WO2017170720A1 - 蓄電デバイス用外装材、及び蓄電デバイス用外装材の製造方法 - Google Patents
蓄電デバイス用外装材、及び蓄電デバイス用外装材の製造方法 Download PDFInfo
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- WO2017170720A1 WO2017170720A1 PCT/JP2017/012964 JP2017012964W WO2017170720A1 WO 2017170720 A1 WO2017170720 A1 WO 2017170720A1 JP 2017012964 W JP2017012964 W JP 2017012964W WO 2017170720 A1 WO2017170720 A1 WO 2017170720A1
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- Prior art keywords
- layer
- base material
- isocyanate
- protective layer
- storage device
- Prior art date
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- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/116—Primary casings; Jackets or wrappings characterised by the material
- H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/116—Primary casings; Jackets or wrappings characterised by the material
- H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
- H01M50/1245—Primary casings; Jackets or wrappings characterised by the material having a layered structure characterised by the external coating on the casing
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/116—Primary casings; Jackets or wrappings characterised by the material
- H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
- H01M50/126—Primary casings; Jackets or wrappings characterised by the material having a layered structure comprising three or more layers
- H01M50/129—Primary casings; Jackets or wrappings characterised by the material having a layered structure comprising three or more layers with two or more layers of only organic material
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/131—Primary casings; Jackets or wrappings characterised by physical properties, e.g. gas permeability, size or heat resistance
- H01M50/133—Thickness
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/14—Primary casings; Jackets or wrappings for protecting against damage caused by external factors
- H01M50/145—Primary casings; Jackets or wrappings for protecting against damage caused by external factors for protecting against corrosion
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/183—Sealing members
- H01M50/186—Sealing members characterised by the disposition of the sealing members
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/183—Sealing members
- H01M50/19—Sealing members characterised by the material
- H01M50/193—Organic material
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/20—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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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B38/00—Ancillary operations in connection with laminating processes
- B32B2038/0052—Other operations not otherwise provided for
- B32B2038/0076—Curing, vulcanising, cross-linking
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2255/00—Coating on the layer surface
- B32B2255/06—Coating on the layer surface on metal layer
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2255/00—Coating on the layer surface
- B32B2255/20—Inorganic coating
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2255/00—Coating on the layer surface
- B32B2255/26—Polymeric coating
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/20—Properties of the layers or laminate having particular electrical or magnetic properties, e.g. piezoelectric
- B32B2307/206—Insulating
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/30—Properties of the layers or laminate having particular thermal properties
- B32B2307/31—Heat sealable
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2457/00—Electrical equipment
- B32B2457/10—Batteries
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2457/00—Electrical equipment
- B32B2457/16—Capacitors
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2553/00—Packaging equipment or accessories not otherwise provided for
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/131—Primary casings; Jackets or wrappings characterised by physical properties, e.g. gas permeability, size or heat resistance
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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
- 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
- Y02E60/13—Energy storage using capacitors
Definitions
- the present invention relates to a packaging material for a power storage device and a method for manufacturing a packaging material for a power storage device.
- secondary batteries such as lithium ion batteries, nickel metal hydride batteries, and lead acid batteries
- electrochemical capacitors such as electric double layer capacitors
- metal cans have been used as exterior materials used in lithium ion batteries, but multilayer films that are lightweight, have high heat dissipation properties, and can be manufactured at low cost are being used.
- the battery contents (positive electrode, separator, negative electrode, electrolyte, etc.) are covered with an exterior material including an aluminum foil layer in order to prevent moisture from entering the interior. It has been adopted.
- a lithium ion battery employing such a configuration is called an aluminum laminate type lithium ion battery.
- An aluminum laminate type lithium ion battery forms a recess in a part of the exterior material by cold molding, accommodates the battery contents in the recess, folds the remaining part of the exterior material, and heats the edge portion.
- An embossed type lithium ion battery sealed with a seal is known. (For example, refer to Patent Document 1).
