WO2015133423A1 - Composition de liant pour pile rechargeable - Google Patents

Composition de liant pour pile rechargeable Download PDF

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Publication number
WO2015133423A1
WO2015133423A1 PCT/JP2015/056046 JP2015056046W WO2015133423A1 WO 2015133423 A1 WO2015133423 A1 WO 2015133423A1 JP 2015056046 W JP2015056046 W JP 2015056046W WO 2015133423 A1 WO2015133423 A1 WO 2015133423A1
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WIPO (PCT)
Prior art keywords
binder composition
expandable particles
heat
secondary battery
sensitive gas
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PCT/JP2015/056046
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English (en)
Japanese (ja)
Inventor
金田　拓也
智一 佐々木
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日本ゼオン株式会社
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Application filed by 日本ゼオン株式会社 filed Critical 日本ゼオン株式会社
Priority to KR1020167017184A priority Critical patent/KR102310732B1/ko
Priority to JP2016506476A priority patent/JP6414201B2/ja
Priority to CN201580004094.2A priority patent/CN105900271B/zh
Publication of WO2015133423A1 publication Critical patent/WO2015133423A1/fr

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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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • 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
    • 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

  • This invention relates to the binder composition for secondary batteries used in order to form the electrode compound-material layer of secondary batteries, such as a lithium ion secondary battery.
  • Lithium ion secondary batteries have a high energy density and are used in the fields of mobile phones and laptop computers. However, with the expansion and development of applications, further improvements in performance are required, such as lowering resistance and increasing capacity. Has been.
  • the separator has an important function of preventing an electrical short circuit between the positive electrode and the negative electrode of the lithium ion secondary battery.
  • a separator used in the lithium ion secondary battery for example, a microporous film made of polyolefin resin is used. in use.
  • the separator normally melts and closes the micropore, thereby preventing lithium ion migration and shutting down the current, thereby shutting down the lithium ion secondary battery. It plays a role in maintaining the safety of secondary batteries.
  • the separator contracts rapidly, and the positive electrode and the negative electrode may be in direct contact with each other, thereby expanding the location where the short circuit occurs.
  • the battery temperature may reach a state where it is abnormally overheated to several hundred degrees Celsius or higher.
  • Patent Document 1 a conductive material whose resistance increases in a temperature range of 90 to 160 ° C. is included in the electrode mixture layer, and electrical insulation can be maintained even at a temperature higher than 160 ° C.
  • a lithium ion secondary battery using a separator made of a material that exhibits ion conductivity even when the temperature rises to 160 ° C. or higher and then is cooled to 100 ° C. or lower has been proposed.
  • Patent Document 1 an electrode mixture layer containing a predetermined conductive material and a separator made of a predetermined material are used in combination, but the separator material is a polyolefin resin or the like that is usually used. However, it is also required to form an electrode mixture layer that can ensure safety corresponding to abnormal heating.
  • the objective of this invention is providing the binder composition for secondary batteries which can obtain the electrode compound-material layer which can improve the safety
  • the present inventors have found that the above object can be achieved by using heat-sensitive gas-expandable particles that expand with gas at a predetermined temperature or higher, and have completed the present invention.
  • V 25 ° C. represents the volume of the heat-sensitive gas-expandable particles at 25 ° C.
  • the binder composition for a secondary battery according to (1) (3)
  • Secondary battery binder composition as described above (4)
  • the thermal gas expandable particles have a core-shell structure, and the core material of the thermal gas expandable particles is a hydrocarbon having a boiling point of 10 to 150 ° C.
  • a binder composition for a secondary battery (6)
  • the thermal gas expandable particle has a core-shell structure, and the shell material of the thermal gas expandable particle is a polymer containing a polymer unit having a nitrile group.
  • the binder composition for secondary batteries as described in 1 above is provided.
  • a binder composition for a secondary battery that can provide an electrode mixture layer that can improve the safety of the secondary battery.
  • the binder composition for a secondary battery according to the present invention is a binder composition for a secondary battery containing heat-sensitive gas-expandable particles and a binder resin, and is formed by the binder composition for a secondary battery.
  • the heat-sensitive gas-expandable particles used in the binder composition for a secondary battery of the present invention are particles that expand due to gas when the temperature exceeds a predetermined temperature.
  • the heat-sensitive gas-expandable particles those having a core-shell structure including a shell material formed of a resin or an elastomer and a core material containing a low boiling point solvent are preferable.
  • the heat-sensitive gas-expandable particles having the core-shell structure are, for example, low-boiling solvents that form the core portion and polymer monomers that form the shell portion with the polymer monomer. And a method of polymerizing in stages by changing the ratio of these monomers over time, a hydrophobic low boiling point solvent and a lipophilic monomer that can become core particles, and a hydrophilic It can be produced by mixing and polymerizing a monomer corresponding to a high shell material.
  • “highly hydrophilic” means that the water solubility at a temperature of 20 ° C. is 1 or more (unit: g / 100 g), preferably 3 or more from the viewpoint that the boundary of the core-shell structure becomes clearer, 4 or more. Are more preferred. There is no particular upper limit, but it is preferably 30 or less.
  • the water solubility at 20 ° C. can be measured by the EPA method (EPA Chemical Fate testing Guideline CG-1500 Water Solubility).
