Classifications

• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
  • C08F114/00—Homopolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen
  • C08F114/18—Monomers containing fluorine
  • C08F114/185—Monomers containing fluorine not covered by the groups C08F114/20 - C08F114/28
• • C—CHEMISTRY; METALLURGY
  • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
  • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
  • C08F214/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen
  • C08F214/18—Monomers containing fluorine
  • C08F214/182—Monomers containing fluorine not covered by the groups C08F214/20 - C08F214/28
• • C—CHEMISTRY; METALLURGY
  • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
  • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
  • C09D127/00—Coating compositions based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Coating compositions based on derivatives of such polymers
  • C09D127/02—Coating compositions based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Coating compositions based on derivatives of such polymers not modified by chemical after-treatment
  • C09D127/12—Coating compositions based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by a halogen; Coating compositions based on derivatives of such polymers not modified by chemical after-treatment containing fluorine atoms
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/403—Manufacturing processes of separators, membranes or diaphragms
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/409—Separators, membranes or diaphragms characterised by the material
  • H01M50/411—Organic material
  • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
  • H01M50/417—Polyolefins
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/409—Separators, membranes or diaphragms characterised by the material
  • H01M50/411—Organic material
  • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
  • H01M50/426—Fluorocarbon polymers
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/409—Separators, membranes or diaphragms characterised by the material
  • H01M50/431—Inorganic material
  • H01M50/434—Ceramics
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/409—Separators, membranes or diaphragms characterised by the material
  • H01M50/443—Particulate material
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/409—Separators, membranes or diaphragms characterised by the material
  • H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/409—Separators, membranes or diaphragms characterised by the material
  • H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
  • H01M50/451—Separators, membranes or diaphragms characterised by the material having a layered structure comprising layers of only organic material and layers containing inorganic material
• • 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

