Classifications

• • 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
  • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
• • 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
  • C01B32/05—Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
• • 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
• • 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
  • H01M4/139—Processes of manufacture
  • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
• • 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
• • 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
  • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
• • 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
  • C01P2004/32—Spheres
• • 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
• • 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
• • 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 multilayer carbon material used for a non-aqueous secondary battery, a negative electrode for a non-aqueous secondary battery formed using the material, and a non-aqueous secondary battery having the negative electrode.
• the tap density of the multilayer structure carbonaceous material for tap density present invention is 0.8 g / cm 3 or more 1.30 g / cm 3 or less, preferably 0.90 g / cm 3 or more 1.20 g / cm 3 or less by weight, more preferably 0.95 g / cm 3 or more 1.10 g / cm 3 or less.
• Ash content contained in the multilayer structure carbon material of the present invention is usually preferably 1% by mass or less and 0.5% by mass or less based on the total mass of the multilayer structure carbon material. More preferably, it is 1 mass% or less. Moreover, it is preferable that the minimum of ash content is 1 ppm or more.
• the reaction area when the negative electrode is formed using the multi-layer structure carbon material is particularly reduced, requiring a lot of time until full charge, and a preferred non-aqueous secondary battery is It tends to be difficult to obtain.
• the crystallite size (Lc) of the graphite particles determined by X-ray diffraction by the Gakushin method is usually in the range of 30 nm or more, preferably 50 nm or more, more preferably 100 nm or more. Below this range, the crystallinity decreases and the initial irreversible capacity of the battery tends to increase.
• the Raman half-value width is too small, the crystallinity of the particle surface becomes too high, and there is a tendency that the number of sites where Li enters the interlayer increases with charge / discharge. That is, there is a tendency that charge acceptance is lowered.
• the Raman half-value width is too large, the crystallinity of the particle surface decreases, the reactivity with the electrolytic solution increases, and the efficiency tends to decrease and the gas generation increases.
• the specific surface area of the graphite particles measured using the BET method is usually 0.1 m 2 / g or more, preferably 0.7 m 2 / g or more, more preferably 1 m 2 / g or more, and more Preferably it is 2 m 2 / g or more.
• the specific surface area is usually 100 m 2 / g or less, preferably 25 m 2 / g or less, more preferably 20 m 2 / g or less, still more preferably 15 m 2 / g or less, particularly preferably 10 m 2 / g or less, most preferably. 7 m 2 / g or less.
• the particle size d90 of the graphite particles determined by the laser diffraction / scattering method is usually 100 ⁇ m or less, preferably 70 ⁇ m or less, more preferably 50 ⁇ m or less, and even more preferably. Is 45 ⁇ m or less, usually 20 ⁇ m or more, preferably 26 ⁇ m or more, more preferably 30 ⁇ m or more, and even more preferably 34 ⁇ m or more.
• the method for measuring d90 is as described above.
• the crystals tend to be oriented in a direction parallel to the electrode plate, and the load characteristics tend to be reduced.
• the Raman half-value width is too large, the crystallinity of the carbon material particle surface is lowered, the reactivity with the electrolytic solution is increased, and there is a tendency that efficiency is lowered and gas generation is increased.
• the Raman R value of the graphitized product is usually 0.5 or more, preferably 0.7 or more, more preferably 0.9 or more.
• the Raman R value is usually 1.5 or less, preferably 1.4 or less.
• the Raman half width in the vicinity of 1580 cm ⁇ 1 of the graphitized portion is not particularly limited, but is usually 60 cm ⁇ 1 or more, preferably 80 cm ⁇ 1 or more, and usually 150 cm ⁇ 1 or less, preferably 140 cm ⁇ 1 or less.
