WO2016080143A1 - 電極構成体固定用両面テープおよび二次電池 - Google Patents
電極構成体固定用両面テープおよび二次電池 Download PDFInfo
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- WO2016080143A1 WO2016080143A1 PCT/JP2015/079938 JP2015079938W WO2016080143A1 WO 2016080143 A1 WO2016080143 A1 WO 2016080143A1 JP 2015079938 W JP2015079938 W JP 2015079938W WO 2016080143 A1 WO2016080143 A1 WO 2016080143A1
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- sensitive adhesive
- double
- pressure
- heat
- sided tape
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Classifications
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- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
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- H01M10/058—Construction or manufacture
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
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- C—CHEMISTRY; METALLURGY
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- H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
- H01M50/233—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions
- H01M50/24—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions adapted for protecting batteries from their environment, e.g. from corrosion
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- H01M50/50—Current conducting connections for cells or batteries
- H01M50/572—Means for preventing undesired use or discharge
- H01M50/574—Devices or arrangements for the interruption of current
- H01M50/578—Devices or arrangements for the interruption of current in response to pressure
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- H01M50/574—Devices or arrangements for the interruption of current
- H01M50/581—Devices or arrangements for the interruption of current in response to temperature
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2203/00—Applications of adhesives in processes or use of adhesives in the form of films or foils
- C09J2203/33—Applications of adhesives in processes or use of adhesives in the form of films or foils for batteries or fuel cells
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
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- C09J2301/124—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet by the arrangement of layers the adhesive layer being present on both sides of the carrier, e.g. double-sided adhesive tape
- C09J2301/1242—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive tape or sheet by the arrangement of layers the adhesive layer being present on both sides of the carrier, e.g. double-sided adhesive tape the opposite adhesive layers being different
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2301/00—Additional features of adhesives in the form of films or foils
- C09J2301/20—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive itself
- C09J2301/208—Additional features of adhesives in the form of films or foils characterized by the structural features of the adhesive itself the adhesive layer being constituted by at least two or more adjacent or superposed adhesive layers, e.g. multilayer adhesive
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2301/00—Additional features of adhesives in the form of films or foils
- C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
- C09J2301/302—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier the adhesive being pressure-sensitive, i.e. tacky at temperatures inferior to 30°C
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2301/00—Additional features of adhesives in the form of films or foils
- C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
- C09J2301/304—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier the adhesive being heat-activatable, i.e. not tacky at temperatures inferior to 30°C
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2421/00—Presence of unspecified rubber
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2423/00—Presence of polyolefin
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2423/00—Presence of polyolefin
- C09J2423/006—Presence of polyolefin in the substrate
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2433/00—Presence of (meth)acrylic polymer
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J2467/00—Presence of polyester
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- H01M2200/00—Safety devices for primary or secondary batteries
- H01M2200/10—Temperature sensitive devices
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- 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
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- 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
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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- 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
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Definitions
- the present invention relates to a double-sided tape for fixing an electrode structure, and more specifically, a heat-sensitive adhesive that can be suitably used for a pouch-type battery that can prevent an electrode active material layer from falling off an electrode and has excellent tab portion sealing performance. And a pressure-sensitive adhesive double-sided tape for fixing an electrode assembly, and a secondary battery to which the electrode assembly is fixed using the double-sided tape.
- Lithium ion secondary batteries which have a high energy density and can be repeatedly charged and discharged, is rapidly expanding by taking advantage of their characteristics.
- Lithium ion secondary batteries are used in fields such as mobile phones, notebook personal computers, and electric vehicles because of their relatively high energy density.
- a lithium ion secondary battery is a secondary battery in which an electrode structure in which a positive electrode member, a separator member, and a negative electrode member are stacked or wound is stored in an exterior body.
- Lithium ion secondary batteries have become widespread in recent years, and at the same time as capacity has increased, improvement in capacity density has also been demanded. In particular, there is a great demand for improving the weight density. Therefore, a pouch-type battery in which an electrode structure is sealed inside a container with a laminate film as an exterior body and heat sealed at the end is proposed because of the demand for weight reduction. Has been.
- batteries for portable electronic devices have also been increased in capacity and size, and in large batteries for use in electric vehicles, the weight of the electrode structure accommodated in the laminate film outer package has increased, so vibration has been applied. In this case, the electrode structure is easy to move. Therefore, the force applied to the tab portion is increased, and the adhesiveness between the tab portion and the exterior body is reduced, which may reduce the sealing performance.
- Patent Document 1 proposes that an adhesive tape having an adhesive layer on one side of a substrate is used for winding a wound battery. However, there is no adhesion capability other than the adhesive surface, and it was not suitable for fixing the electrode structure to the exterior body.
- Patent Document 2 and Patent Document 3 describe that a double-sided pressure-sensitive adhesive tape having pressure-sensitive adhesive layers on both surfaces of a base material is used for fixing a battery outer body and an electrode structure.
- Patent Document 3 in order to prevent problems such as sticking at the entrance when the electrode structure to which the double-sided adhesive tape is attached is sealed in the battery outer body, the adhesion of the electrode structure before sealing is avoided. It has been proposed to use a release sheet on the surface. However, when the release sheet is peeled off and the exterior body and the electrode assembly are adhered, air bubbles remain between the adhesive tape and the exterior body, particularly the adhesive force after high-temperature storage deteriorates, and the resulting lithium The capacity retention rate of the ion secondary battery after high temperature storage was not sufficient.
- Patent Document 4 discloses an adhesive tape in which an acrylic or silicone adhesive is applied to a film such as a biaxially stretched polypropylene film, but both surfaces are adhesive surfaces made of the same material. It was not possible to satisfy both the performances of winding the structure and fixing it to the exterior body.
- An object of the present invention is to provide a double-sided tape for fixing an electrode structure, which can wind the electrode structure and can fix the electrode structure to an exterior body even when an external force such as vibration is applied, And it is providing the secondary battery which fixed the electrode structure using this double-sided tape.
- the present inventors have found that the above object can be achieved by using a double-sided tape having a heat-sensitive adhesive layer on one side of the substrate and a pressure-sensitive adhesive layer on the other side, thereby completing the present invention. It came to do.
- a double-sided tape for fixing an electrode assembly comprising: a surface having a pressure-sensitive adhesive for bonding; and a surface having a heat-sensitive adhesive for bonding to the pouch-type exterior body
- the double-sided tape for fixing an electrode structure according to (1) wherein an outermost layer or an uppermost lower surface of the electrode structure is metal.
- the double-sided tape for fixing an electrode structure according to (1), wherein an outermost layer or an uppermost lower surface of the electrode structure is a resin.
- a pressure-sensitive adhesive layer formed using the pressure-sensitive adhesive on one side of the base material comprising (meth) acrylic acid alkyl ester and unsaturated carboxylic acid or its A double-sided tape for fixing an electrode assembly according to any one of (1) to (3), characterized in that it is formed of an acrylic pressure-sensitive adhesive and / or a rubber-based pressure-sensitive adhesive modified with a derivative, (5)
- a heat-sensitive adhesive layer formed using the heat-sensitive adhesive is provided on one side of a substrate, and the heat-sensitive adhesive layer is formed of a rubber-based pressure-sensitive adhesive or a modified polyolefin-based pressure-sensitive adhesive.
- the double-sided tape for fixing an electrode structure according to any one of (1) to (3), (6) A heat-sensitive adhesive layer formed on one surface of the substrate using the heat-sensitive adhesive, and a pressure-sensitive adhesive layer formed on the other surface of the substrate using the pressure-sensitive adhesive.
- the base material is made of polyolefin resin or polyester
- the pressure-sensitive adhesive layer is an acrylic adhesive modified with (meth) acrylic acid alkyl ester and unsaturated carboxylic acid or derivative thereof.
- Double-sided tape, (7) The melting point or bonding temperature of the heat-sensitive adhesive layer formed using the heat-sensitive adhesive is lower than the heat-sealing temperature for sealing the opening of the pouch-type exterior body.
- a secondary battery is provided in which the electrode structure is bonded and fixed to the pouch-type exterior body using the double-sided electrode fixing tape according to any one of (1) to (8).
- the electrode structure can be wound and the electrode structure can be fixed to the pouch-type exterior body even when an external force such as vibration is applied. Can do.
- the secondary battery which fixed the electrode structure using this double-sided tape can be provided.
- the double-sided tape for fixing an electrode assembly of the present invention (hereinafter sometimes simply referred to as “double-sided tape”) stores an electrode assembly in which a positive electrode member, a separator member and a negative electrode member are laminated or wound in a pouch-type exterior body.
- a double-sided tape for fixing an electrode assembly used for a secondary battery, a surface having a pressure-sensitive adhesive for adhering to the electrode assembly, and a surface having a heat-sensitive adhesive for adhering to the exterior body; Is provided.
- the double-sided tape of the present invention has a surface (pressure-sensitive adhesive layer) having a pressure-sensitive adhesive for adhering to an electrode assembly and a surface (thermal-sensitive adhesive) having a heat-sensitive adhesive for adhering to a pouch-type exterior body. Layer).
- the pressure sensitive adhesive layer is preferably formed on one side of the substrate, and the heat sensitive adhesive layer is preferably formed on the other side of the substrate.
- the material constituting the base material used for the double-sided tape of the present invention is not particularly limited.
- polyolefin such as polyethylene, polypropylene (PP), polyvinyl chloride, ethylene-vinyl acetate copolymer (EVA); polyethylene terephthalate (PET), Polybutylene terephthalate (PBT), Polyester such as polyethylene naphthalate (PEN); Polyarylate; Polyurethane; Polycarbonate; Polyamide; Polyimide (PI); Polyphenylene sulfide (PPS); Polytetrafluoroethylene and these
- the film which consists of a composite etc. is mentioned.
- it is preferable to use a flexible and stretchable polypropylene and it is more preferable to use an unstretched polypropylene having a high stretchability.
- Polypropylene is a homopolymer of propylene (hereinafter sometimes abbreviated as homo-PP), a random copolymer copolymerized with ethylene (hereinafter abbreviated as EPC), or polypropylene.
- EPC random copolymer copolymerized with ethylene
- polypropylene examples thereof include a block copolymer (hereinafter sometimes abbreviated as block PP) in which an elastomer component of an ethylene / propylene copolymer is blended at a molecular level during polymerization.