• JP-A-8-231645 Japanese Patent Publication No. 2008-524824
• compositions for coating a separator for an electrochemical device comprising a polymer containing trifluoroethylene units, said polymer having a trifluoroethylene unit content of , 57 to 100 mol% with respect to all monomer units, and when the polymer contains monomer units other than trifluoroethylene units, the other monomers are tetrafluoro At least one monomer ( ⁇ ), and a composition is provided.
• the substrate is preferably made of an organic material.
• it contains trifluoroethylene units, tetrafluoroethylene units and monomer ( ⁇ ) units, wherein monomer ( ⁇ ) is a fluorinated monomer (with the proviso that trifluoroethylene and tetrafluoroethylene fluoroethylene) and at least one polymer selected from the group consisting of polar group-containing monomers.
• monomer ( ⁇ ) is a fluorinated monomer (with the proviso that trifluoroethylene and tetrafluoroethylene fluoroethylene) and at least one polymer selected from the group consisting of polar group-containing monomers.
• porous films such as microporous polyolefin films made of polyethylene, polypropylene, etc. have been generally used as separators.
• these polyolefin porous membranes are highly heat-shrinkable, they have the problem of low dimensional stability at high temperatures.
• the separator may thermally shrink and break, causing an internal short circuit, which may lead to fire or the like.
• heat shrinkage resistance of separators In order to improve the safety of batteries under these high temperatures, there is a demand for improved heat shrinkage resistance of separators.
• the content of other monomer units in the polymer is preferably 0 to 43 mol%, more preferably 40 mol% or less, and still more preferably 38 mol%, based on the total monomer units. or less, particularly preferably 35 mol % or less, more preferably 1 mol % or more, and still more preferably 2 mol % or more.
• fluorinated monomer among others, at least one selected from the group consisting of VdF, CTFE, 2,3,3,3-tetrafluoropropene, HFP and fluoroalkyl vinyl ether is preferable, and CTFE, 2,3 , 3,3-tetrafluoropropene, HFP and fluoroalkylvinyl ether are more preferred.
• the fluorinated monomer may or may not have a polar group.
• a fluorinated monomer having a polar group may be used as the fluorinated monomer.
• non-fluorinated monomers examples include non-fluorinated monomers having no polar group such as ethylene and propylene, and non-fluorinated monomers having a polar group.
• a fluorinated monomer having a polar group and a non-fluorinated monomer having a polar group may be collectively referred to as a polar group-containing monomer.
• the polymer Since the polymer provides excellent adhesion between the substrate and the coating layer, it further contains a monomer (3) unit represented by general formula (3) as another monomer unit. is preferred.
• X is a single bond or an atomic group with a molecular weight of 500 or less composed of 1 to 20 atoms in the main chain.
• trifluoroethylene homopolymer trifluoroethylene/TFE copolymer, trifluoroethylene/TFE/HFP copolymer, trifluoroethylene/TFE/2,3,3,3-tetrafluoropropene copolymer, trifluoroethylene/TFE/CTFE copolymer, trifluoroethylene/TFE/(meth)acrylic acid copolymer, trifluoroethylene/TFE/3-butenoic acid copolymer, trifluoroethylene/TFE/4-pentenoic acid copolymer, trifluoroethylene/TFE/2-carboxyethyl acrylate copolymer, trifluoroethylene/TFE/acryloyloxyethyl succinic acid copolymer, Examples include trifluoroethylene/TFE/HFP/(meth)acrylic acid copolymer.
• the number average molecular weight (in terms of polystyrene) of the polymer is preferably 7,000 to 1,500,000, more preferably 21,000 or more, still more preferably 35,000 or more, more preferably 1,400,000 or less, and still more preferably 1,200,000 or less. , particularly preferably 1,100,000 or less.
• the number average molecular weight can be measured by gel permeation chromatography (GPC) using dimethylformamide as a solvent.
• the melting point of the polymer is preferably 100 to 245°C, more preferably 150°C or higher, even more preferably 180°C or higher, and particularly preferably 195°C or higher.
• the melting point of the polymer was determined using a differential scanning calorimetry (DSC) instrument, increasing the temperature from 30°C to 300°C at a rate of 10°C/min, then decreasing the temperature at 10°C/min to 30°C, and again at 10°C/min. It can be obtained as the temperature for the maximum value in the heat of fusion curve when the temperature is raised to 300 ° C. at the rate of .
• Peroxide polymerization initiators include the oil-soluble peroxides described above.
• Redox polymerization initiators include combinations of the above-described peroxides and reducing agents.
• surfactant known surfactants can be used, for example, nonionic surfactants, anionic surfactants, cationic surfactants and the like can be used.
• fluorine-containing anionic surfactants are preferable, and may contain ether bonds (that is, oxygen atoms may be inserted between carbon atoms), linear or branched fluorine-containing surfactants having 4 to 20 carbon atoms.
• Anionic surfactants are more preferred.
• the amount of surfactant added (to solvent) is preferably 50 to 5000 ppm.
• Examples of the solvent include water, a mixed solvent of water and alcohol, and the like.
• the total amount of monomers to be charged is 1:1 to 1:10, preferably 1:1 to 1:5 in terms of mass ratio of total amount of monomers to water.
• At least one selected from the group consisting of the ester (1) represented by the general formula (1) and the ketone (2) represented by the general formula (2) can be used as the solvent.
• the content ratio of the polymer and the inorganic particles is preferably 50:50 to 1:99, more preferably 30:70 to 2:98, and still more preferably 50:50 to 1:99 in mass ratio ((polymer):(inorganic particles)). is from 20:80 to 3:97.
• the average particle size of the metal hydroxide particles is preferably 25 ⁇ m or less, more preferably 10 ⁇ m or less, still more preferably 5 ⁇ m or less, particularly preferably 1 ⁇ m or less, and preferably 0.02 ⁇ m or more. .
• the average particle size of metal hydroxide particles is a value obtained by measurement with a transmission electron microscope.
• the Gurley value of the electrochemical device separator is preferably 500 sec/100 cc Air or less, more preferably 300 sec/100 cc Air or less.
• the Gurley value is also preferably 50 sec/100 cc Air or more.
• the Gurley value is a value obtained by measuring with a Gurley densometer according to JIS P 8117.
• Carbonaceous materials capable of intercalating and desorbing lithium ions include artificial graphite or purified natural graphite produced by high-temperature treatment of graphitizable pitch obtained from various raw materials, or the surface of these graphites with pitch or other organic matter. Those obtained by carbonization after treatment are preferred.
• the concentration of the electrolyte salt is preferably 0.8 mol/liter or more, more preferably 1.0 mol/liter or more. Although the upper limit depends on the organic solvent for dissolving the electrolyte salt, it is usually 1.5 mol/liter.
• the shape of the lithium-ion secondary battery is arbitrary, and examples include cylindrical, square, laminated, coin-shaped, and large-sized.
• the shape and structure of the positive electrode, negative electrode, and separator can be changed according to the shape of each battery.
• polymer The present disclosure contains trifluoroethylene units, tetrafluoroethylene units and monomer ( ⁇ ) units, wherein monomer ( ⁇ ) is a fluorinated monomer (excluding trifluoroethylene and tetrafluoroethylene). ) and a polymer that is at least one selected from the group consisting of polar group-containing monomers. Specific embodiments of this terpolymer will now be described in detail.
• the laminate of the present disclosure includes a base material formed from an organic material and a coating layer formed from the composition described above. Therefore, since the coating layer can be easily formed, the laminate of the present disclosure can be manufactured with high productivity. In addition, the coating layer has high electrolyte resistance, and therefore the coating layer is less likely to dissolve and swell even when in contact with the electrolyte used in the lithium ion secondary battery. Furthermore, the laminate of the present disclosure is less likely to shrink when exposed to high temperature environments.
• Comparative Examples 1-2 Using polymers h and i alone, a separator was produced in the same manner as in Experimental Example 1, and the thermal shrinkage rate was measured. Table 1 shows the results.

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• 2022
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