• the method of coating the graphite particles with the carbonaceous material is a method of using the carbon precursor for obtaining the carbonaceous material as it is, and heating the mixture of the carbon precursor and the graphite particle powder to obtain a composite powder, A carbonaceous material powder obtained by partially carbonizing the carbon precursor described above is prepared in advance, and this is mixed with a graphite particle powder and then heat-treated to form a composite. It is possible to employ a method in which a graphite particle powder, a carbonaceous material powder, and a carbon precursor are mixed and heat-treated to form a composite.
• Second step The mixture is heated to obtain an intermediate substance from which volatile components generated from the solvent and the carbon precursor are removed. This heating may be performed while stirring the mixture as necessary. Moreover, even if the volatile matter remains, it is not a problem because it is removed in a later third step.
• the second step and the fourth step may be omitted depending on circumstances, and the fourth step may be performed before the third step.
• powder processing such as pulverization, pulverization, classification, etc. is performed again after the completion of the third step to obtain a multi-layer structure carbon material. .
• a carbonaceous material such as natural graphite, graphite such as artificial graphite, carbon black such as acetylene black, and amorphous carbon such as needle coke is used as a secondary material.
• a carbonaceous material such as natural graphite, graphite such as artificial graphite, carbon black such as acetylene black, and amorphous carbon such as needle coke is used as a secondary material.
• examples of the current collector include metal foil, metal cylinder, metal coil, metal plate, metal thin film, expanded metal, punch metal, and foam metal.
• a metal thin film is preferable, a copper foil is more preferable, and a rolled copper foil obtained by a rolling method and an electrolytic copper foil obtained by an electrolytic method are more preferable.
• the binder for binding the active material is not particularly limited as long as it is a material that is stable with respect to the electrolyte and the solvent used when manufacturing the electrode.
• resin-based polymers such as polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, aromatic polyamide, cellulose, nitrocellulose; SBR (styrene / butadiene rubber), isoprene rubber, butadiene rubber, fluorine rubber, NBR ( Acrylonitrile-butadiene rubber), rubbery polymers such as ethylene / propylene rubber; styrene / butadiene / styrene block copolymers and hydrogenated products thereof; EPDM (ethylene-propylene-diene terpolymer), styrene / ethylene / Thermoplastic elastomeric polymers such as butadiene / styrene copolymer, s
• Non-aqueous secondary battery [Non-aqueous secondary battery]
• the non-aqueous secondary battery of the present invention will be described in detail.
• an aqueous solvent or an organic solvent is used as a dispersion medium.
• aqueous solvent water is usually used, and additives such as alcohols such as ethanol and cyclic amides such as N-methylpyrrolidone may be added to water up to about 30% by mass or less. it can.
• the non-aqueous electrolyte used in the present invention may contain various auxiliary agents such as cyclic carbonates having unsaturated bonds in the molecule and conventionally known overcharge inhibitors, deoxidizers, and dehydrants. Good.
• vinylene carbonate and vinyl ethylene carbonate are preferable, and vinylene carbonate is particularly preferable.
• Cycle characteristics of the battery can be improved by including in the electrolyte a cyclic carbonate having an unsaturated bond in the molecule.
• a stable protective film can be formed on the surface of the negative electrode.
• this property is not sufficiently improved.
• the content in the non-aqueous electrolyte is preferably in the above range.
• Example 3 A negative electrode material 3 was obtained in the same manner as in Example 1 except that the amount of amorphous carbon added was 0.6% by mass.
• a negative electrode material 12 was obtained in the same manner as in Example 1 except that scale natural graphite (G) was used as the graphite particles and the amount of amorphous carbon added was 2.7 mass%.
• G scale natural graphite

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• Engineering & Computer Science (AREA)
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• Organic Chemistry (AREA)
• Materials Engineering (AREA)
• Manufacturing & Machinery (AREA)
• Composite Materials (AREA)
• Battery Electrode And Active Subsutance (AREA)
• Secondary Cells (AREA)
• Carbon And Carbon Compounds (AREA)

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• 2013
  • 2013-02-22 CN CN201380009104.2A patent/CN104115313B/zh active Active
  • 2013-02-22 JP JP2013032824A patent/JP6251964B2/ja active Active
  • 2013-02-22 WO PCT/JP2013/054616 patent/WO2013125710A1/ja active Application Filing
  • 2013-02-22 KR KR1020147020902A patent/KR102061629B1/ko active Active

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