- the melting point of EPC resin is around 140 ° C.
- the melting point of homo PP and block PP is 160 ° C. to 165 ° C.
- the thickness of the polyolefin film is not particularly limited, but the film thickness is preferably in the range of 10 to 100 ⁇ m for ease of handling.
- the heat-sensitive adhesive constituting the heat-sensitive adhesive layer is a pressure-sensitive adhesive that does not show adhesiveness at room temperature, or has low adhesiveness and can be easily peeled off, and has heat melting properties that do not adversely affect battery performance.
- the tack strength at 25 ° C. is less than 0.8 N and the tack strength at 60 ° C. is 0.8 N or more.
- the tack strength is a value measured using a probe tack tester.
- an adhesive is applied to a 50 ⁇ m thick PET film at a thickness of 5 ⁇ m, and a probe tack tester ( TAC-1000), 10 mm ⁇ SUS probe, pressing speed 1 mm / sec, peeling speed 10 mm / sec, pressing pressure 0.98 N / cm 2 , pressing time 1 sec, probe temperature 25 ° C. Or it can measure at 60 degreeC.
- a probe tack tester TAC-1000
- 10 mm ⁇ SUS probe 10 mm ⁇ SUS probe
- pressing speed 1 mm / sec peeling speed 10 mm / sec
- pressing pressure 0.98 N / cm 2 pressing time 1 sec
- heat-sensitive adhesive include the above-mentioned properties among, for example, polyolefin pressure-sensitive adhesives such as rubber pressure-sensitive adhesives, acrylic pressure-sensitive adhesives, and modified polyolefin pressure-sensitive adhesives, modified acrylic pressure-sensitive adhesives, and silicone pressure-sensitive adhesives. Things.
- polyolefin-based pressure-sensitive adhesives such as modified polyolefin-based pressure-sensitive adhesives, modified acrylic pressure-sensitive adhesives, and rubber-based pressure-sensitive adhesives are preferable, and thermoplastic elastomers among rubber-based pressure-sensitive adhesives are most preferable.
- examples of the modified polyolefin pressure-sensitive adhesive include a pressure-sensitive adhesive mainly composed of an unsaturated carboxylic acid or an anhydride thereof, or a polyolefin modified with a silane coupling agent.
- unsaturated carboxylic acids or anhydrides thereof include acrylic acid, methacrylic acid, maleic acid, maleic anhydride, citraconic acid, citraconic anhydride, itaconic acid, itaconic anhydride, monoepoxy compounds of these derivatives and the above acids.
- examples include ester compounds, polymers having a group capable of reacting with these acids in the molecule, and reaction products of these acids. These metal salts can also be used.
- maleic anhydride is more preferably used. These can be used alone or in admixture of two or more.
- silane coupling agent for modifying the polyolefin examples include vinyltriethoxysilane, methacryloyloxytrimethoxysilane, and ⁇ -methacryloyloxypropyltriacetyloxysilane.
- the acrylic adhesive modified denatured using the (meth) acrylic-acid alkylester and unsaturated carboxylic acid or its derivative (s) is mentioned.
- (meth) acryl means both “acryl” and “methacryl”.
- the rubber-based pressure-sensitive adhesive include rubbers such as butyl rubber, butadiene rubber, isoprene rubber, EPDM, and pressure-sensitive adhesives containing modified products thereof.
- thermoplastic elastomer examples include a copolymer of an aromatic vinyl monomer and a conjugated diene monomer.
- diblock type block polymers such as styrene-butadiene block copolymer and styrene-isoprene block polymer; styrene-butadiene-styrene Triblock type block polymers such as block polymers, styrene-isoprene-styrene block polymers (SIS), styrene-butadiene-isoprene block polymers, styrene-isobutylene-styrene block polymers (SIBS); styrene-butadiene-styrene-butadiene block polymers, Styrene-isoprene-styrene-isoprene block poly
- the melting point or bonding temperature of the heat-sensitive adhesive layer needs to be lower than the cutoff temperature of the separator.
- a pouch-type exterior body made of a laminate material such as an aluminum laminate, but it is higher than the heat fusion temperature of the components used for laminating the pouch-type exterior body.
- the heat-sensitive adhesive layer needs to have a low melting point or bonding temperature.
- heat-sensitive adhesive layer when the heat-sensitive adhesive layer is bonded to the pouch-type exterior body, it is preferable to perform heat fusion at a temperature lower than the melting point of the substrate. If the substrate has low-temperature heat-fusibility, a heat-sensitive adhesive layer is considered unnecessary, but in that case, the substrate is likely to wrinkle in the process of applying and drying the pressure-sensitive adhesive, and it becomes easy to stretch and dimensional stability Therefore, it is necessary to provide a heat-sensitive adhesive layer.
- heat-sealing it is preferable to apply pressure in addition to the above heat. Specifically, heat fusion can be performed using a hot press machine or the like. The applied pressure is preferably 0.5 MPa or more and less than 2 MPa. If the pressure is less than 0.5 MPa, the effect of pressure is small, and if it is 2 MPa or more, the microporous portion of the separator in the secondary battery may be clogged, which may deteriorate the battery performance.
- an organic lubricant that imparts film slipperiness or an inorganic or organic antiblocking agent that prevents blocking may be added to the extent that adhesiveness and battery performance are not degraded.
- the pressure-sensitive adhesive constituting the pressure-sensitive adhesive layer is an adhesive that exhibits tackiness at room temperature.
- the pressure-sensitive adhesive is not particularly limited as long as it is a pressure-sensitive adhesive that does not adversely affect battery performance, but an adhesive having a tack strength at 25 ° C. of 0.8 N or more is preferable.
- the tack strength measurement method is the same as described above.
- Examples of the pressure-sensitive adhesive include those having the above characteristics among rubber-based adhesives, acrylic-based adhesives, silicone-based adhesives, and the like. Among these, acrylic adhesives and rubber adhesives are preferable.
- an acrylic pressure-sensitive adhesive for example, a main monomer capable of forming a polymer having a relatively low glass transition temperature (Tg), an adhesive property and a cohesive force, and a polymer having a relatively high Tg can be formed.
- a pressure-sensitive adhesive made of an acrylic copolymer obtained by polymerizing a monomer component such as a comonomer and a functional group-containing monomer capable of improving the formation of a crosslinking point and adhesiveness is used.
- Examples of the main monomer of the acrylic copolymer include, for example, ethyl acrylate, butyl acrylate, amyl acrylate, 2-ethylhexyl acrylate, acrylic acid alkyl esters such as octyl acrylate, and acrylic acid cyclohexane such as cyclohexyl acrylate.
- Aralkyl esters such as alkyl esters and benzyl acrylate, alkyl methacrylates such as butyl methacrylate and 2-ethylhexyl methacrylate, cycloalkyl methacrylates such as cyclohexyl methacrylate, and methacrylic acid aralkyl esters such as benzyl methacrylate.
- Examples of the comonomer include vinyl group-containing compounds such as methyl acrylate, methyl methacrylate, ethyl methacrylate, vinyl acetate, vinyl propionate, vinyl ether, styrene, acrylonitrile, and methacrylonitrile.
- Examples of the functional group-containing monomer include carboxyl group-containing monomers such as acrylic acid, methacrylic acid, crotonic acid, maleic acid, fumaric acid, and itaconic acid; 2-hydroxyethyl (meth) acrylate, 2-hydroxypropyl (meth) Hydroxyl group-containing monomers such as acrylate, 4-hydroxybutyl (meth) acrylate, N-methylolacrylamide, and allyl alcohol; 3 such as dimethylaminoethyl (meth) acrylate, diethylaminoethyl (meth) acrylate, and dimethylaminopropyl (meth) acrylate Secondary amino group-containing monomers; amide group-containing monomers such as acrylamide and methacrylamide; N-methyl (meth) acrylamide, N-ethyl (meth) acrylamide, N-methoxymethyl (meth) acryl Bromide, N- ethoxymethyl (meth) acrylamide, N-t
- an acrylic copolymer having excellent adhesiveness, cohesiveness, and durability can be obtained.
- an acrylic pressure-sensitive adhesive modified with the above (meth) acrylic acid alkyl ester and the unsaturated carboxylic acid exemplified above as the carboxyl group-containing monomer or a derivative thereof is preferable.
- a pressure-sensitive adhesive layer having arbitrary quality and characteristics according to the application can be formed by appropriately selecting a polymer as a main component of the pressure-sensitive adhesive.
- Examples of the rubber-based adhesive include natural rubber, butadiene rubber, isoprene rubber, chloroprene rubber, styrene-butadiene copolymer rubber, ethylene-propylene diene copolymer rubber, and acrylonitrile-butadiene copolymer rubber.
- halogenated rubber examples include halogenated butyl rubber such as brominated butyl rubber and chlorinated butyl rubber, halogenated isobutylene-paramethylstyrene copolymer (eg brominated), chloroprene rubber, epichlorohydrin rubber, Examples thereof include chlorosulfonated polyethylene, chlorinated polyethylene, maleic acid-modified chlorinated polyethylene, chlorinated acrylic rubber, fluororubber, epoxidized acrylic rubber, and acrylic rubber copolymerized with a halogen monomer.
- polybutadiene and polyisoprene having no polarity are preferable for reasons of resistance to dissolution in an electrolytic solution, and polybutadiene is particularly preferable.
- the weight average molecular weight of the polymer constituting the pressure sensitive adhesive is not particularly limited, but is, for example, 100,000 to 1,500,000, preferably 300,000 to 1,000,000. If the molecular weight is too small, the pressure-sensitive adhesive has poor adhesive strength and cohesive strength, and if the molecular weight is too large, the pressure-sensitive adhesive becomes hard and the adhesiveness becomes insufficient, so that the workability of sticking tends to deteriorate.
- the Tg of the polymer is not particularly limited, but is preferably ⁇ 20 ° C. or lower. When Tg is too high, the pressure-sensitive adhesive becomes hard depending on the use temperature, and the tackiness may not be maintained.
- the pressure-sensitive adhesive either a crosslinked type or a non-crosslinked type can be used.
- the pressure-sensitive adhesive may contain a crosslinking agent in addition to the polymer.
