by Shinky Co., Ltd., product number "NP-100") together with 2 mm zirconia balls (2.5 g), and the mixture was mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. Thereby, particles were obtained.
  • a planetary ball mill manufactured by Shinky Co., Ltd., product number "NP-100”
  • Comparative Example 4 0.0255 g of graphite (manufactured by Toyo Tanso Co., Ltd., product number "PF8”) and 0.6 g of Si particles (manufactured by Kanto Chemical Co., Inc., average particle size: 100 nm, true density: 2.33) were added to a planetary ball mill (manufactured by Shinky Co., Ltd., The particles were placed in a container of product number "NP-100”), and the particles were mixed by planetary stirring at a rotation speed of 2000 rpm for 25 minutes. Thereby, particles were obtained. In Comparative Example 4, 2 mm zirconia balls were not used.
  • Atmosphere Air atmosphere Temperature rise rate: 10 ° C / min Temperature range: 40 ° C to 1000 ° C
  • 3 to 6 are diagrams showing the results of thermogravimetric analysis and measurement of particles before removing amorphous carbon in Examples 1 to 4, respectively.
  • 7 to 10 are diagrams showing the results of thermogravimetric analysis and measurement of particles after removing amorphous carbon in Examples 1 to 4, respectively.
  • 11 to 14 are diagrams showing the results of thermogravimetric analysis and measurement of the particles of Comparative Examples 1 to 4, respectively, in order.
  • the Si particles of Comparative Example 1 (uncoated Si particles) used as the raw material have a weight increase start temperature of around 400 to 500 ° C. as shown in FIG. 11, whereby the oxidation temperature of Si in Examples 1 to 4 is set. It is shifted to the high temperature side, and it can be seen that the Si particles are covered with flaky graphite. Further, in FIGS. 7 to 10, it can be seen that the weight loss on the low temperature side (around 500 ° C.) existing in FIGS. 3 to 6 is reduced or disappears. This makes it possible to confirm that the amorphous carbon has decreased or disappeared.
  • FIG. 15 is a diagram showing a transmission electron micrograph of the particles obtained in Example 4 before removing amorphous carbon.
  • FIG. 16 is a diagram showing a transmission electron micrograph of the particles obtained in Example 4 after removing amorphous carbon.
  • the coating layer was formed on the entire surface of the particle body.
  • the thickness of the coating layer was 5 nm to 40 nm before removing the amorphous carbon and 0.5 nm to 10 nm after removing the amorphous carbon.
  • the conductivity is improved by coating the silicon particles of Comparative Example 1 having high resistance with carbon, and further improving the conductivity by removing amorphous carbon and increasing the coating ratio of crystalline carbon. I was able to confirm that.

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