- the deeper the recess formed by cold forming the more battery contents can be accommodated, so the energy density can be increased.
- the adhesive layer and the metal foil layer may break. For this reason, the exterior material is required to have good deep drawability.
- a nylon film may be used as a base material layer as the outermost layer of the exterior material.
- the nylon film is basic, there is a problem that when the nylon film is brought into contact with the electrolyte solution (acidic) for lithium ion battery, the nylon film is melted and the characteristics as the exterior material cannot be expressed. Nylon films are also less resistant to alcohol.
- the nylon film used for the base material layer has high water absorption, and the base material layer tends to contain water particularly in a high-humidity environment such as in-vehicle use or an environment where rainwater is likely to be flooded.
- a voltage is applied from the outside in that state, the insulation is lowered, and the metal foil layer bonded to the base material layer is energized, which adversely affects battery performance.
- the battery cell and the product housing are brought into close contact with each other with an adhesive tape (PSA tape).
- PSA tape adhesive tape
- the battery cell and the product housing may be separated from each other.
- the ionization cell is in a floating state in the product casing, and a load is applied to the terminal portion due to various vibrations, which may cause a short circuit. Therefore, the adhesiveness with the battery cell product housing
- one of the functions required by storage device manufacturers as one of the long-term reliability performances of storage devices for storage devices is a test for storing storage devices in a hot water environment for a certain period. At that time, there is a problem that peeling (hereinafter referred to as delamination) occurs between the base material layer and the metal foil layer of the exterior material over time.
- the present invention has been made in view of the above circumstances, and an object thereof is to provide an exterior material for an electricity storage device that has good electrolytic solution resistance and alcohol resistance and excellent adhesion to an adhesive tape. Furthermore, it aims at providing the exterior material for electrical storage devices which is excellent also in high deep-drawing moldability, delamination-proof property, and insulation. Another object of the present invention is to provide a method for producing such an exterior material for an electricity storage device.
- the present invention comprises a structure in which at least a base material protective layer, a base material layer, an adhesive layer, a metal foil layer, a sealant adhesive layer, and a sealant layer are laminated in this order.
- the layer is a cured material of a raw material containing a polyester resin or acrylic resin and a curing agent, and the polyester resin or acrylic resin has a reactive group that reacts with the curing agent at the terminal or side chain, or both.
- the curing agent contains an isocyanate other than the alicyclic isocyanate and an alicyclic isocyanate, and the ratio of the weight [a] of the isocyanate other than the alicyclic isocyanate to the weight [b] of the alicyclic isocyanate ([a ] / [B]) is provided from 99/1 to 80/20.
- This exterior device for an electricity storage device has good electrolytic solution resistance and alcohol resistance, and is excellent in adhesion to an adhesive tape.
- a nylon film may be used for the outermost layer in a consumer electrical storage device exterior material in order to improve moldability.
- the nylon film is basic, if the electrolytic solution for an electricity storage device (acidic) comes into contact with the nylon film, the nylon dissolves and cannot be used as a battery cell.
- a coating layer in which a curing agent is blended with a polyester resin or an acrylic resin is provided as a base material protective layer on the outermost layer of the film. In that case, it is possible to give a suitable characteristic with respect to a coating layer by using resin and hardening
- the ratio ([B] / [A]) of the number of moles [B] of the reactive group of the curing agent to the number of moles [A] of the reactive group of the polyester resin or acrylic resin is 5 to 60. Is preferred. According to this, the moldability of the power storage device exterior material is improved. When the ratio [B] / [A] is less than 5, there are few reactive groups in the curing agent, and this tends to reduce the adhesion between the base material protective layer and the base material layer.
- the ratio [B] / [A] exceeds 60, the bond point between the polyester resin or acrylic resin and the curing agent tends to increase and the base material protective layer tends to be hard, and the deep drawing of the exterior material Sometimes cracks tend to occur, and it tends to be difficult to obtain high deep drawability. Further, when the ratio [B] / [A] is 5 to 20, the hardness of the base material protective layer can be suppressed while sufficiently ensuring the adhesion between the base material protective layer and the base material layer. It is possible to suppress cracks during deep drawing molding, and high insulation can be obtained in a deep drawing molded exterior material.