  • the water solubility (unit: g / 100 g) of a typical monomer and solvent at a temperature of 20 ° C. is shown in parentheses as follows.
  • the material of the shell material is not particularly limited as long as it has electrolyte resistance and is flexible enough to prevent cracking when the heat-sensitive gas-expandable particles expand. Polymerization having a nitrile group It is preferable to use a polymer containing units.
  • polymer unit having a nitrile group examples include an ⁇ , ⁇ -ethylenically unsaturated nitrile monomer unit.
  • the “monomer unit” is a structural unit formed by polymerizing monomers.
  • the monomer forming the ⁇ , ⁇ -ethylenically unsaturated nitrile monomer unit is not limited as long as it is an ⁇ , ⁇ -ethylenically unsaturated compound having a nitrile group, and acrylonitrile; ⁇ -chloroacrylonitrile, ⁇ - ⁇ -halogenoacrylonitrile such as bromoacrylonitrile; ⁇ -alkylacrylonitrile such as methacrylonitrile; and the like. Acrylonitrile and methacrylonitrile are preferred. These ⁇ , ⁇ -ethylenically unsaturated nitrile monomers may be used in combination.
  • the polymer containing a polymer unit having a nitrile group may be a copolymer of a monomer that forms a polymer unit having a nitrile group and a copolymerizable monomer.
  • the copolymerizable monomer include unsaturated carboxylic acids such as acrylic acid, methacrylic acid, itaconic acid, and fumaric acid; two or more carbons such as ethylene glycol dimethacrylate, diethylene glycol dimethacrylate, and trimethylolpropane triacrylate.
  • Carboxylates having carbon double bonds including styrene, chlorostyrene, vinyl toluene, t-butyl styrene, vinyl benzoic acid, methyl vinyl benzoate, vinyl naphthalene, chloromethyl styrene, hydroxymethyl styrene, ⁇ -methyl styrene, Styrene monomers such as divinylbenzene; Amide monomers such as acrylamide, N-methylolacrylamide, and acrylamide-2-methylpropanesulfonic acid; Olefins such as ethylene and propylene; Diene monomers such as soprene; monomers containing halogen atoms such as vinyl chloride and vinylidene chloride; vinyl esters such as vinyl acetate, vinyl propionate, vinyl butyrate, vinyl benzoate; methyl vinyl ether, ethyl vinyl ether, butyl vinyl ether Vinyl ethers such as methyl vinyl ketone, eth
  • the core material as the inclusion of the shell material of the heat-sensitive gas-expandable particles is not particularly limited as long as it vaporizes when the secondary battery becomes high temperature, but is a hydrocarbon having a boiling point of 10 to 150 ° C. Preferably there is.
  • hydrocarbon having a boiling point of 10 to 150 ° C. examples include isopentane, isooctane, n-pentane, n-hexane, isohexane, heptane, petroleum ether and the like.
  • the volume change of the heat-sensitive gas expandable particles can be obtained, for example, as the volume change of the cast film formed of the heat-sensitive gas expandable particles.
  • the particle size of the heat-sensitive gas-expandable particles is preferably 0.1 to 10 ⁇ m, more preferably 0.3 to 3 ⁇ m, and particularly preferably 0.3 to 1 ⁇ m.
  • the particle diameter can be obtained from an average value obtained by observing an electron microscope and calculating (a + b) / 2 with respect to 100 or more particles, where a is the longest side of the particle image and b is the shortest side.
  • the diene polymer is a polymer containing monomer units obtained by polymerizing conjugated dienes such as butadiene and isoprene.
  • the proportion of monomer units obtained by polymerizing conjugated diene in the diene polymer is usually 40% by weight or more, preferably 50% by weight or more, more preferably 60% by weight or more.
  • Examples of the polymer include homopolymers of conjugated dienes such as polybutadiene and polyisoprene; and copolymers of monomers that are copolymerizable with conjugated dienes.
  • Examples of the copolymerizable monomer include ⁇ , ⁇ -unsaturated nitrile compounds such as acrylonitrile and methacrylonitrile; unsaturated carboxylic acids such as acrylic acid and methacrylic acid; styrene, chlorostyrene, vinyltoluene, and t-butyl.
  • Styrene monomers such as styrene, vinyl benzoic acid, methyl vinyl benzoate, vinyl naphthalene, chloromethyl styrene, hydroxymethyl styrene, ⁇ -methyl styrene and divinyl benzene; olefins such as ethylene and propylene; vinyl chloride and vinylidene chloride Halogen atom-containing monomers such as vinyl acetate, vinyl propionate, vinyl butyrate, vinyl benzoate, etc .; vinyl ethers such as methyl vinyl ether, ethyl vinyl ether, butyl vinyl ether; methyl vinyl ketone, ethyl vinyl Vinyl ketones such as ketone, butyl vinyl ketone, hexyl vinyl ketone, and isopropenyl vinyl ketone; and heterocyclic ring-containing vinyl compounds such as N-vinyl pyrrolidone, vinyl pyridine, and vinyl imidazole.
  • the acrylic polymer is a polymer containing a monomer unit obtained by polymerizing an acrylic ester and / or a methacrylic ester.