- a crosslinking agent it can select suitably according to the kind of the crosslinkable functional group which an adhesive has, for example, an epoxy type crosslinking agent, an isocyanate type crosslinking agent, a metal chelate type crosslinking agent, a metal alkoxide type crosslinking agent, a metal salt type Examples include a crosslinking agent, an amine-based crosslinking agent, a hydrazine-based crosslinking agent, and an aldehyde-based crosslinking agent. These crosslinking agents can be used alone or in combination of two or more.
- pressure sensitive adhesives include UV absorbers, tackifiers, softeners (plasticizers), anti-aging agents, stabilizers, fillers, pigments, dyes, and silane coupling agents as necessary.
- tackifier include rosin and derivatives thereof, polyterpene, terpene phenol resin, coumarone-indene resin, petroleum resin, styrene resin, xylene resin and the like.
- softening agent include liquid polyether, glycol ester, liquid polyterpene, liquid polyacrylate, phthalic acid ester, trimellitic acid ester, and the like.
- a release film is laminated on the heat-sensitive adhesive layer and / or the pressure-sensitive adhesive layer in order to protect the heat-sensitive adhesive layer and / or the pressure-sensitive adhesive layer. Also good.
- the release film those commonly used in the field of pressure-sensitive adhesive tapes or sheets can be used. For example, on a support made of a paper material such as glassine paper or a resin film such as polyethylene, polypropylene, polyester, etc. A film on which a mold release agent is formed can be used.
- the adhesive force between the double-sided tape of the present invention and the electrode structure is preferably 10 N / 15 mm or more.
- thermoforming the heat-sensitive adhesive layer and the pressure-sensitive adhesive layer of the above double-sided tape there are a co-extrusion method such as a T-die method and an inflation method, and a casting method.
- a cast method is preferred because a thin heat-sensitive adhesive layer and a pressure-sensitive adhesive layer can be easily formed.
- the thickness of the heat-sensitive adhesive layer is less than 1 ⁇ m, the heat-resisting heat and pressure cause the molten resin to flow and the heat-sensitive adhesive layer to become thin, resulting in a decrease in adhesive strength. For this reason, a thicker heat-sensitive adhesive layer is more advantageous for adhesion, but if it is too thick, the relative volume of the entire battery with respect to the electrode structure becomes large, so that the capacity characteristics of the battery are lowered, and economic efficiency is increased. From this point of view, the thickness of the heat-sensitive adhesive layer is preferably 1 to 10 ⁇ m.
- the thickness of the pressure sensitive adhesive layer is preferably 1 to 20 ⁇ m for the same reason as described above. More preferably, it is 2 to 10 ⁇ m.
- the positive electrode member used in the present invention is formed by laminating a positive electrode active material layer on a current collector.
- the positive electrode member is a positive electrode active material, a binder resin for the positive electrode, a solvent used for manufacturing the positive electrode, a water-soluble polymer used as necessary, and a slurry for the positive electrode containing other components such as a conductive additive. It can be obtained by applying to the surface and drying. That is, the positive electrode active material layer is formed on the current collector by applying the slurry for the positive electrode to the surface of the current collector and drying it. Alternatively, the positive electrode active material layer may be formed on the current collector by obtaining composite particles by granulating the positive electrode slurry and compression-molding the current on the current collector.
- the positive electrode active material when the electrochemical device of the present invention is a lithium ion secondary battery, an active material capable of doping and dedoping lithium ions is used, and the positive electrode active material is composed of an inorganic compound and an organic compound. Broadly divided.
- Examples of the positive electrode active material made of an inorganic compound include transition metal oxides, transition metal sulfides, lithium-containing composite metal oxides of lithium and transition metals, and the like.
- Examples of the transition metal include Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Mo.
- Transition metal oxides include MnO, MnO 2 , V 2 O 5 , V 6 O 13 , TiO 2 , Cu 2 V 2 O 3 , amorphous V 2 O—P 2 O 5 , MoO 3 , V 2 O. 5 , V 6 O 13 and the like. Among them, MnO, V 2 O 5 , V 6 O 13 and TiO 2 are preferable from the viewpoint of cycle stability and capacity.
- the lithium-containing composite metal oxide include a lithium-containing composite metal oxide having a layered structure, a lithium-containing composite metal oxide having a spinel structure, and a lithium-containing composite metal oxide having an olivine structure.
- lithium-containing composite metal oxide having a layered structure examples include lithium-containing cobalt oxide (LiCoO 2 ) (hereinafter sometimes referred to as “LCO”), lithium-containing nickel oxide (LiNiO 2 ), and Co—Ni—Mn.
- LCO lithium-containing cobalt oxide
- LiNiO 2 lithium-containing nickel oxide
- Co—Ni—Mn examples thereof include lithium composite oxides, lithium composite oxides of Ni—Mn—Al, and lithium composite oxides of Ni—Co—Al.
- lithium-containing composite metal oxide having a spinel structure examples include lithium manganate (LiMn 2 O 4 ) and Li [Mn 3/2 M 1/2 ] O 4 in which a part of Mn is substituted with another transition metal (here, M may be Cr, Fe, Co, Ni, Cu or the like.
- Li x MPO 4 (wherein, M is Mn, Fe, Co, Ni, Cu, Mg, Zn, V, Ca, Sr, Ba, Ti, Al, Lix MPO 4 ) as the lithium-containing composite metal oxide having an olivine structure.
- An olivine type lithium phosphate compound represented by at least one selected from Si, B, and Mo, 0 ⁇ X ⁇ 2) may be mentioned.
- a conductive polymer such as polyacetylene or poly-p-phenylene can be used.
- An iron-based oxide having poor electrical conductivity may be used as a positive electrode active material covered with a carbon material by allowing a carbon source material to be present during reduction firing. These compounds may be partially element-substituted.
- the positive electrode active material may be a mixture of the above inorganic compound and organic compound.
- the positive electrode active material may be any material that can reversibly carry lithium ions and anions such as tetrafluoroborate.
- carbon allotropes can be preferably used, and electrode active materials used in electric double layer capacitors can be widely used.
- Specific examples of the allotrope of carbon include activated carbon, polyacene (PAS), carbon whisker, carbon nanotube, and graphite.
- the volume average particle diameter of the positive electrode active material can reduce the blending amount of the binder resin for the positive electrode when preparing the positive electrode slurry, and can suppress the decrease in battery capacity, and the positive electrode slurry.
- the viscosity is preferably 1 to 50 ⁇ m, more preferably 2 to 30 ⁇ m.
- Binder resin for positive electrode examples include polyethylene, polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), tetrafluoroethylene-hexafluoropropylene copolymer (FEP), polyacrylic acid derivatives, polyacrylonitrile derivatives, and the like.
- a soft polymer such as an acrylic soft polymer, a diene soft polymer, an olefin soft polymer, and a vinyl soft polymer.
- a binder resin may be used individually by 1 type, and may be used combining two or more types by arbitrary ratios.
- water-soluble polymer used in the positive electrode slurry as needed include cellulose polymers such as carboxymethyl cellulose, methyl cellulose, ethyl cellulose and hydroxypropyl cellulose, and ammonium salts or alkali metal salts thereof, propylene glycol alginate.
- Alginate such as sodium alginate, polyacrylic acid and polyacrylic acid (or methacrylic acid) salt such as sodium polyacrylic acid (or methacrylic acid), polyvinyl alcohol, modified polyvinyl alcohol, poly-N- Vinylacetamide, polyethylene oxide, polyvinylpyrrolidone, polycarboxylic acid, oxidized starch, phosphate starch, casein, various modified starches, Chin, such as chitosan derivatives, and the like.
- “(modified) poly” means “unmodified poly” or “modified poly”.
- the water-soluble polymer refers to a polymer having an undissolved content of less than 10.0% by weight when 25 g of the polymer is dissolved in 100 g of pure water at 25 ° C.
- the conductive auxiliary agent used as necessary for the positive electrode slurry is not particularly limited as long as it is a conductive material, but a conductive particulate material is preferable, for example, furnace black, acetylene black, And conductive carbon black such as ketjen black; graphite such as natural graphite and artificial graphite; and carbon fibers such as polyacrylonitrile-based carbon fiber, pitch-based carbon fiber, and vapor grown carbon fiber.
- solvent used for preparation of positive electrode either water or an organic solvent may be used.
- organic solvent include cycloaliphatic hydrocarbons such as cyclopentane and cyclohexane; aromatic hydrocarbons such as toluene and xylene; ketones such as ethyl methyl ketone and cyclohexanone; ethyl acetate, butyl acetate, and ⁇ -butyrolactone Esters such as ⁇ -caprolactone; alkyl nitriles such as acetonitrile and propionitrile; ethers such as tetrahydrofuran and ethylene glycol diethyl ether: alcohols such as methanol, ethanol, isopropanol, ethylene glycol, and ethylene glycol monomethyl ether; N Amides such as -methylpyrrolidone and N, N-dimethylformamide; among them, N-methylpyrrolidon
- the amount of the solvent may be adjusted so that the viscosity of the positive electrode slurry is suitable for coating.
- the solid content concentration of the positive electrode slurry is preferably adjusted to 30 to 90% by weight, more preferably 40 to 80% by weight.
- the current collector As a material of the current collector used for the positive electrode member, for example, metal, carbon, conductive polymer, and the like can be used, and metal is preferably used.
- metal aluminum, platinum, nickel, tantalum, titanium, stainless steel, and other alloys are usually used, but copper, aluminum, or an aluminum alloy is used from the viewpoint of conductivity and voltage resistance. preferable.
- high-purity aluminum disclosed in JP 2001-176757 A can be suitably used.
- the current collector is in the form of a film or a sheet, and the thickness thereof is appropriately selected depending on the purpose of use, but is preferably 1 to 200 ⁇ m, more preferably 5 to 100 ⁇ m, and still more preferably 10 to 50 ⁇ m.
- the positive electrode member can be manufactured by forming a positive electrode active material layer on the current collector.
- Examples of the method for forming the positive electrode active material layer on the current collector include a method in which a positive electrode slurry is applied on the current collector and dried.
- the method for applying the positive electrode slurry to the surface of the current collector is not particularly limited. For example, a doctor blade method, a dip method, a reverse roll method, a direct roll method, a gravure method, an extrusion method, a brush coating method, and the like. Is mentioned.
- drying method examples 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 preferably 5 to 30 minutes, and the drying temperature is preferably 40 to 180 ° C.