- the electrical resistance is preferably 2000 M ⁇ or more.
- the reactive groups of the polyester resin or acrylic resin are all hydroxyl groups, and the hydroxyl value of the polyester resin or acrylic resin is preferably 5 to 70 KOHmg / g.
- the isocyanate other than the alicyclic isocyanate is preferably an aliphatic isocyanate adduct or burette. According to these, the electrolytic solution resistance and alcohol resistance of the base material protective layer are further improved.
- the number average molecular weight of the polyester resin or acrylic resin is preferably 2000 to 30000.
- the electrolytic solution resistance of the base material protective layer is further improved when the base material protective layer is contacted with the electrolytic solution for an electricity storage device (acidic).
- the alcohol resistance of the substrate protective layer is further improved.
- the number average molecular weight exceeds 30000, the polyester resin or the acrylic resin becomes difficult to dissolve in the solvent, and it tends to be difficult to apply and form on the base material layer.
- the glass transition temperature (Tg) of the base material protective layer is preferably 60 to 140 ° C.
- the Tg is 60 to 140 ° C.
- the hardness of the base material protective layer can be made moderate while further suppressing the blocking during winding due to the low Tg of the base material protective layer. Resistance to delamination can be obtained.
- the base material protective layer may further contain a filler. Thereby, the slipperiness of the exterior material can be improved, and the exterior design can be imparted to the exterior material.
- the thickness of the base material protective layer is preferably 1 to 5 ⁇ m, and the ratio of the thickness of the base material protective layer to the thickness of the base material layer is preferably 35% or less.
- the ratio of the thickness of the base material protective layer is 35%, more sufficient deep drawing moldability can be obtained while having the role of protecting the base material layer.
- the thickness of the base material protective layer is less than 1 ⁇ m, the base material protective effect for preventing the permeation of moisture that penetrates and absorbs moisture from the surface of the base material protective layer tends to be small, and moisture tends to permeate. Lamination may occur, or the base material protective layer itself may break during molding. On the other hand, if the thickness exceeds 5 ⁇ m, delamination tends to occur because the base material protective layer itself may break during molding.
- the present invention includes a step of bonding a base material layer to one surface of the metal foil layer via an adhesive layer, a step of forming a base material protective layer on the surface opposite to the adhesive layer of the base material layer, And a step of forming a sealant layer on the surface opposite to the adhesive layer of the metal foil layer via the sealant adhesive layer, and the base material protective layer is a raw material containing a polyester resin or an acrylic resin and a curing agent
- the polyester resin or acrylic resin has a reactive group that reacts with the curing agent at the terminal or side chain, or both, and the curing agent is an isocyanate other than the alicyclic isocyanate and an alicyclic
- the ratio of the weight [a] of the isocyanate other than the alicyclic isocyanate to the weight [b] of the alicyclic isocyanate ([a] / [b]) is 99/1 to 80/20, Manufacture of exterior materials for electricity storage devices To provide a method.
- the present invention also includes a step of forming a base material protective layer on one surface of the base material layer, a surface of the base material layer opposite to the base material protective layer, and an adhesive layer on one side of the metal foil layer.
- a step of bonding the surfaces, and a step of forming a sealant layer on the surface opposite to the adhesive layer of the metal foil layer via the sealant adhesive layer, and the base material protective layer is made of a polyester resin or an acrylic resin.
- a cured product of a raw material containing a curing agent, the polyester resin or acrylic resin has a reactive group that reacts with the curing agent at the terminal or side chain, or both, and the curing agent is other than alicyclic isocyanate
- the ratio ([a] / [b]) of the weight [a] of the isocyanate other than the alicyclic isocyanate and the weight [b] of the alicyclic isocyanate is 99/1. 80/20 power storage device To provide a process for the preparation of the scan for the exterior materials.