  • the proportion of monomer units obtained by polymerizing acrylic acid ester and / or methacrylic acid ester in the acrylic polymer is usually 40% by weight or more, preferably 50% by weight or more, more preferably 60% by weight or more.
  • Examples of the polymer include homopolymers of acrylic acid esters and / or methacrylic acid esters, and copolymers with monomers copolymerizable therewith.
  • Examples of the copolymerizable monomer include unsaturated carboxylic acids such as acrylic acid, methacrylic acid, itaconic acid, and fumaric acid; two or more carbons such as ethylene glycol dimethacrylate, diethylene glycol dimethacrylate, and trimethylolpropane triacrylate.
  • unsaturated carboxylic acids such as acrylic acid, methacrylic acid, itaconic acid, and fumaric acid
  • two or more carbons such as ethylene glycol dimethacrylate, diethylene glycol dimethacrylate, and trimethylolpropane triacrylate.
  • Carboxylates having carbon double bonds including styrene, chlorostyrene, vinyl toluene, t-butyl styrene, vinyl benzoic acid, methyl vinyl benzoate, vinyl naphthalene, chloromethyl styrene, hydroxymethyl styrene, ⁇ -methyl styrene, Styrenic monomers such as divinylbenzene; Amide monomers such as acrylamide, N-methylolacrylamide, and acrylamide-2-methylpropanesulfonic acid; ⁇ , ⁇ -insoluble such as acrylonitrile and methacrylonitrile Nitrile compounds; olefins such as ethylene and propylene; diene monomers such as butadiene and isoprene; monomers containing halogen atoms such as vinyl chloride and vinylidene chloride; vinyl acetate, vinyl propionate, vinyl butyrate, vinyl benzoate Vinyl esters such as methyl vinyl
  • the fluorine-based polymer is a polymer containing a monomer unit containing a fluorine atom.
  • Specific examples of the fluoropolymer include polytetrafluoroethylene, polyvinylidene fluoride, tetrafluoroethylene / perfluoroalkyl vinyl ether copolymer, ethylene / tetrafluoroethylene copolymer, ethylene / chlorotrifluoroethylene copolymer, A perfluoroethylene propene copolymer may be mentioned.
  • the binder composition for secondary batteries of the present invention comprises the above-mentioned heat-sensitive gas-expandable particles and a binder resin.
  • V (25 ° C. represents the volume of the cast film at 25 ° C.), and is preferably from 15 to 25.
  • the volume change of the cast film formed by the secondary battery binder composition of the present invention is too large, the adhesive strength / cohesive strength of the secondary battery binder composition will be reduced, and the cycle characteristics of the secondary battery obtained will be descend.
  • the volume change of the cast film formed by the binder composition for a secondary battery of the present invention is too small, the distance between the electrode active materials cannot be sufficiently widened, so that the desired safety may not be obtained. is there.
  • the mixing method of the heat-sensitive gas-expandable particles and the binder resin is not particularly limited, and examples thereof include a method using a mixing apparatus such as a stirring type, a shaking type, and a rotary type.
  • the binder composition of this invention can be used for the electrode for secondary batteries.
  • An electrode for a secondary battery is obtained by forming an electrode mixture layer on a current collector, and the electrode mixture layer is made of an electrode active material, the binder composition of the present invention, and a thickener used as necessary. And a conductive material.
  • the content of the binder composition in the electrode mixture layer is 0.1 to 20 parts by weight, preferably 0.2 to 15 parts by weight, and more preferably 0.3 parts by weight with respect to 100 parts by weight of the electrode mixture layer. ⁇ 10 parts by weight.
  • the electrode mixture layer is formed by applying and drying an electrode active material, a binder composition of the present invention, a slurry composition for an electrode containing a thickener and a conductive material, if necessary, on a current collector.
  • the method for applying the electrode slurry composition on the current collector is not particularly limited. Examples thereof include a doctor blade method, a dip method, a reverse roll method, a direct roll method, a gravure method, an extrusion method, a comma direct coating, a slide die coating, and a brush coating method.
  • the drying method include drying with warm air, hot air, low-humidity air, vacuum drying, and drying by irradiation with (far) infrared rays or electron beams.
  • the drying time is usually 1 to 60 minutes, and the drying temperature is usually 40 to 180 ° C.
  • the electrode mixture layer may be formed by repeating the application and drying of the electrode slurry composition a plurality of times.
  • the slurry composition for an electrode can be obtained by mixing an electrode active material, a binder, a thickener and a conductive material used as necessary, and a solvent such as water.
  • the mixing method is not particularly limited, and examples thereof include a method using a mixing apparatus such as a stirring type, a shaking type, and a rotary type.
  • a method using a dispersion kneader such as a homogenizer, a ball mill, a sand mill, a roll mill, a planetary mixer, and a planetary kneader can be used.
  • the material of the current collector is, for example, metal, carbon, conductive polymer, etc., and metal is preferably used.
  • As the current collector metal aluminum, platinum, nickel, tantalum, titanium, stainless steel, copper, other alloys and the like are usually used. Among these, it is preferable to use copper, aluminum, or an aluminum alloy in terms of conductivity and voltage resistance.