- the porosity of the positive electrode active material layer can be lowered.
- the porosity is preferably 5% or more, more preferably 7% or more, preferably 30% or less, more preferably 20% or less.
- the porosity is too small, it is difficult to obtain a high volume capacity, and the positive electrode active material layer is easily peeled off from the current collector.
- the porosity is too large, the charging efficiency and the discharging efficiency are lowered.
- the positive electrode active material layer includes a curable polymer, it is preferable to cure the polymer after the positive electrode active material layer is formed.
- the composite particles When granulating the positive electrode slurry to obtain composite particles, the composite particles may be formed into a sheet and then laminated on the current collector. However, the composite particles may be rolled on the current collector.
- the positive electrode active material layer is preferably formed by a method of direct pressure molding such as pressure molding.
- separator member As the material of the separator constituting the separator member, for example, a polyolefin resin such as polyethylene or polypropylene, or a microporous film or nonwoven fabric containing an aromatic polyamide resin; a porous resin coat containing an inorganic ceramic powder; be able to.
- a polyolefin resin such as polyethylene or polypropylene, or a microporous film or nonwoven fabric containing an aromatic polyamide resin
- porous resin coat containing an inorganic ceramic powder be able to.
- microporous membranes made of polyolefin resins (polyethylene, polypropylene, polybutene, polyvinyl chloride) and mixtures or copolymers thereof; polyesters such as polyethylene terephthalate, polycycloolefins, polyether sulfones.
- a polyolefin-based resin or polyester it is preferable to use a polyolefin-based resin or polyester, the thickness of the whole separator can be reduced, and the active material ratio in the lithium ion secondary battery can be increased to increase the capacity per volume. Therefore, a microporous membrane made of polyolefin resin is more preferable.
- the thickness of the separator is preferably 0.5 to 40 ⁇ m from the viewpoint of reducing the internal resistance due to the separator in the lithium ion secondary battery and from the viewpoint of excellent workability when manufacturing the lithium ion secondary battery. More preferably, the thickness is 1 to 30 ⁇ m, still more preferably 1 to 25 ⁇ m.
- the negative electrode member used in the present invention is formed by laminating a negative electrode active material layer on a current collector.
- the negative electrode of the electrochemical device is a negative electrode active material, a binder resin for the negative electrode, a solvent used for preparing the negative electrode, a water-soluble polymer used as necessary, and a slurry for the negative electrode containing other components such as a conductive additive. It can be obtained by applying to the surface of the electric body and drying. That is, the negative electrode active material layer is formed on the current collector by applying the slurry for the negative electrode to the surface of the current collector and drying it. Alternatively, the negative electrode active material layer may be formed on the current collector by obtaining composite particles by granulating a slurry for the negative electrode and compression molding the current on the current collector.
- Examples of the negative electrode active material when the electrochemical device of the present invention is a lithium ion secondary battery include carbonaceous materials such as amorphous carbon, graphite, natural graphite, mesocarbon microbeads, pitch-based carbon fibers; Conductive polymers; metals such as silicon, tin, zinc, manganese, iron, nickel or alloys thereof; oxides or sulfates of the metals or alloys; metal lithium; Li—Al, Li—Bi—Cd, Li— Examples thereof include lithium alloys such as Sn—Cd; lithium transition metal nitrides; silicon and the like.
- a material obtained by attaching a conductive agent to the surface of the negative electrode active material particles by, for example, a mechanical modification method may be used.
- a negative electrode active material may be used individually by 1 type, and may be used combining two or more types by arbitrary ratios.
- the particle size of the negative electrode active material particles is usually selected as appropriate in consideration of other components of the electrochemical element.
- the 50% volume cumulative diameter of the negative electrode active material particles is preferably 1 to 50 ⁇ m, more preferably 15 to 30 ⁇ m.
- the content of the negative electrode active material in the negative electrode active material layer can increase the capacity of the lithium ion secondary battery, and improve the flexibility of the negative electrode and the binding property between the current collector and the negative electrode active material layer. From the viewpoint of achieving the above, it is preferably 90 to 99.9% by weight, more preferably 95 to 99% by weight.
- the negative electrode binder resin for example, the same positive electrode binder resin may be used.
- resins such as polyethylene, tetrafluoroethylene-hexafluoropropylene copolymer (FEP), polyacrylic acid derivatives, polyacrylonitrile derivatives; acrylic soft polymers, diene soft polymers, olefin soft polymers, Examples thereof include soft polymers such as vinyl-based soft polymers.
- a binder resin may be used individually by 1 type, and may be used combining two or more types by arbitrary ratios.
- the water-soluble polymer and conductive auxiliary used as necessary for the negative electrode slurry the water-soluble polymer and conductive auxiliary that can be used for the positive electrode slurry can be used.
- solvent used for preparation of negative electrode either water or an organic solvent may be used.
- organic solvent include cycloaliphatic hydrocarbons such as cyclopentane and cyclohexane; aromatic hydrocarbons such as toluene and xylene; ketones such as ethyl methyl ketone and cyclohexanone; ethyl acetate, butyl acetate, and ⁇ -butyrolactone Esters such as ⁇ -caprolactone; alkyl nitriles such as acetonitrile and propionitrile; ethers such as tetrahydrofuran and ethylene glycol diethyl ether: alcohols such as methanol, ethanol, isopropanol, ethylene glycol, and ethylene glycol monomethyl ether; N Amides such as -methylpyrrolidone and N, N-dimethylformamide; among them, N-methylpyrrolidon
- the amount of the solvent may be adjusted so that the viscosity of the negative electrode slurry is suitable for coating. Specifically, it is used by adjusting so that the solid content concentration of the slurry for negative electrode is preferably 30 to 90% by weight, more preferably 40 to 80% by weight.
- the current collector used for the negative electrode for example, a metal, carbon, a conductive polymer, or the like can be used, and a metal is preferably used. Usually, copper, platinum, nickel, tantalum, titanium, stainless steel, other alloys, etc. are used as the metal. Of these, copper is preferably used from the viewpoint of conductivity.
- the current collector is in the form of a film or a sheet, and the thickness thereof is appropriately selected depending on the purpose of use, but is preferably 1 to 200 ⁇ m, more preferably 5 to 100 ⁇ m, and still more preferably 10 to 50 ⁇ m.
- the negative electrode member can be produced by forming a negative electrode active material layer on the current collector.
- Examples of the method for forming the negative electrode active material layer on the current collector include a method in which a negative electrode slurry is applied on the current collector and dried.
- the method for applying the negative electrode slurry to the surface of the current collector is not particularly limited.
- a doctor blade method, a dip method, a reverse roll method, a direct roll method, a gravure method, an extrusion method, a brush coating method, and the like is not particularly limited.
- a doctor blade method for example, a doctor blade method, a dip method, a reverse roll method, a direct roll method, a gravure method, an extrusion method, a brush coating method, and the like. Is mentioned.
- drying method examples 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 preferably 5 to 30 minutes, and the drying temperature is preferably 40 to 180 ° C.
- the negative electrode active material layer is preferably subjected to pressure treatment using, for example, a die press or a roll press as necessary.
- the porosity is preferably 5% or more, more preferably 7% or more, preferably 30% or less, more preferably 20% or less.
- the porosity is too large, it is difficult to obtain a high volume capacity, and the negative electrode active material layer is easily peeled off from the current collector. On the other hand, if the porosity is too small, the rate characteristics are degraded.
- the negative electrode active material layer contains a curable polymer, it is preferable to cure the polymer after the formation of the negative electrode active material layer.
- the thickness of the negative electrode active material layer is not particularly limited, but is usually 5 to 1000 ⁇ m, preferably 20 to 500 ⁇ m, more preferably 30 to 300 ⁇ m.
- the composite particles When obtaining composite particles from the negative electrode slurry, the composite particles may be formed into a sheet and then laminated on the current collector. It is preferable to form the negative electrode active material layer by a direct pressure molding method.
- the lithium ion secondary battery using the double-sided tape of the present invention includes, for example, a method of obtaining an electrode structure, putting the electrode structure bonded with the double-sided tape of the present invention into a pouch-type exterior body, and sealing the same. It is done.
- the positive electrode member and the negative electrode member are overlapped via a separator member, and this is wound or folded according to the battery shape to obtain an electrode structure such as a wound body or a laminate.
- the double-sided tape of the present invention is affixed to the outermost layer or the uppermost lower surface of the electrode structure and is wound.
- a double-sided tape is affixed so that the surface bonded to the electrode structure becomes a pressure-sensitive adhesive layer.
- the outermost layer or the uppermost lower surface of the electrode structure is a current collector (metal) or a separator member (resin) constituting the positive electrode member or the negative electrode member.
- the positive electrode lead and the negative electrode lead which are thin metal plates for taking out electricity to the outside, are connected in advance to each of the positive electrode member and the negative electrode member in the electrode structure, or a tab is directly connected. It is necessary. When the lead is connected, it is necessary to be connected to the tab of the metal plate that is a member to be heat sealed with the pouch-type exterior body.
- the electrode assembly to which the double-sided tape is attached is accommodated in a pouch-type exterior body as a battery container.
- the material of the battery container (pouch-type outer package) in the present invention is a laminate film made of polyethylene or polypropylene resin, in which the innermost layer has heat sealability and includes an aluminum foil layer, Except for a part of the pouch-type exterior body that is an injection port for injection, heat sealing is performed including the tab.
- heat is applied to the flat pouch-type exterior body containing the electrode structure to which the double-sided tape is attached by applying heat at a predetermined temperature from the top and bottom of the flat plate for a predetermined time.
- the heat-sensitive adhesive layer of the tape is bonded to the inner surface of the exterior body. That is, the pouch-type exterior body and the electrode structure are bonded with a double-sided tape.
- the temperature at the time of bonding the pouch-type exterior body and the electrode structure with the double-sided tape is preferably lower than the temperature at which an opening of the pouch-type exterior body described later is sealed, and is preferably 80 to 100 ° C. .
- the opening of the pouch-type outer package is sealed with heat, whereby a lithium ion secondary battery is obtained.
- the temperature when sealing the opening of the pouch-type exterior body is usually 120 to 150 ° C.
- Examples of the electrolytic solution used for the lithium ion secondary battery include a nonaqueous electrolytic solution in which a supporting electrolyte is dissolved in a nonaqueous solvent.