- an exterior material for an electricity storage device that has good electrolytic solution resistance and alcohol resistance and is excellent in adhesion to an adhesive tape. Furthermore, it is possible to provide an exterior material for an electricity storage device that is also excellent in high deep drawability, delamination resistance, and insulation.
- the present invention can also provide a method for producing such an exterior material for an electricity storage device.
- FIG. 1 It is a schematic sectional drawing of the exterior material for electrical storage devices which concerns on one Embodiment of this invention. It is a figure which shows the embossing type exterior material obtained using the exterior material for electrical storage devices which concerns on one Embodiment of this invention, (a) is the perspective view, (b) is the embossing shown to (a). It is a longitudinal cross-sectional view along the bb line of the type exterior material.
- FIG. 1 It is a perspective view which shows the process of manufacturing a secondary battery using the exterior material for electrical storage devices which concerns on one Embodiment of this invention, (a) shows the state which prepared the exterior material for electrical storage devices, (b) Shows a state in which an exterior device for an electricity storage device and a battery element processed into an embossed type are prepared, (c) shows a state in which a part of the exterior material for an electricity storage device is folded and the end is melted, (d ) Shows a state where both sides of the folded portion are folded upward.
- FIG. 1 is a cross-sectional view schematically showing an embodiment of an exterior material for an electricity storage device of the present invention.
- an exterior material (exterior material for an electricity storage device) 10 of this embodiment includes a base material layer 11, a base material protective layer 12 provided on one surface side of the base material layer 11, An adhesive layer 13 provided on the opposite side of the substrate layer 11 from the substrate protective layer 12, and a corrosion prevention treatment layer 15 a on both sides provided on the opposite side of the adhesive layer 13 from the substrate layer 11,
- the metal foil layer 14 having 15b, the sealant adhesive layer 16 provided on the opposite side of the adhesive layer 13 of the metal foil layer 14, and the metal foil layer 14 provided on the opposite side of the sealant adhesive layer 16 It is a laminate in which the sealant layer 17 is laminated.
- the corrosion prevention treatment layer 15a is provided on the surface of the metal foil layer 14 on the adhesive layer 13 side
- the corrosion prevention treatment layer 15b is provided on the surface of the metal foil layer 14 on the sealant adhesion layer 16 side.
- the base material protective layer 12 is the outermost layer
- the sealant layer 17 is the innermost layer. That is, the exterior material 10 is used with the base material protective layer 12 facing the outside of the electricity storage device and the sealant layer 17 facing the inside of the electricity storage device.
- each layer will be described.
- the base material layer 11 provides heat resistance in a sealing process when manufacturing the electricity storage device, and plays a role of suppressing the generation of pinholes that can occur during molding and distribution.
- scratch resistance, chemical resistance, insulation, and the like can be imparted.
- the base material layer 11 is preferably a layer made of a resin film formed of an insulating resin.
- the resin film include stretched or unstretched films such as polyester films, polyamide films, and polypropylene films.
- the base material layer 11 may be a single layer film composed of any of these resin films, or may be a laminated film composed of two or more of these resin films.
- the base material layer 11 is preferably a polyamide film and more preferably a biaxially stretched polyamide film because of excellent moldability.
- the polyamide resin forming the polyamide film include nylon 6, nylon 6,6, a copolymer of nylon 6 and nylon 6,6, nylon 6,10, polymetaxylylene adipamide (MXD6), nylon 11 , Nylon 12 and the like.
- nylon 6 (ONy) is preferable from the viewpoint of excellent heat resistance, puncture strength, and impact strength.
- Examples of the stretching method for the biaxially stretched film include a sequential biaxial stretching method, a tubular biaxial stretching method, and a simultaneous biaxial stretching method.
- the biaxially stretched film is preferably stretched by a tubular biaxial stretching method from the viewpoint of obtaining better deep drawability.