  • the thickness of the current collector is preferably 5 to 100 ⁇ m, more preferably 8 to 70 ⁇ m, and still more preferably 10 to 50 ⁇ m.
  • the electrode active material (positive electrode active material) of the positive electrode for the lithium ion secondary battery includes a metal oxide capable of reversibly doping and dedoping lithium ions. It is done. Examples of the metal oxide include lithium cobaltate, lithium nickelate, lithium manganate, and lithium iron phosphate.
  • the positive electrode active material illustrated above may be used independently according to a use, and may be used in mixture of multiple types.
  • the negative electrode active material (negative electrode active material) as the counter electrode of the positive electrode for a lithium ion secondary battery
  • low crystalline carbon non-graphitizable carbon, non-graphitizable carbon, pyrolytic carbon, etc.
  • Crystalline carbon graphite (natural graphite, artificial graphite)
  • alloy materials such as tin and silicon, oxides such as silicon oxide, tin oxide, and lithium titanate.
  • the negative electrode active material illustrated above may be used independently according to a use suitably, and may be used in mixture of multiple types.
  • the shape of the electrode active material of the electrode for a lithium ion secondary battery is preferably a granulated particle.
  • a higher-density electrode can be formed during electrode molding.
  • the volume average particle diameter of the electrode active material of the electrode for a lithium ion secondary battery is usually 0.1 to 100 ⁇ m, preferably 0.5 to 50 ⁇ m, more preferably 0.8 to 30 ⁇ m for both the positive electrode and the negative electrode.
  • the electrode mixture layer of the present invention may contain a conductive material as necessary.
  • the conductive material is not particularly limited as long as it is a conductive material, but a conductive particulate material is preferable.
  • conductive carbon black such as furnace black, acetylene black, and ketjen black
  • natural graphite such as artificial graphite
  • carbon fibers such as polyacrylonitrile-based carbon fiber, pitch-based carbon fiber, and vapor grown carbon fiber.
  • the average particle diameter when the conductive material is a particulate material is not particularly limited, but is preferably smaller than the average particle diameter of the electrode active material, from the viewpoint of expressing sufficient conductivity with a smaller amount of use,
  • the thickness is preferably 0.001 to 10 ⁇ m, more preferably 0.05 to 5 ⁇ m, and still more preferably 0.1 to 1 ⁇ m.
  • the electrode mixture layer of the present invention may contain a thickener as necessary.
  • thickeners include cellulosic polymers such as carboxymethylcellulose, methylcellulose, hydroxypropylcellulose, and ammonium salts and alkali metal salts thereof; (modified) poly (meth) acrylic acid and ammonium salts and alkali metal salts thereof; ) Polyvinyl alcohols such as polyvinyl alcohol, copolymers of acrylic acid or acrylate and vinyl alcohol, maleic anhydride or copolymers of maleic acid or fumaric acid and vinyl alcohol; polyethylene glycol, polyethylene oxide, polyvinyl pyrrolidone, modified Examples thereof include polyacrylic acid, oxidized starch, phosphoric acid starch, casein, various modified starches, acrylonitrile-butadiene copolymer hydride, and the like. Among these, it is preferable to use carboxymethylcellulose, ammonium salt of carboxymethylcellulose, and alkali metal salt.
  • the content of the thickener in the electrode mixture layer is preferably within a range that does not affect the battery characteristics, and is preferably 0.1 to 5 parts by weight, more preferably 0.2 parts per 100 parts by weight of the electrode mixture layer. -4 parts by weight, more preferably 0.3-3 parts by weight.
  • the usage mode of the electrode for an electrochemical element of the present invention includes a lithium ion secondary battery using such an electrode.
  • a lithium ion secondary battery uses an electrode for an electrochemical device in which an electrode mixture layer containing the binder composition of the present invention is formed as at least one of a positive electrode and a negative electrode, and further includes a separator and an electrolytic solution.
  • a polyolefin resin such as polyethylene or polypropylene
  • a microporous film or nonwoven fabric containing an aromatic polyamide resin a porous resin coat containing an inorganic ceramic powder, or the like
  • a porous resin coat containing an inorganic ceramic powder, or the like can be used.
  • the thickness of the separator is preferably 0.5 to 40 ⁇ m, more preferably from the viewpoint of reducing resistance due to the separator in the lithium ion secondary battery and excellent workability when manufacturing the lithium ion secondary battery.
  • the thickness is 1 to 30 ⁇ m, more preferably 1 to 25 ⁇ m.
  • the electrolytic solution is not particularly limited.
  • a solution obtained by dissolving a lithium salt as a supporting electrolyte in a non-aqueous solvent can be used.
  • the lithium salt include LiPF 6 , LiAsF 6 , LiBF 4 , LiSbF 6 , LiAlCl 4 , LiClO 4 , CF 3 SO 3 Li, C 4 F 9 SO 3 Li, CF 3 COOLi, (CF 3 CO) 2 NLi , (CF 3 SO 2 ) 2 NLi, (C 2 F 5 SO 2 ) NLi, and other lithium salts.
  • LiPF 6 , LiClO 4 , and CF 3 SO 3 Li that are easily soluble in a solvent and exhibit a high degree of dissociation are preferably used. These can be used alone or in admixture of two or more.