- a lithium salt is preferably used as the supporting electrolyte.
- Examples of 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 the like.
- 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 preferable.
- One of these may be used alone, or two or more of these may be used in combination at any ratio. Since the lithium ion conductivity increases as the supporting electrolyte having a higher degree of dissociation is used, the lithium ion conductivity can be adjusted depending on the type of the supporting electrolyte.
- the concentration of the supporting electrolyte in the electrolytic solution is preferably used at a concentration of 0.5 to 2.5 mol / L depending on the type of the supporting electrolyte. If the concentration of the supporting electrolyte is too low or too high, the ionic conductivity may decrease.
- the non-aqueous solvent is not particularly limited as long as it can dissolve the supporting electrolyte.
- non-aqueous solvents include carbonates such as dimethyl carbonate (DMC), ethylene carbonate (EC), diethyl carbonate (DEC), propylene carbonate (PC), butylene carbonate (BC), methyl ethyl carbonate (MEC);
- DMC dimethyl carbonate
- EC ethylene carbonate
- DEC diethyl carbonate
- PC propylene carbonate
- BC butylene carbonate
- MEC methyl ethyl carbonate
- esters such as ⁇ -butyrolactone and methyl formate
- ethers such as 1,2-dimethoxyethane and tetrahydrofuran
- sulfur-containing compounds such as sulfolane and dimethyl sulfoxide
- ionic liquids used also as supporting electrolytes used also as supporting electrolytes.
- a non-aqueous solvent may be used individually by 1 type, and may be used combining two or more types by arbitrary ratios. In general, the lower the viscosity of the non-aqueous solvent, the higher the lithium ion conductivity, and the higher the dielectric constant, the higher the solubility of the supporting electrolyte, but since both are in a trade-off relationship, the lithium ion conductivity depends on the type of solvent and the mixing ratio. It is recommended to adjust the conductivity.
- the nonaqueous solvent may be used in combination or in whole or in a form in which all or part of hydrogen is replaced with fluorine.
- an additive may be included in the electrolytic solution.
- the additive include carbonates such as vinylene carbonate (VC); sulfur-containing compounds such as ethylene sulfite (ES); and fluorine-containing compounds such as fluoroethylene carbonate (FEC).
- An additive may be used individually by 1 type and may be used combining two or more types by arbitrary ratios.
- Capacity maintenance rate after vibration test The lithium ion secondary batteries obtained in the examples and comparative examples were charged to 4.2 V by a constant current method at a charge rate of 0.1 C at 60 ° C., and then discharged at a discharge rate of 0.1 C. A charge / discharge test was performed by repeating the cycle of discharging to 0 V five times, and the fifth discharge capacity was set as the initial capacity.
- this lithium ion secondary battery was fixed to a sieve having an inner diameter of 200 mm, vibrated with a low-tap type sieve shaker for 1 hour, then subjected to the same charge / discharge test as described above, and the discharge capacity after the vibration test was measured. .
- the ratio of the discharge capacity after the vibration test to the initial discharge capacity was determined as the capacity maintenance ratio. It shows that the capacity
- Capacity maintenance rate after high temperature storage The lithium ion secondary battery after confirming the initial capacity was charged to 4.2 V and stored in an environment of 60 ° C. for 30 days. Next, after performing a vibration test in the same manner as described above, the discharge capacity was measured. This discharge capacity was taken as the discharge capacity after storage at high temperature, and the discharge capacity after storage at high temperature relative to the initial discharge capacity was calculated. It shows that it is excellent in high temperature storage characteristics, so that this value is large.
- Example 1 (Production of double-sided tape) A homo PP film having a thickness of 20 ⁇ m was used as the base material of the double-sided tape.
- a rubber adhesive butadiene rubber (product name “Nipol BR1220”, manufactured by Nippon Zeon Co., Ltd.) 60 parts by weight and a styrene-isoprene-styrene block polymer (product name “Quintac 3620” Nippon Zeon) as a heat-sensitive adhesive on one side of the substrate A mixture of 40 parts by weight) was cast so that the thickness of the heat-sensitive adhesive layer was 4 ⁇ m and dried at 60 ° C. to form a heat-sensitive adhesive layer.
- butadiene rubber product name “Nipol BR1220”, manufactured by Nippon Zeon Co., Ltd.
- a styrene-isoprene-styrene block polymer product name “Quintac 3620” Nippon Zeon
- a pressure-sensitive adhesive layer is formed on the other surface of the substrate by applying a butyl acetate solution of a pressure-sensitive adhesive so that the thickness of the pressure-sensitive adhesive layer is 4 ⁇ m and drying.
- a pressure-sensitive adhesive an acrylic ester copolymer using 90 parts by weight of butyl acrylate and 10 parts by weight of acrylic acid as monomer components [weight average molecular weight (Mw) 500,000] 100 weights
- a crosslinking agent-containing acrylic pressure-sensitive adhesive composition comprising 2 parts by weight of trimethylolpropane tolylene diisocyanate (crosslinking agent).
- a binder resin 2.0 parts of a mixed polyvinylidene fluoride (a 1: 1 mixture of KYNARHSV900 and KYNAR720 manufactured by Arkema), which is a fluorine-containing polymer, is added with an appropriate amount of NMP, and stirred with a planetary mixer.
- a positive electrode slurry composition was prepared.
- An aluminum foil having a thickness of 15 ⁇ m was prepared as a current collector.
- the positive electrode slurry composition was applied to both sides of an aluminum foil so that the coating amount after drying was 25 mg / cm 2 , dried at 60 ° C. for 20 minutes, 120 ° C. for 20 minutes, and then heat-treated at 150 ° C. for 2 hours. Thus, a positive electrode raw material was obtained.
- This positive electrode original fabric was rolled with a roll press to produce a sheet-like positive electrode member comprising a positive electrode active material layer having a density of 3.9 g / cm 3 and an aluminum foil. This was cut into a width of 48 mm and a length of 50 cm, and an aluminum lead as a positive electrode lead was connected.
- a copper foil having a thickness of 15 ⁇ m was prepared as a current collector.
- the negative electrode slurry composition was applied on both sides of a copper foil so that the coating amount after drying was 10 mg / cm 2 , dried at 60 ° C. for 20 minutes, 120 ° C. for 20 minutes, and then heat-treated at 150 ° C. for 2 hours. Thus, a negative electrode raw material was obtained.
- This negative electrode original fabric was rolled with a roll press to produce a sheet-like negative electrode member comprising a negative electrode active material layer having a density of 1.8 g / cm 3 and a copper foil. This was cut into a width of 50 mm and a length of 52 cm, and a nickel lead as a negative electrode lead was connected.
- the obtained sheet-like positive electrode member and sheet-like negative electrode member were wound using a core having a diameter of 20 mm with a separator member interposed therebetween to obtain a wound body as an electrode structure.
- a separator member a polypropylene microporous film having a thickness of 20 ⁇ m was used.
- the wound body was compressed from one direction at a speed of 10 mm / second until a thickness of 4.5 mm was reached.
- the shape was substantially an ellipse, and the ratio of the major axis to the minor axis of the ellipse was 7.7.
- the pressure-sensitive adhesive layer side of the double-sided tape cut to 45 mm x 50 mm is opposed to the outermost layer of the wound body, and is attached and wound, and then accommodated in a predetermined aluminum laminate case as a pouch-type exterior body did. And after arrange
- the heat-sensitive adhesive layer of the double-sided tape and The inner surface of the pouch-type exterior body was adhered. That is, the pouch-type exterior body and the electrode structure were bonded with a double-sided tape.
- the shape of the obtained pouch-type battery was 35 mm wide, 48 mm high, and 5 mm thick.
- Example 2 In Example 1, instead of the crosslinker-containing acrylic pressure-sensitive adhesive composition as a pressure-sensitive adhesive, 100 parts by weight of natural rubber (pressure-sensitive adhesive component), 40 parts by weight of a terpene resin (tackifying resin), petroleum-based resin (A double-sided tape was prepared in the same manner as in Example 1 except that a pressure-sensitive adhesive comprising 30 parts by weight of a tackifying resin) and an anti-aging agent (trade name “Sumilyzer NW”, manufactured by Sumitomo Chemical Co., Ltd.) was used. A lithium ion secondary battery was produced.
- natural rubber pressure-sensitive adhesive component
- tackifying resin terpene resin
- petroleum-based resin A double-sided tape was prepared in the same manner as in Example 1 except that a pressure-sensitive adhesive comprising 30 parts by weight of a tackifying resin) and an anti-aging agent (trade name “Sumilyzer NW”, manufactured by Sumitomo Chemical Co., Ltd.) was used.
- a lithium ion secondary battery was produced
- Example 3 A styrene-isoprene-styrene block polymer (SIS) is used as a heat-sensitive adhesive instead of a rubber-based adhesive, and a butadiene rubber (product name “Nipol” is used as a pressure-sensitive adhesive in place of an acrylic pressure-sensitive adhesive composition containing a crosslinking agent.
- SIS styrene-isoprene-styrene block polymer
- Nipol butadiene rubber
- a double-sided tape and a lithium ion secondary battery were prepared in the same manner as in Example 1 except that “BR1220” (manufactured by Nippon Zeon Co., Ltd.) was used.
- Example 4 Styrene-isobutylene-styrene block polymer (SIBS) is used as a heat-sensitive adhesive instead of a rubber-based adhesive, and butadiene rubber (product name “Nipol” is used as a pressure-sensitive adhesive in place of an acrylic pressure-sensitive adhesive composition containing a crosslinking agent.
- SIBS Styrene-isobutylene-styrene block polymer
- Nipol butadiene rubber
- a double-sided tape and a lithium ion secondary battery were prepared in the same manner as in Example 1 except that “BR1220” (manufactured by Nippon Zeon Co., Ltd.) was used.
- Example 5 instead of rubber adhesives, polypropylene modified with maleic anhydride is used as a heat-sensitive adhesive, and butadiene rubber (product name “Nipol BR1220”, instead of an acrylic pressure-sensitive adhesive composition containing a crosslinking agent) as a pressure-sensitive adhesive.
- Nipol BR1220 butadiene rubber
- a double-sided tape and a lithium ion secondary battery were prepared in the same manner as in Example 1 except that Nippon Zeon Co., Ltd. was used.