- the thickness of the base material layer 11 is preferably 6 to 40 ⁇ m, and more preferably 10 to 30 ⁇ m. When the thickness of the base material layer 11 is 6 ⁇ m or more, there is a tendency that the pinhole resistance and the insulation of the power storage device exterior material 10 can be improved. If the thickness of the base material layer 11 exceeds 40 ⁇ m, the total thickness of the power storage device exterior material 10 becomes large, which is not desirable because it may be necessary to reduce the electric capacity of the battery.
- the base material protective layer 12 is a layer provided on one surface side of the base material layer 11 and is a layer formed using a polyester resin or an acrylic resin and a curing agent. That is, the base material protective layer 12 is a cured product of a raw material containing a polyester resin or an acrylic resin and a curing agent.
- the polyester resin is a copolymer made from a polyvalent carboxylic acid and a polyhydric alcohol as raw materials, and has a reactive group to be reacted with the curing agent at a terminal, a side chain, or both.
- the polyester resin is preferably a polyester polyol.
- the polyester polyol include a polyester polyol obtained by reacting one or more dicarboxylic acids with a diol.
- dicarboxylic acid either an aliphatic dicarboxylic acid or an aromatic dicarboxylic acid can be used.
- specific examples include aliphatic dicarboxylic acids such as succinic acid, glutaric acid, adipic acid, pimelic acid, suberic acid, azelaic acid, sebacic acid and brassic acid; aromatic dicarboxylic acids such as isophthalic acid, terephthalic acid and naphthalenedicarboxylic acid. Is mentioned.
- diol examples include aliphatic diols such as ethylene glycol, propylene glycol, butanediol, neopentyl glycol, methylpentanediol, hexanediol, heptanediol, octanediol, nonanediol, decanediol, and dodecanediol; cyclohexanediol, water
- diol examples include aliphatic diols such as added xylylene glycol; and aromatic diols such as xylylene glycol.
- examples of the raw material for the polyester polyol include polyester polyols obtained by reacting the dicarboxylic acid with one or more compounds having three or more hydroxyl groups.
- the unreacted site is the terminal or side chain of the polyester polyol, or both hydroxyl groups.
- examples of the compound having three or more hydroxyl groups include hexanetriol, trimethylolpropane, and pentaerythritol.
- the acrylic resin is an acrylic polyol having a terminal unit or a side chain of the repeating unit, or both hydroxyl groups.
- the acrylic polyol include a copolymer obtained by copolymerizing at least a hydroxyl group-containing acrylic monomer and (meth) acrylic acid. In this case, it is preferable that a repeating unit derived from (meth) acrylic acid is contained as a main component.
- the hydroxyl group-containing acrylic monomer include 2-hydroxyethyl (meth) acrylate and 2-hydroxypropyl (meth) acrylate.
- alkyl (meth) acrylate monomers examples include methyl, ethyl, n-propyl, i-propyl, n -Butyl group, i-butyl group, t-butyl group, 2-ethylhexyl group, cyclohexyl group, etc.
- alkyl groups include methyl, ethyl, n-propyl, i-propyl, n -Butyl group, i-butyl group, t-butyl group, 2-ethylhexyl group, cyclohexyl group, etc.
- alkyl group examples include methyl, ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a t-butyl group, a 2-ethylhexyl group, and a cyclohexyl group.
- the hydroxyl value of the polyester resin or acrylic resin is preferably 5 to 70 KOHmg / g.
- the hydroxyl value is 5 or more, the adhesion between the base material protective layer 12 and the base material layer 11 is better expressed when a polyester resin or acrylic resin and a curing agent are appropriately blended as described below.
- the hydroxyl value is 70 or less, the molecular weight of the polyester resin or acrylic resin tends to increase, so that the film strength is improved, or the cross-linked structure is moderately dense and hardly brittle.
- the hydroxyl value of the polyester resin or acrylic resin is more preferably 30 to 70 KOHmg / g.