  • the amount of the supporting electrolyte is usually 1 wt% or more, preferably 5 wt% or more, and usually 30 wt% or less, preferably 20 wt% or less with respect to the electrolytic solution. If the amount of the supporting electrolyte is too small or too large, the ionic conductivity is lowered, and the charging characteristics and discharging characteristics of the battery are degraded.
  • the solvent used in the electrolytic solution is not particularly limited as long as it can dissolve the supporting electrolyte.
  • Alkyl carbonates such as carbonate (BC) and methyl ethyl carbonate (MEC); esters such as ⁇ -butyrolactone and methyl formate; ethers such as 1,2-dimethoxyethane; tetrahydrofuran; sulfolane and dimethyl sulfoxide Sulfur-containing compounds are used.
  • dimethyl carbonate, ethylene carbonate, propylene carbonate, diethyl carbonate, and methyl ethyl carbonate are preferable because high ion conductivity is easily obtained and the use temperature range is wide. These can be used alone or in admixture of two or more. Moreover, it is also possible to use an electrolyte containing an additive.
  • the additive is preferably a carbonate compound such as vinylene carbonate (VC).
  • electrolytic solutions include gel polymer electrolytes in which a polymer electrolyte such as polyethylene oxide or polyacrylonitrile is impregnated with an electrolytic solution, lithium sulfide, LiI, Li 3 N, Li 2 SP—P 2 S 5 glass ceramic, etc.
  • An inorganic solid electrolyte can be mentioned.
  • a lithium ion secondary battery is obtained by stacking a negative electrode and a positive electrode through a separator, winding this according to the shape of the battery, folding it into a battery container, pouring the electrolyte into the battery container and sealing it. It is done. Further, if necessary, an expanded metal, an overcurrent prevention element such as a fuse or a PTC element, a lead plate and the like can be inserted to prevent an increase in pressure inside the battery and overcharge / discharge.
  • the shape of the battery may be any of a laminated cell type, a coin type, a button type, a sheet type, a cylindrical type, a square type, a flat type, and the like.
  • a binder composition for a secondary battery that can provide an electrode mixture layer that can improve the safety of the secondary battery.
  • the volume change of the binder composition, the high-temperature cycle characteristics of the lithium ion secondary battery, and the safety test were evaluated as follows.
  • V (150 degreeC) volume of the cast film of the binder composition at 150 degreeC
  • V (150 degreeC) volume of the cast film of the binder composition at 150 degreeC
  • the volume change (v (150 ° C.) / V (25 ° C.)) of the cast film of heat-sensitive gas-expandable particles was also calculated in the same manner as the volume change of the binder composition. That is, the dispersion of the heat-sensitive gas-expandable particles is poured into a Teflon (registered trademark) container, formed into a film in an environment of 23 ° C. and 50% RH, and further vacuum dried at 25 ° C. for 24 hours. A film of heat-sensitive gas expandable particles having a thickness of 1 mm was obtained. This film was cut into a size of 10 cm long ⁇ 1 cm wide to obtain a test piece.
  • Teflon registered trademark
  • v (25 ° C.) volume of cast film of heat-sensitive gas-expandable particles at 25 ° C.
  • v (150 ° C.) volume of cast film of heat-sensitive gas-expandable particles at 150 ° C.
  • volume change (v (150 ° C.) / V (25 ° C.)) of the cast film of heat-sensitive gas-expandable particles was determined.
  • volume change of the binder resin was calculated in the same manner as the volume change of the binder composition.
  • volume changes of the cast films of the binder resins a to d used in the examples and comparative examples are all the same. 1.0.
  • the elapsed time was evaluated according to the following criteria, and the results are shown in Table 1. The longer the elapsed time, the higher the safety of the battery. A: 30 minutes or more B: 20 minutes or more and less than 30 minutes C: 10 minutes or more and less than 20 minutes D: Less than 10 minutes
  • Example 1 (Production of heat-sensitive gas expandable particles A) In a reactor equipped with a stirrer, 94.0 parts of acrylonitrile as a monomer, 5.0 parts of methacrylic acid, 1.0 part of ethylene glycol dimethacrylate (Kyoeisha Chemical Co., Ltd.
  • Light Ester EG Light Ester EG
  • isopentane as a swelling agent 20.0 parts
  • 1.0 part of sodium dodecylbenzenesulfonate as an emulsifier 1.0 part of t-butylperoxy-2-ethylhexanoate (“NOBUTYL CO.”
  • NOBUTYL CO t-butylperoxy-2-ethylhexanoate
  • aqueous phase polymerization inhibitor 0.5 part of hydroquinone and 400 parts of ion-exchanged water were added and stirred until coarse droplets could not be visually confirmed.
  • binder composition 1 50 parts of heat-sensitive gas-expandable particles A corresponding to the solid content, 50 parts of binder resin a corresponding to the solid content, and ion-exchanged water were stirred for 1 hour in a 25 ° C. environment. This obtained the water dispersion of the binder composition 1 whose solid content concentration is 30 weight%. The volume change (V (150 ° C.) / V (25 ° C.)) of the cast film formed from this binder composition 1 was 17.0.