- one pressure-sensitive adhesive layer of the double-sided pressure-sensitive adhesive tape is used as an electrode structure in the production of a lithium ion secondary battery.
- a release tape was attached to the other pressure-sensitive adhesive layer of the double-sided tape.
- the release tape was peeled off, and the aluminum laminate case and the electrode assembly with double-sided adhesive tape were bonded.
- a lithium ion secondary battery was produced in the same manner as in Example 1 except that the lithium ion secondary battery was produced in this manner.
- the double-sided thermal tape was placed at the center of the electrode assembly in the production of a lithium ion secondary battery.
- the four corners of the double-sided thermal tape were fixed to the electrode structure with imide tape so that the adhesive layer was in contact with the electrode structure (temporarily fixed).
- the electrode assembly with double-sided thermal tape was housed in an aluminum laminate case. After housing, a temperature of 80 ° C. and a pressure of 1 MPa were applied, and the electrode structure and the case were bonded via a double-sided thermal tape.
- a lithium ion secondary battery was produced in the same manner as in Example 1 except that the lithium ion secondary battery was produced in this manner.
- the pressure-sensitive adhesive layer of the double-sided tape was affixed to the electrode assembly and wound, and then housed in an aluminum laminate case. And after arrange
- the adhesive layer of the double-sided tape and the inner surface of the pouch-type exterior body are bonded to each other by contacting the electrolyte. It was. That is, the pouch-type exterior body and the electrode structure were bonded with a double-sided tape. Thereafter, the electrolyte injection port was sealed to complete a pouch-type lithium ion secondary battery.
- Example 6 A double-sided tape and a lithium ion secondary battery were prepared in the same manner as in Example 5 except that a plastic outer can was used instead of the aluminum laminate case.
- the pressure-sensitive adhesive layer of the double-sided tape and the electrode assembly were adhered, and then accommodated in a plastic outer can.
- the outer can was placed on a hot plate heated to 80 ° C. so that the heat-sensitive adhesive layer was on the hot plate side, and heated for 40 seconds.
- a double-sided tape for fixing an electrode structure used for an electrochemical element in which an electrode structure in which a positive electrode member, a separator member, and a negative electrode member are laminated or wound is stored in a pouch-type exterior body
- the peel strength of the double-sided tape for fixing an electrode assembly having a pressure-sensitive adhesive for adhering to the structure and a surface having a heat-sensitive adhesive for adhering to the exterior body is good.
- the capacity retention after the vibration test and the capacity retention after high-temperature storage of the lithium ion secondary battery using the tape were good (Examples 1 to 5).
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Abstract
Description
(1) 正極部材、セパレータ部材および負極部材を積層または捲回した電極構成体をパウチ型外装体内に格納した電気化学素子に用いる電極構成体固定用両面テープであって、前記電極構成体と接着するための感圧接着剤を有する面と、前記パウチ型外装体と接着するための感熱接着剤を有する面とを備えることを特徴とする電極構成体固定用両面テープ、
(2) 前記電極構成体の最外層または最上下面が金属であることを特徴とする(1)記載の電極構成体固定用両面テープ、
(3) 前記電極構成体の最外層または最上下面が樹脂であることを特徴とする(1)記載の電極構成体固定用両面テープ、
(4) 基材の片面に前記感圧接着剤を用いて形成された感圧接着剤層を備え、前記感圧接着剤層は、(メタ)アクリル酸アルキルエステルと、不飽和カルボン酸またはその誘導体とを用いて変性されたアクリル系粘着剤および/またはゴム系粘着剤で形成されることを特徴とする(1)~(3)の何れかに記載の電極構成体固定用両面テープ、
(5) 基材の片面に前記感熱接着剤を用いて形成された感熱接着剤層を備え、前記感熱接着剤層は、ゴム系粘着剤または変性ポリオレフィン系粘着剤で形成されることを特徴とする(1)~(3)の何れかに記載の電極構成体固定用両面テープ、
(6) 基材の一方の面に前記感熱接着剤を用いて形成された感熱接着剤層と、前記基材の他方の面に前記感圧接着剤を用いて形成された感圧接着剤層とを備え、前記基材は、ポリオレフィン樹脂またはポリエステルからなり、前記感圧接着剤層は、(メタ)アクリル酸アルキルエステルと、不飽和カルボン酸またはその誘導体とを用いて変性されたアクリル系粘着剤および/またはゴム系粘着剤で形成され、前記感熱接着剤層は、ゴム系粘着剤により形成されることを特徴とする(1)~(3)の何れかに記載の電極構成体固定用両面テープ、
(7) 前記パウチ型外装体の開口部を封口するための熱融着温度よりも、前記感熱接着剤を用いて形成された感熱接着剤層の融点または接着温度の方が低いことを特徴とする(1)~(6)の何れかに記載の電極構成体固定用両面テープ、
(8) 前記感熱接着剤は、ブロックポリマーである(1)~(7)の何れかに記載の電極構成体固定用両面テープ、
(9)(1)~(8)の何れかに記載の電極構成体固定用両面テープにより前記電極構成体が前記パウチ型外装体に接着固定されてなる二次電池
が提供される。
本発明の両面テープは、電極構成体と接着するための感圧接着剤を有する面(感圧接着剤層)と、パウチ型外装体と接着するための感熱接着剤を有する面(感熱接着剤層)とを有する。また、感圧接着剤層は基材の片面に形成され、感熱接着剤層は基材のもう一方の面に形成されることが好ましい。
本発明の両面テープに用いる基材を構成する材料としては、特に限定されないが、例えば、ポリエチレン、ポリプロピレン(PP)、ポリ塩化ビニル、エチレン-酢酸ビニル共重合体(EVA)などのポリオレフィン;ポリエチレンテレフタレート(PET)、ポリブチレンテレフタレート(PBT)、ポリエチレンナフタレート(PEN)などのポリエステル;ポリアリレート;ポリウレタン;ポリカーボネート;ポリアミド;ポリイミド(PI);ポリフェニレンサルファイド(PPS);ポリ4フッ化エチレン、及びこれらの複合体等がからなるフィルムが挙げられる。これらの中でも、柔軟性があり伸縮性のあるポリプロピレンを用いることが好ましく、さらに伸縮性の大きい、延伸されていないポリプロピレンを用いることがより好ましい。
ポリオレフィンフィルムの厚みは特に制限されないが、取扱いの容易性からフィルムの厚みは10~100μmの範囲であることが好ましい。
感熱接着剤層を構成する感熱接着剤は、常温では接着性を示さない、または接着性が弱く容易に剥離できるものであり、電池性能に悪影響を及ぼさない熱溶融性を有する粘着剤であれば特に限定されるものではないが、25℃におけるタック強度が0.8N未満であり、60℃におけるタック強度が0.8N以上であるものが好ましい。ここで、タック強度は、プローブタック試験機を用いて測定した値であり、具体的には、厚さ50μmのPETフィルム上に、接着剤を厚さ5μmで塗工し、プローブタック試験機(レスカ社製、TAC-1000)を用い、10mmφのSUS製プローブを使用して押付速度1mm/sec、引きはがし速度10mm/sec、押付圧力0.98N/cm2、押付時間1sec、プローブ温度25℃または60℃で測定できる。
感熱接着剤の種類としては、例えば、ゴム系粘着剤、アクリル系粘着剤、変性ポリオレフィン系粘着剤等のポリオレフィン系粘着剤、変性アクリル系粘着剤、シリコーン系粘着剤等の中で上記特性を有するものが挙げられる。なかでも変性ポリオレフィン系粘着剤等のポリオレフィン系粘着剤、変性アクリル系粘着剤、ゴム系粘着剤が好ましく、ゴム系粘着剤の中の熱可塑性エラストマーが最も好ましい。