- the hydroxyl value can be measured, for example, by acetylating a hydroxyl group in a sample using acetic anhydride and titrating unused acetic acid with a potassium hydroxide solution.
- the number average molecular weight (Mn) of the polyester resin or acrylic resin is preferably 2000 or more from the viewpoint of resistance to chemicals such as an electrolytic solution for an electricity storage device (acidic) and alcohol. From the viewpoint of solubility, the number average molecular weight (Mn) is preferably 30000 or less. The value of this number average molecular weight can be measured by gel permeation chromatography (GPC).
- isocyanate other than alicyclic isocyanate and alicyclic isocyanate are used.
- Any of the isocyanates is a polyisocyanate containing a plurality of isocyanate groups (hereinafter sometimes simply referred to as “isocyanate” or “polyisocyanate compound”), and serves to crosslink the polyester resin or acrylic resin.
- isocyanate or “polyisocyanate compound” includes adducts, burettes, and isocyanurates (nurates) of the isocyanate.
- a polyfunctional aliphatic isocyanate compound a polyfunctional aromatic isocyanate compound, or a polyfunctional alicyclic isocyanate compound can be used.
- an aliphatic isocyanate compound can be preferably used.
- the mixture containing this aliphatic isocyanate type compound and an alicyclic isocyanate type compound may be sufficient.
- the exterior for the electricity storage device The material 10 has good electrolytic solution resistance and alcohol resistance, and has excellent adhesion to the adhesive tape.
- the ratio ([a] / [b]) of the weight [a] of the isocyanate other than the alicyclic isocyanate to the weight [b] of the alicyclic isocyanate is 99/1 to 80/20. .
- the ratio of the alicyclic isocyanate When the ratio of the alicyclic isocyanate is higher than this, the film quality as the coating layer becomes hard, and the moldability of the electricity storage device exterior material 10 is adversely affected. In addition, since the alicyclic isocyanate has a bulky structure, it easily penetrates various chemicals (electrolytic solution and alcohol). Therefore, if the ratio of the alicyclic isocyanate is higher than this, the chemical resistance and alcohol resistance are reduced. There is a risk of damage. Moreover, when the ratio of alicyclic isocyanate is lower than this, the adhesiveness with respect to an adhesive tape will be inferior.
- isocyanates other than alicyclic isocyanates include aliphatic and aromatic isocyanates.
- examples of the aliphatic isocyanate include hexamethylene diisocyanate (HDI), and examples of the aromatic isocyanate include tolylene diisocyanate (TDI) and diphenylmethane diisocyanate (MDI).
- HDI hexamethylene diisocyanate
- examples of the aromatic isocyanate include tolylene diisocyanate (TDI) and diphenylmethane diisocyanate (MDI).
- the polyfunctional isocyanate modified body etc. from 1 type, or 2 or more types of these diisocyanates are mentioned.
- aliphatic isocyanates are preferable, and adducts and burettes thereof are particularly preferable.
- an adduct or burette of hexamethylene diisocyanate is preferably used for imparting electrolyte resistance.
- these curing agents when these curing agents are used, alcohol resistance tends to be exhibited. For example, when a battery cell manufacturer prints with an inkjet printer for lot trace management, incorrect information may be printed. In that case, the printed part is wiped off with alcohol and printed again, but these curing agent types are also effective in improving the wiping resistance against the alcohol.
- Examples of the aliphatic isocyanate compound include hexamethylene diisocyanate (HDI) and xylylene diisocyanate (XDI).
- An example of the alicyclic isocyanate compound is isophorone diisocyanate (IPDI).
- Examples of the aromatic isocyanate compound include tolylene diisocyanate (TDI) and diphenylmethane diisocyanate (MDI).
- a multimer for example, trimer
- Such multimers are classified into adduct bodies, biuret bodies, nurate bodies, etc., but it is desirable to use an adduct body from the viewpoint of enhancing the deep drawability of the outer packaging material 10.