  • the above-mentioned slurry composition for negative electrode was applied on a copper foil (current collector) having a thickness of 20 ⁇ m by a comma coater so that the coating amount was 9.8 to 10.2 mg / cm 2 .
  • the copper foil coated with the negative electrode slurry composition is transported in an oven at 80 ° C. for 2 minutes and further in an oven at 120 ° C. for 2 minutes at a speed of 0.3 m / min.
  • the slurry composition of was dried and the negative electrode original fabric was obtained.
  • the obtained negative electrode raw material was pressed with a roll press machine so that the density of the composite layer became 1.45 to 1.55 g / cm 3, and further placed in an environment of 120 ° C. under vacuum conditions for 10 hours.
  • a negative electrode sheet having a negative electrode mixture layer formed thereon was produced.
  • the negative electrode sheet was cut into a predetermined size, processed, and the negative electrode lead was welded to obtain a negative electrode.
  • the obtained positive electrode slurry composition was applied onto a 20 ⁇ m thick aluminum foil with a comma coater and dried. This drying was performed by transporting the aluminum foil in an oven at 60 ° C. at a speed of 0.5 m / min for 2 minutes. Thereafter, heat treatment was performed at 120 ° C. for 2 minutes to obtain a positive electrode raw material.
  • the obtained positive electrode raw material is dried and then pressed with a roll press machine so that the mixed material layer density is 3.40 to 3.50 g / cm 3 , and vacuum conditions are used for the purpose of removing moisture.
  • a positive electrode sheet in which a positive electrode mixture layer was formed on a current collector was produced in an environment of 120 ° C. for 3 hours. The positive electrode sheet was cut into a predetermined size, processed, and the positive electrode lead was welded to obtain a positive electrode.
  • the negative electrode manufactured above and the positive electrode were wound into a jelly roll shape together with a single-layer polypropylene separator (thickness 25 ⁇ m, porosity 55%) manufactured by a dry method to produce an electrode group. .
  • This electrode group was inserted into a pouch-type battery case, and after pouring a nonaqueous electrolytic solution, the opening of the battery case was sealed with a heat sealer to complete a lithium ion secondary battery.
  • the design capacity of the battery was 2000 mAh.
  • the non-aqueous electrolyte a solution obtained by adding 2% by volume of VC (vinylene carbonate) to a LiPF 6 solution having a concentration of 1.0 M was used as the non-aqueous electrolyte.
  • Example 2 (Preparation of binder composition 2)
  • the heat-sensitive gas-expandable particles A were stirred for 5 hours under an environment of 25 ° C., and 5 parts by weight corresponding to the solid content, 95 parts by weight of the binding resin a, and ion-exchanged water. This obtained the water dispersion of the binder composition 2 whose solid content concentration is 30 weight%.
  • the volume change (V (150 ° C.) / V (25 ° C.)) of the cast film formed from this binder composition 2 was 2.6.
  • a negative electrode, a positive electrode, and a lithium ion secondary battery were manufactured in the same manner as in Example 1 except that the binder composition 2 was used.
  • Example 3 (Preparation of binder composition 3)
  • the heat-sensitive gas-expandable particles A were agitated for 1 hour in an environment of 25 ° C. in an amount of 85 parts in terms of solids, the binder resin a 15 in terms of solids, and ion-exchanged water. This obtained the water dispersion of the binder composition 3 whose solid content concentration is 30 weight%.
  • the volume change (V (150 ° C.) / V (25 ° C.)) of the cast film formed from this binder composition 3 was 28.2.
  • a negative electrode, a positive electrode, and a lithium ion secondary battery were manufactured in the same manner as in Example 1 except that the binder composition 3 was used.
  • Example 4 (Production of heat-sensitive gas-expandable particles B) In a reactor equipped with a stirrer, 93.0 parts of methacrylonitrile as a monomer, 5.0 parts of acrylic acid, 2.0 parts of divinylbenzene, 20.0 parts of isopentane as a swelling agent, dodecylbenzenesulfonic acid as an emulsifier 1.0 part of sodium, 1.0 part of t-butylperoxy-2-ethylhexanoate (NOF "Perbutyl O") as a polymerization initiator, 0.5 part of hydroquinone as an aqueous phase polymerization inhibitor And 400 parts of ion-exchanged water were added and stirred until coarse droplets could not be visually confirmed.
  • Example 5 (Production of heat-sensitive gas-expandable particles C) 1. In a reactor equipped with a stirrer, 50.0 parts of acrylonitrile and 44.0 parts of methacrylonitrile, 5.0 parts of methacrylic acid, ethylene glycol dimethacrylate (Kyoeisha Chemical Co., Ltd.
  • Light Ester EG 0 parts, 20.0 parts of isooctane as a swelling agent, 0.3 part of sodium dodecylbenzenesulfonate as an emulsifier, t-butylperoxy-2-ethylhexanoate as a polymerization initiator (“Perbutyl O )), 1.0 part of hydroquinone as an aqueous phase polymerization inhibitor, and 400 parts of ion-exchanged water were added and stirred until no coarse droplets could be visually confirmed.