ゴム系粘着剤としては、ブチルゴム、ブタジエンゴム、イソプレンゴム、EPDMなどのゴム、およびその変性体を含む粘着剤があげられる。
熱融着させる際には、上記の熱に加えてさらに圧力を付与するのが好ましい。具体的には、熱プレス機等を用いて熱融着させることができる。付与する圧力は、0.5MPa以上、2MPa未満が好ましい。0.5MPa未満では圧力の効果が少なく、2MPa以上では二次電池におけるセパレータの微多孔部を閉塞させてしまうことにより電池性能が悪化する可能性がある。
感圧接着剤層を構成する感圧接着剤は、常温で粘着性を示す接着剤である。感圧接着剤としては、電池性能に悪影響を及ぼさない粘着剤であれば特に限定されるものではないが、25℃におけるタック強度が0.8N以上であるものが好ましい。尚、タック強度の測定方法は前記同様である。
感圧接着剤の種類としては、例えば、ゴム系粘着剤、アクリル系粘着剤、シリコーン系粘着剤等の中で上記特性を有するものが挙げられる。これらの中でもアクリル系粘着剤、およびゴム系粘着剤が好ましい。
中でも、上記の(メタ)アクリル酸アルキルエステルと、上記においてカルボキシル基含有モノマーとして例示した不飽和カルボン酸、またはその誘導体とを用いて変性されたアクリル系粘着剤が好ましい。
このように、感圧接着剤の主成分となるポリマーを適宜選択することにより、用途に応じた任意の品質、特性を有する粘着剤層を形成することができる。
また、感圧接着剤層の厚みは、上記と同じ理由から1~20μmであることが好ましい。より好ましくは、2~10μmである。
本発明に用いる正極部材は、正極活物質層を集電体上に積層してなる。正極部材は、正極活物質、正極用結着樹脂、正極の作製に用いる溶媒、必要に応じて用いられる水溶性高分子、導電助剤等のその他の成分を含む正極用スラリーを集電体の表面に塗布し、乾燥させることにより得ることができる。即ち、正極用スラリーを集電体の表面に塗布し、乾燥させることにより集電体に正極活物質層が形成される。
また、正極用スラリーを造粒することにより複合粒子を得て、集電体上に圧縮成形することにより、集電体上に正極活物質層を形成してもよい。
本発明の電気化学素子がリチウムイオン二次電池である場合の正極活物質としては、リチウムイオンをドープ及び脱ドープ可能な活物質が用いられ、無機化合物からなるものと有機化合物からなるものとに大別される。
正極用結着樹脂としては、例えば、ポリエチレン、ポリテトラフルオロエチレン(PTFE)、ポリフッ化ビニリデン(PVDF)、テトラフルオロエチレン-ヘキサフルオロプロピレン共重合体(FEP)、ポリアクリル酸誘導体、ポリアクリロニトリル誘導体などの樹脂;アクリル系軟質重合体、ジエン系軟質重合体、オレフィン系軟質重合体、ビニル系軟質重合体等の軟質重合体等が挙げられる。なお、結着樹脂は、1種類を単独で用いてもよく、2種類以上を任意の比率で組み合わせて用いてもよい。
正極用スラリーに必要に応じて用いられる水溶性高分子の具体例としては、カルボキシメチルセルロース、メチルセルロース、エチルセルロースおよびヒドロキシプロピルセルロースなどのセルロース系ポリマー、ならびにこれらのアンモニウム塩またはアルカリ金属塩、アルギン酸プロピレングリコールエステルなどのアルギン酸エステル、ならびにアルギン酸ナトリウムなどのアルギン酸塩、ポリアクリル酸、およびポリアクリル酸(またはメタクリル酸)ナトリウムなどのポリアクリル酸(またはメタクリル酸)塩、ポリビニルアルコール、変性ポリビニルアルコール、ポリ-N-ビニルアセトアミド、ポリエチレンオキシド、ポリビニルピロリドン、ポリカルボン酸、酸化スターチ、リン酸スターチ、カゼイン、各種変性デンプン、キチン、キトサン誘導体などが挙げられる。なお、本発明において、「(変性)ポリ」は「未変性ポリ」又は「変性ポリ」を意味する。また、本発明において、水溶性高分子とは、25℃において、高分子0.5gを100gの純水に溶解させた場合の未溶解分が10.0重量%未満の高分子をいう。
正極の作製に用いる溶媒としては、水及び有機溶媒のいずれを使用してもよい。有機溶媒としては、例えば、シクロペンタン、シクロヘキサン等の環状脂肪族炭化水素類;トルエン、キシレン等の芳香族炭化水素類;エチルメチルケトン、シクロヘキサノン等のケトン類;酢酸エチル、酢酸ブチル、γ-ブチロラクトン、ε-カプロラクトン等のエステル類;アセトニトリル、プロピオニトリル等のアルキルニトリル類;テトラヒドロフラン、エチレングリコールジエチルエーテル等のエーテル類:メタノール、エタノール、イソプロパノール、エチレングリコール、エチレングリコールモノメチルエーテル等のアルコール類;N-メチルピロリドン、N,N-ジメチルホルムアミド等のアミド類;などが挙げられるが、中でもN-メチルピロリドン(NMP)が好ましい。なお、溶媒は、1種類を単独で用いてもよく、2種類以上を任意の比率で組み合わせて用いてもよい。中でも、溶媒としては水を用いることが好ましい。
正極部材に用いる集電体の材料としては、たとえば、金属、炭素、導電性高分子などを用いることができ、好適には金属が用いられる。金属としては、通常、アルミニウム、白金、ニッケル、タンタル、チタン、ステンレス鋼、その他の合金等が使用されるが、導電性、耐電圧性の面から、銅、アルミニウム又はアルミニウム合金を使用するのが好ましい。また、高い耐電圧性が要求される場合には特開2001-176757号公報等で開示される高純度のアルミニウムを好適に用いることができる。集電体は、フィルム又はシート状であり、その厚みは、使用目的に応じて適宜選択されるが、好ましくは1~200μm、より好ましくは5~100μm、さらに好ましくは10~50μmである。
正極部材は、集電体上に正極活物質層を形成することによって製造することができる。
集電体上に正極活物質層を形成するための方法としては、例えば、正極用スラリーを集電体上に塗布し、乾燥する方法が挙げられる。正極用スラリーを集電体の表面に塗布する方法は特に限定されないが、例えば、ドクターブレード法、ディップ法、リバースロール法、ダイレクトロール法、グラビア法、エクストルージョン法、およびハケ塗り法などの方法が挙げられる。
さらに、正極活物質層が硬化性の重合体を含む場合は、正極活物質層の形成後に重合体を硬化させることが好ましい。
セパレータ部材を構成するセパレータの材料としては、例えば、ポリエチレン、ポリプロピレンなどのポリオレフィン樹脂や、芳香族ポリアミド樹脂を含んでなる微孔膜または不織布;無機セラミック粉末を含む多孔質の樹脂コート;などを用いることができる。具体例を挙げると、ポリオレフィン系(ポリエチレン、ポリプロピレン、ポリブテン、ポリ塩化ビニル)、及びこれらの混合物あるいは共重合体等の樹脂からなる微多孔膜;ポリエチレンテレフタレート等のポリエステル、ポリシクロオレフィン、ポリエーテルスルフォン、ポリアミド、ポリイミド、ポリイミドアミド、ポリアラミド、ナイロン、ポリテトラフルオロエチレン等の樹脂からなる微多孔膜;ポリオレフィン系の繊維を織ったもの又はその不織布;絶縁性物質粒子の集合体等が挙げられる。これらの中でも、ポリオレフィン系の樹脂または、ポリエステルを用いることが好ましく、セパレータ全体の膜厚を薄くすることができ、リチウムイオン二次電池内の活物質比率を上げて体積あたりの容量を上げることができるため、ポリオレフィン系の樹脂からなる微多孔膜がより好ましい。
本発明に用いる負極部材は、負極活物質層を集電体上に積層してなる。電気化学素子の負極は、負極活物質、負極用結着樹脂、負極の作製に用いる溶媒、必要に応じて用いられる水溶性高分子、導電助剤等のその他の成分を含む負極用スラリーを集電体の表面に塗布し、乾燥させることにより得ることができる。即ち、負極用スラリーを集電体の表面に塗布し、乾燥させることにより集電体に負極活物質層が形成される。
また、負極用スラリーを造粒することにより複合粒子を得て、集電体上に圧縮成形することにより、集電体上に負極活物質層を形成してもよい。
本発明の電気化学素子がリチウムイオン二次電池である場合の負極活物質としては、例えば、アモルファスカーボン、グラファイト、天然黒鉛、メソカーボンマイクロビーズ、ピッチ系炭素繊維等の炭素質材料;ポリアセン等の導電性高分子;ケイ素、錫、亜鉛、マンガン、鉄、ニッケル等の金属又はこれらの合金;前記金属又は合金の酸化物又は硫酸塩;金属リチウム;Li-Al、Li-Bi-Cd、Li-Sn-Cd等のリチウム合金;リチウム遷移金属窒化物;シリコン等が挙げられる。また、負極活物質として、当該負極活物質の粒子の表面に、例えば機械的改質法によって導電剤を付着させたものを用いてもよい。また、負極活物質は、1種類を単独で用いてもよく、2種類以上を任意の比率で組み合わせて用いてもよい。
負極用結着樹脂としては、例えば、正極用結着樹脂と同様のものを用いても良い。また、例えば、ポリエチレン、テトラフルオロエチレン-ヘキサフルオロプロピレン共重合体(FEP)、ポリアクリル酸誘導体、ポリアクリロニトリル誘導体などの樹脂;アクリル系軟質重合体、ジエン系軟質重合体、オレフィン系軟質重合体、ビニル系軟質重合体等の軟質重合体等が挙げられる。なお、結着樹脂は、1種類を単独で用いてもよく、2種類以上を任意の比率で組み合わせて用いてもよい。
負極用スラリーに必要に応じて用いられる水溶性高分子、導電助剤としては、上述の正極用スラリーに用いることができる水溶性高分子および導電助剤をそれぞれ使用することができる。
負極の作製に用いる溶媒としては、水及び有機溶媒のいずれを使用してもよい。有機溶媒としては、例えば、シクロペンタン、シクロヘキサン等の環状脂肪族炭化水素類;トルエン、キシレン等の芳香族炭化水素類;エチルメチルケトン、シクロヘキサノン等のケトン類;酢酸エチル、酢酸ブチル、γ-ブチロラクトン、ε-カプロラクトン等のエステル類;アセトニトリル、プロピオニトリル等のアルキルニトリル類;テトラヒドロフラン、エチレングリコールジエチルエーテル等のエーテル類:メタノール、エタノール、イソプロパノール、エチレングリコール、エチレングリコールモノメチルエーテル等のアルコール類;N-メチルピロリドン、N,N-ジメチルホルムアミド等のアミド類;などが挙げられるが、中でもN-メチルピロリドン(NMP)が好ましい。なお、溶媒は、1種類を単独で用いてもよく、2種類以上を任意の比率で組み合わせて用いてもよい。中でも、溶媒としては水を用いることが好ましい。
負極に用いる集電体は、たとえば、金属、炭素、導電性高分子などを用いることができ、好適には金属が用いられる。金属としては、通常、銅、白金、ニッケル、タンタル、チタン、ステンレス鋼、その他の合金等が使用される。これらの中で導電性の面から、銅を使用するのが好ましい。集電体は、フィルム又はシート状であり、その厚みは、使用目的に応じて適宜選択されるが、好ましくは1~200μm、より好ましくは5~100μm、さらに好ましくは10~50μmである。
負極部材は、集電体上に負極活物質層を形成することによって製造することができる。
集電体上に負極活物質層を形成するための方法としては、例えば、負極用スラリーを集電体上に塗布し、乾燥する方法が挙げられる。
さらに、負極活物質層が硬化性の重合体を含む場合は、負極活物質層の形成後に重合体を硬化させることが好ましい。
本発明の両面テープを用いたリチウムイオン二次電池は、例えば、電極構成体を得て、本発明の両面テープを接着させた電極構成体をパウチ型外装体に入れ、封口する方法などが挙げられる。
リチウムイオン二次電池に用いる電解液としては、例えば、非水溶媒に支持電解質を溶解した非水電解液が挙げられる。支持電解質としては、リチウム塩が好ましく用いられる。リチウム塩としては、例えば、LiPF6、LiAsF6、LiBF4、LiSbF6、LiAlCl4、LiClO4、CF3SO3Li、C4F9SO3Li、CF3COOLi、(CF3CO)2NLi、(CF3SO2)2NLi、(C2F5SO2)NLiなどが挙げられる。中でも、溶媒に溶けやすく高い解離度を示すLiPF6、LiClO4、CF3SO3Liが好ましい。これらは1種類を単独で用いてもよく、2種類以上を任意の比率で組み合わせて用いてもよい。解離度の高い支持電解質を用いるほど、リチウムイオン伝導度が高くなるので、支持電解質の種類によりリチウムイオン伝導度を調節することができる。