- an adduct of an aliphatic isocyanate compound or a mixture of this with an alicyclic isocyanate compound is used as the polyisocyanate compound, it can be deep-drawn while preventing the penetration of chemicals.
- the base material protective layer 12 excellent in the protective performance of the layer 11 can be formed.
- curing agents for the coating liquid which comprises the base-material protective layer 12 together.
- Other curing agents include melamine, a compound having a carboxyl group, a compound having a glycidyl group, and a hydroxyl group, depending on the terminal or side chain of the polyester resin or acrylic resin to be crosslinked, or both substituents. Examples thereof include compounds, carbodiimides, amides and amines.
- the blending ratio of the polyester resin or acrylic resin as the main agent and the curing agent is such that the number of reactive groups at the terminal or side chain of the polyester resin or acrylic resin, or both, is [A], and the reaction of the isocyanate curing agent.
- the ratio [B] / [A] is preferably 5 to 60 when the number of moles of the functional group is [B].
- the resistance to the electrolytic solution is considered to be affected by the cross-linked structure of the base material protective layer 12. Therefore, the inventor believes that the reactive group of the curing agent needs to be excessively blended with the reactive group of the polyester resin to increase the crosslink density. When [B] / [A] is 5 or more, the crosslinked structure is sufficient, and the electrolytic solution resistance is further improved.
- the crosslinked structure does not become too dense (the base material protective layer 12 does not become too hard), and has a favorable effect on molding and the like.
- curing agent ratios since it becomes difficult to obtain the adhesiveness of the base material protective layer 12 and the base material layer 11, it is preferable to set it as the said range.
- the ratio [B] / [A] is less than 5, there are few reactive groups of the polyisocyanate compound, and therefore the adhesion between the base material protective layer and the base material layer tends to be low.
- the ratio [B] / [A] is more preferably 5-20.
- the glass transition temperature (Tg) of the base material protective layer 12 is preferably 60 to 140 ° C.
- Tg is less than 60 ° C.
- the tackiness of the base material protective layer 12 tends to be high, so that blocking tends to occur, and the hardness as a cured film tends to be insufficient. There is a tendency not to be able to stop.
- the Tg is higher than 140 ° C., the cured film is too hard and becomes brittle, and there is a tendency that cold molding cannot be performed at a sufficient drawing depth.
- the base material protective layer 12 is formed using a raw material containing a polyester resin and a curing agent.
- the raw materials include fillers, flame retardants, lubricants (slip agents), antiblocking agents, antioxidants, light stabilizers, tackifiers, leveling agents for imparting coating stability, antifoaming agents, etc.
- Various additives such as a stabilizer, a catalyst for preventing blocking after coating (promoting the reaction of the coating liquid), a reaction retarding agent for controlling the pot life of the coating liquid (acetylacetone is preferably used) An agent may be included.
- the outer surface of the base material protective layer 12 can be matted.
- the base material protective layer 12 is a coating layer made of a raw material containing a polyester resin or acrylic resin and a curing agent, for example, a reaction is involved in comparison with nylon (base material layer itself). Therefore, it tends to be inferior in slipperiness and the moldability may be lowered. Therefore, by matting and adjusting the surface roughness, the slipperiness of the surface of the base material protective layer 12 is improved, and it is easy to suppress the exterior material 10 from being excessively adhered to the mold in cold forming. It is easy to ensure good moldability. Moreover, since the matte effect etc. are also acquired by mat
- fine particles (inorganic filler) of inorganic materials such as silica, alumina, barium sulfate, calcium carbonate, titanium oxide, acrylic beads, urethane beads, polyester beads (organic filler), and the like can be used.
- silica fine particles are preferable because resin cracking (whitening due to fine cracks) hardly occurs during press molding of the exterior material.
- the use of hydrophobic fine particles of silica as a filler improves the dispersibility during coating and allows the filler to be uniformly dispersed in the base material protective layer.
- the average particle size of the filler can be selected as necessary.