  • Perbutyl O t-butylperoxy-2-ethylhexanoate
  • binder composition 5 Preparation of binder composition 5 50 parts of heat-sensitive gas-expandable particles C corresponding to solid content, 50 parts of binder resin a corresponding to solid content, and ion-exchanged water were stirred for 1 hour in a 25 ° C. environment. This obtained the water dispersion of the binder composition 5 whose solid content concentration is 30 weight%. The volume change (V (150 ° C.) / V (25 ° C.)) of the cast film formed from this binder composition 5 was 9.5. A negative electrode, a positive electrode, and a lithium ion secondary battery were manufactured in the same manner as in Example 1 except that the binder composition 5 was used.
  • Example 7 (Production of binder resin c) In a 5 MPa pressure vessel equipped with a stirrer, 19.9 parts of acrylonitrile as a monomer, 80.0 parts of acrylic acid, 0.1 part of ethylene glycol dimethacrylate (“Kyoeisha Chemical Co., Ltd.“ Light Ester EG ”), ion exchange as a solvent 150 parts of water and 1.0 part of potassium persulfate as a polymerization initiator were added and stirred sufficiently, and then heated to 55 ° C. to initiate polymerization. When the monomer consumption reached 95.0%, the reaction was stopped by cooling.
  • a 5% aqueous sodium hydroxide solution was added to the aqueous dispersion containing the polymer thus obtained to adjust the pH to 8. Then, the unreacted monomer was removed by heating under reduced pressure. Furthermore, it cooled to 30 degrees C or less after that. Thereby, water-soluble binder resin c was obtained.
  • Example 8 (Preparation of binder composition 8) An aqueous dispersion of heat-sensitive gas-expandable particles A and PVDF (polyvinylidene fluoride, “KF-1100” manufactured by Kureha Chemical Co., Ltd.) as a binder resin d are mixed at a weight to solid content ratio of 1: 1. Further, NMP (N-methyl-2-pyrrolidone) was added. The binder composition 8 which uses NMP as a solvent was prepared by removing water from this by vacuum distillation. The volume change (V (150 ° C.) / V (25 ° C.)) of the cast film formed from this binder composition 8 was 17.0.
  • PVDF polyvinylidene fluoride, “KF-1100” manufactured by Kureha Chemical Co., Ltd.
  • NMP N-methyl-2-pyrrolidone
  • the obtained positive electrode slurry composition was applied onto a 20 ⁇ m thick aluminum foil with a comma coater and dried. This drying was performed by transporting the aluminum foil in an oven at 60 ° C. at a speed of 0.5 m / min for 2 minutes. Thereafter, heat treatment was performed at 120 ° C. for 2 minutes to obtain a positive electrode raw material.
  • the obtained positive electrode raw material is dried and then pressed with a roll press machine so that the mixed material layer density is 3.40 to 3.50 g / cm 3 , and vacuum conditions are used for the purpose of removing moisture.
  • a positive electrode sheet was formed by forming a positive electrode mixture layer on the current collector in an environment of 120 ° C. for 3 hours. The positive electrode sheet was cut into a predetermined size, processed, and the positive electrode lead was welded to obtain a positive electrode.
  • the above-mentioned slurry composition for negative electrode was applied on a copper foil (current collector) having a thickness of 20 ⁇ m by a comma coater so that the coating amount was 9.8 to 10.2 mg / cm 2 .
  • the copper foil coated with the negative electrode slurry composition is transported in an oven at 80 ° C. for 2 minutes and further in an oven at 120 ° C. for 2 minutes at a speed of 0.3 m / min.
  • the slurry composition of was dried and the negative electrode original fabric was obtained.
  • the obtained negative electrode raw material was pressed with a roll press machine so that the density of the composite layer became 1.45 to 1.55 g / cm 3, and further placed in an environment of 120 ° C. under vacuum conditions for 10 hours.
  • a negative electrode sheet having a negative electrode mixture layer formed thereon was prepared. The negative electrode sheet was cut into a predetermined size, processed, and the negative electrode lead was welded to obtain a negative electrode.
  • the negative electrode manufactured above and the positive electrode were wound into a jelly roll shape together with a single-layer polypropylene separator (thickness 25 ⁇ m, porosity 55%) manufactured by a dry method to produce an electrode group. .
  • This electrode group was inserted into a pouch-type battery case, and after pouring a nonaqueous electrolytic solution, the opening of the battery case was sealed with a heat sealer to complete a lithium ion secondary battery.
  • the design capacity of the battery was 2000 mAh.
  • the non-aqueous electrolyte a solution obtained by adding 2% by volume of VC (vinylene carbonate) to a LiPF 6 solution having a concentration of 1.0 M was used as the non-aqueous electrolyte.
  • Example 2 (Production of heat-sensitive gas-expandable particles D) Thermally-sensitive gas-expandable particles were produced under the same conditions as in Example 1 except that the amount of isopentane used in Example 1 (Production of thermal-sensitive gas-expandable particles A) was 1.8 parts. An aqueous dispersion of heat-sensitive gas-expandable particles D having a diameter of 600 nm was obtained. The volume change of the heat-sensitive gas expandable particles D was 2.7.
  • Example 4 (Production of heat-sensitive gas expandable particles E) Thermally-sensitive gas-expandable particles were produced under the same conditions as in Example 1 except that the amount of isopentane used in (Production of thermal-sensitive gas-expandable particles A) in Example 1 was 40.0 parts. An aqueous dispersion of heat-sensitive gas-expandable particles E having a diameter of 600 nm was obtained. The volume change of the heat-sensitive gas expandable particles E was 65.0.