実施例及び比較例において、剥離強度、振動試験後の容量維持率及び高温保存後の容量維持率の評価はそれぞれ以下のように行った。
実施例及び比較例において得られた両面テープを15mm幅に切断し、電極構成体側面をアルミ箔、銅箔及びPP製セパレータにそれぞれ貼り付け、引っ張り試験器を用いて50mm/分の速度で180°剥離強度を測定した。結果を表1に示す。
比較例5において得られた両面テープの外装体側面を、エチレンカーボネート及びエチルメチルカーボネートの混合溶媒(重量比にてエチレンカーボネート/エチルメチルカーボネート=3/7)中に、常温で1分間浸漬させた後、直ちに80℃のホットプレート上で外装体の内面に圧着し、混合溶媒を蒸発させたのちに冷却し、同様に剥離強度を測定した。結果を表1に示す。
実施例及び比較例において得られたリチウムイオン二次電池について、60℃で充電レート0.1Cとした定電流法により、4.2Vまで充電を行なった後、放電レート0.1Cにて、3.0Vまで放電するサイクルを5回繰り返す充放電試験を行い、5回目の放電容量を初期容量とした。
初期容量を確認後のリチウムイオン二次電池に対して、4.2Vまで充電し、60℃の環境下で30日間保存した。次に、上記と同様に振動試験した後に放電容量を測定した。この放電容量を高温保存後の放電容量とし、初期放電容量に対する高温保存後の放電容量を算出した。この値が大きいほど高温保存特性に優れることを示す。
(両面テープの作製)
両面テープの基材には、厚みが20μmのホモPPフィルムを用いた。基材の片面に感熱接着剤としてのゴム系接着剤(ブタジエンゴム(製品名「Nipol BR1220」、日本ゼオン社製)60重量部とスチレン-イソプレン-スチレンブロックポリマー(製品名「Quintac 3620」日本ゼオン社製)40重量部との混合物)を、感熱接着剤層の厚さが4μmになるようにキャストして、60℃で乾燥することにより、感熱接着剤層を形成した。
正極活物質としてLiCoO2、100部と、導電助剤としてアセチレンブラック(AB35,電気化学工業社製 デンカブラック粉状品=個数粒子径35nm、比表面積68m2/g)2.0部と、正極用結着樹脂として、フッ素含有重合体である混合ポリフッ化ビニリデン(アルケマ社製KYNARHSV900とKYNAR720との1:1混合物)2.0部を、適量のNMPを添加してプラネタリーミキサーにて撹拌し、正極用スラリー組成物を調製した。
負極活物質として球状人造黒鉛(粒子径=12μm)100部、負極用結着樹脂としてスチレンブタジエンゴム(粒子径180nm、ガラス転移温度=-40℃)1部、増粘剤としてカルボキシメチルセルロース1部及び適量の水をプラネタリーミキサーにて撹拌し、負極用スラリー組成物を調製した。
得られたシート状の正極部材およびシート状の負極部材を、セパレータ部材を介在させて直径20mmの芯を用いて捲回し、電極構成体としての捲回体を得た。セパレータ部材としては、厚さ20μmのポリプロピレン製微多孔膜を用いた。捲回体は、10mm/秒のスピードで厚さ4.5mmになるまで一方向から圧縮した。捲回体を芯の軸方向から見た場合の形状は略楕円であり、この楕円の短径に対する長径の比は7.7であった。
実施例1において、感圧接着剤として架橋剤含有アクリル系粘着剤組成物の代わりに、天然ゴム(粘着剤成分)100重量部、テルペン系樹脂(粘着付与樹脂)40重量部、石油系樹脂(粘着付与樹脂)30重量部、及び老化防止剤(商品名「スミライザーNW」、住友化学(株)製)からなる感圧接着剤を用いた以外は、実施例1と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。
感熱接着剤としてゴム系接着剤の代わりに、スチレン-イソプレン-スチレンブロックポリマー(SIS)を用い、感圧接着剤として架橋剤含有アクリル系粘着剤組成物の代わりに、ブタジエンゴム(製品名「Nipol BR1220」、日本ゼオン社製)を用いた以外は、実施例1と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。
感熱接着剤としてゴム系接着剤の代わりに、スチレン-イソブチレン-スチレンブロックポリマー(SIBS)を用い、感圧接着剤として架橋剤含有アクリル系粘着剤組成物の代わりに、ブタジエンゴム(製品名「Nipol BR1220」、日本ゼオン社製)を用いた以外は、実施例1と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。
感熱接着剤としてゴム系接着剤の代わりに、無水マレイン酸で変性したポリプロピレンを用い、感圧接着剤として架橋剤含有アクリル系粘着剤組成物の代わりに、ブタジエンゴム(製品名「Nipol BR1220」、日本ゼオン社製)を用いた以外は、実施例1と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。
両面テープの作製において、感熱接着剤層を形成しなかった以外は、実施例1と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。
両面テープの作製において、感熱接着剤層を形成しなかった以外は、実施例2と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。
両面テープの作製において、感熱接着剤層を形成せず、基材の両面に感圧接着剤としてのブタジエンゴム(製品名「Nipol BR1220」、日本ゼオン社製)を用い、感圧接着剤層を形成したこと以外は、実施例1と同様に両面テープの作製を行った。
両面テープの作製において、感圧接着剤層を形成せず、基材の両面に感熱接着剤としてのスチレン-イソプレン-スチレンブロックポリマー(SIS)を用い、感熱接着剤層を形成したこと以外は、実施例1と同様に両面テープの作製を行った。
両面テープの作製において、感熱接着剤層を形成する代わりに、電解液と接触後に接着力を発現する性質を有するオリエンテッドポリスチレンを用い、電解液と接触後に接着力を発現する接着剤層を形成し、感圧接着剤として架橋剤含有アクリル系粘着剤組成物の代わりに、ブタジエンゴム(製品名「Nipol BR1220」、日本ゼオン社製)を用いたこと以外は、実施例1と同様に両面テープの作製を行った。
その後、電解液注入口を封口し、パウチ型のリチウムイオン二次電池を完成した。
アルミラミネート製ケースに代えて、プラスチック製外装缶を用いたこと以外は、実施例5と同様に両面テープの作製及びリチウムイオン二次電池の作製を行った。リチウムイオン二次電池の作製においては、両面テープの感圧接着剤層と電極構成体を接着させ、その後、プラスチック製外装缶に収容した。次いで、80℃に加熱したホットプレート上に、感熱接着剤層がホットプレート側になるように外装缶を置き、40秒間加熱した。
Claims (9)
- 正極部材、セパレータ部材および負極部材を積層または捲回した電極構成体をパウチ型外装体内に格納した電気化学素子に用いる電極構成体固定用両面テープであって、
前記電極構成体と接着するための感圧接着剤を有する面と、前記パウチ型外装体と接着するための感熱接着剤を有する面とを備えることを特徴とする電極構成体固定用両面テープ。 - 前記電極構成体の最外層または最上下面が金属であることを特徴とする請求項1記載の電極構成体固定用両面テープ。
- 前記電極構成体の最外層または最上下面が樹脂であることを特徴とする請求項1記載の電極構成体固定用両面テープ。
- 基材の片面に前記感圧接着剤を用いて形成された感圧接着剤層を備え、
前記感圧接着剤層は、(メタ)アクリル酸アルキルエステルと、不飽和カルボン酸またはその誘導体とを用いて変性されたアクリル系粘着剤および/またはゴム系粘着剤で形成されることを特徴とする請求項1~3の何れか一項に記載の電極構成体固定用両面テープ。 - 基材の片面に前記感熱接着剤を用いて形成された感熱接着剤層を備え、
前記感熱接着剤層は、ゴム系粘着剤または変性ポリオレフィン系粘着剤で形成されることを特徴とする請求項1~3の何れか一項に記載の電極構成体固定用両面テープ。 - 基材の一方の面に前記感熱接着剤を用いて形成された感熱接着剤層と、
前記基材の他方の面に前記感圧接着剤を用いて形成された感圧接着剤層と
を備え、
前記基材は、ポリオレフィン樹脂またはポリエステルからなり、
前記感圧接着剤層は、(メタ)アクリル酸アルキルエステルと、不飽和カルボン酸またはその誘導体とを用いて変性されたアクリル系粘着剤および/またはゴム系粘着剤で形成され、
前記感熱接着剤層は、ゴム系粘着剤により形成されることを特徴とする請求項1~3の何れか一項に記載の電極構成体固定用両面テープ。 - 前記パウチ型外装体の開口部を封口するための熱融着温度よりも、前記感熱接着剤を用いて形成された感熱接着剤層の融点または接着温度の方が低いことを特徴とする請求項1~6の何れか一項に記載の電極構成体固定用両面テープ。
- 前記感熱接着剤は、ブロックポリマーである請求項1~7の何れか一項に記載の電極構成体固定用両面テープ。
- 請求項1~8の何れか一項に記載の電極構成体固定用両面テープにより前記電極構成体が前記パウチ型外装体に接着固定されてなる二次電池。
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US15/520,940 US10530012B2 (en) | 2014-11-18 | 2015-10-23 | Method for producing an electrochemical device |
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CN201580055311.0A CN106797055B (zh) | 2014-11-18 | 2015-10-23 | 使用双面胶带固定电极构成体的方法以及二次电池 |
PL15861350T PL3223356T3 (pl) | 2014-11-18 | 2015-10-23 | Zastosowanie taśmy dwustronnej do mocowania korpusu składowego elektrody, i bateria akumulatorowa |
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US10530012B2 (en) | 2020-01-07 |
EP3223356B1 (en) | 2020-08-05 |
KR102330760B1 (ko) | 2021-11-23 |
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CN106797055A (zh) | 2017-05-31 |
US20170346130A1 (en) | 2017-11-30 |
CN106797055B (zh) | 2020-11-17 |
JP6635043B2 (ja) | 2020-01-22 |
EP3223356A4 (en) | 2018-05-30 |
KR20170085053A (ko) | 2017-07-21 |
JPWO2016080143A1 (ja) | 2017-08-24 |
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PL3223356T3 (pl) | 2020-11-30 |
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