  • binder composition 12 50 parts of heat-sensitive gas-expandable particles E corresponding to the solid content, 50 parts of binder resin a corresponding to the solid content, and ion-exchanged water were stirred for 1 hour in a 25 ° C. environment. Thus, an aqueous dispersion of the binder composition 12 having a solid content concentration of 30% by weight was obtained. The volume change (V (150 ° C.) / V (25 ° C.)) of the cast film formed from this binder composition 12 was 33.0. A negative electrode, a positive electrode, and a lithium ion secondary battery were produced in the same manner as in Example 1 except that the binder composition 12 was used.
  • the obtained positive electrode slurry composition was applied onto a 20 ⁇ m thick aluminum foil with a comma coater and dried. This drying was performed by transporting the aluminum foil in an oven at 60 ° C. at a speed of 0.5 m / min for 2 minutes. Thereafter, heat treatment was performed at 120 ° C. for 2 minutes to obtain a positive electrode raw material.
  • the obtained positive electrode raw material is dried and then pressed with a roll press machine so that the mixed material layer density is 3.40 to 3.50 g / cm 3 , and vacuum conditions are used for the purpose of removing moisture.
  • a positive electrode sheet was formed by forming a positive electrode mixture layer on the current collector in an environment of 120 ° C. for 3 hours. The positive electrode sheet was cut into a predetermined size, processed, and the positive electrode lead was welded to obtain a positive electrode.
  • the obtained slurry composition for negative electrode was applied on a copper foil (current collector) having a thickness of 20 ⁇ m by a comma coater so that the coating amount was 9.8 to 10.2 mg / cm 2 .
  • the copper foil coated with the negative electrode slurry composition is transported in an oven at 80 ° C. for 2 minutes and further in an oven at 120 ° C. for 2 minutes at a speed of 0.3 m / min.
  • the slurry composition of was dried and the negative electrode original fabric was obtained.
  • the obtained negative electrode raw material was pressed with a roll press machine so that the density of the composite layer became 1.45 to 1.55 g / cm 3, and further placed in an environment of 120 ° C. under vacuum conditions for 10 hours.
  • a negative electrode sheet having a negative electrode mixture layer formed thereon was produced.
  • the negative electrode sheet was cut into a predetermined size, processed, and the negative electrode lead was welded to obtain a negative electrode.
  • a lithium ion secondary battery was produced in the same manner as in Example 1 except that the positive electrode and the negative electrode obtained above were used.
  • the lithium ion secondary battery obtained by using the secondary battery binder composition was good in high-temperature cycle characteristics and safety.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Connection Of Batteries Or Terminals (AREA)
  • Secondary Cells (AREA)

Abstract

　L'invention concerne une composition de liant pour une pile rechargeable, la composition de liant comprenant des particules expansibles de gaz thermosensible et une résine de liaison, laquelle composition de liant pour une pile rechargeable est telle que la variation de volume (V (150 °C)/V (25 °C)) d'un film coulé formé par la composition de liant pour une pile rechargeable est comprise entre 2 et 30 (où " V (150 °C) " indique le volume du film coulé à 150 °C, et " V (25 °C)" indique le volume du film coulé à 25 °C).
PCT/JP2015/056046 2014-03-03 2015-03-02 Composition de liant pour pile rechargeable WO2015133423A1 (fr)

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KR20240035448A (ko) 2021-07-27 2024-03-15 니폰 제온 가부시키가이샤 전기 화학 소자용 전극 및 전기 화학 소자용 전극의 제조 방법

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WO2019189865A1 (fr) * 2018-03-30 2019-10-03 三井化学株式会社 Électrode négative contenant des microcapsules, et batterie secondaire au lithium-ion équipée de celle-ci
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WO2022113860A1 (fr) * 2020-11-30 2022-06-02 日本ゼオン株式会社 Composition de liant pour électrodes de batteries secondaires au lithium-ion non aqueux, son procédé de production, solution de liant pour électrodes de batteries secondaires au lithium-ion non aqueux, composition de suspension pour électrodes de batteries secondaires au lithium-ion non aqueux, électrode pour batteries secondaires au lithium-ion non aqueux, et batterie secondaire au lithium-ion non aqueux
WO2023008266A1 (fr) * 2021-07-27 2023-02-02 日本ゼオン株式会社 Composition de liant pour éléments électrochimiques, composition de bouillie pour électrodes d'élément électrochimique, électrode pour éléments électrochimiques et élément électrochimique
KR20240035448A (ko) 2021-07-27 2024-03-15 니폰 제온 가부시키가이샤 전기 화학 소자용 전극 및 전기 화학 소자용 전극의 제조 방법
KR20240035397A (ko) 2021-07-27 2024-03-15 니폰 제온 가부시키가이샤 전기 화학 소자용 바인더 조성물, 전기 화학 소자 전극용 슬러리 조성물, 전기 화학 소자용 전극, 및 전기 화학 소자

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CN105900271A (zh) 2016-08-24
CN105900271B (zh) 2018-07-17

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