- the filler size is preferably from submicron (nm order) to less than 10 ⁇ m. At that time, fillers having different particle size distributions may be blended. The average particle diameter can be measured by a Coulter counter method.
- the filler content in the base material protective layer 12 is preferably 5 to 50% by mass.
- the content ratio of the filler 5% by mass or more it becomes easy to impart lubricity to the surface of the base material protective layer 12.
- the lubricant examples include fatty acid amides such as oleic acid amide, erucic acid amide, stearic acid amide, behenic acid amide, ethylene bisoleic acid amide, and ethylene biserucic acid amide.
- fatty acid amides such as oleic acid amide, erucic acid amide, stearic acid amide, behenic acid amide, ethylene bisoleic acid amide, and ethylene biserucic acid amide.
- various filler-based anti-blocking agents such as silica are preferable.
- the above-mentioned additives may be used alone or in combination of two or more.
- the thickness of the base material protective layer 12 is selected according to the required characteristics for the exterior material 10, and can be, for example, about 1 to 10 ⁇ m or 1 to 5 ⁇ m. If the thickness is less than 1 ⁇ m, there is a tendency that the substrate protection effect that prevents the penetration of moisture that penetrates and absorbs moisture from the surface of the substrate protective layer tends to be obtained, and delamination occurs because moisture easily penetrates. Alternatively, the base material protective layer itself may break during molding. On the other hand, if the thickness exceeds 5 ⁇ m, delamination tends to occur because the base material protective layer itself may break during molding.
- the ratio of the thickness of the base material protective layer to the thickness of the base material layer 11 is preferably 3.5 to 35% or less.
- the ratio of the thickness of the base material protective layer is 3.5 to 35%, it is possible to obtain more sufficient deep drawability while having the role of protecting the base material layer.
- the electrical resistance (insulation resistance) between the layers is preferably 2000 M ⁇ or more, and more preferably 10,000 M ⁇ or more.
- the insulation resistance between the base material protective layer 12 and the metal foil layer 14 is specifically the insulation resistance in the laminated portion of the base material protective layer 12, the base material layer 11, the adhesive layer 13, and the metal foil layer 14.
- Corrosion prevention treatment layers 15a and 15b may be provided on one surface or both surfaces of the metal foil layer 14, and the influence of the presence or absence of these layers on the insulation resistance value is negligible.
- the adhesive layer 13 is a layer that bonds the base material layer 11 and the metal foil layer 14 together.
- the adhesive layer 13 has an adhesive force necessary for firmly bonding the base material layer 11 and the metal foil layer 14, and the metal foil layer 14 is broken by the base material layer 11 during cold forming. It also has follow-up property for suppressing this (performance for reliably forming the adhesive layer 13 on the member without peeling even if the member is deformed / stretched).
- a curable polyurethane adhesive can be used.
- the molar ratio of the isocyanate group of the curing agent to the hydroxyl group of the main agent is preferably 1 to 10, more preferably 2 to 5.
- the polyurethane adhesive is subjected to aging at 40 ° C. or more for 4 days or more, for example, whereby the reaction between the hydroxyl group of the main agent and the isocyanate group of the curing agent proceeds, and the base material layer 11 and the metal foil layer This makes it possible to achieve a stronger bond with 14.
- the thickness of the adhesive layer 13 is preferably 1 to 10 ⁇ m and more preferably 2 to 6 ⁇ m from the viewpoint of obtaining desired adhesive strength, followability, workability, and the like.
- the pigment may be an organic or inorganic pigment, or a mixture of these pigments.
- the kind of pigment is not particularly limited when it is in a range that does not impair the adhesion of the adhesive layer 13.
- organic pigments include azo, phthalocyanine, quinacridone, anthraquinone, dioxazine, indigothioindigo, perinone-perylene, and isoindolenin
- inorganic pigments include carbon black.
- organic pigments for example, the following pigments can be used.
- Yellow isoindolinone, isoindoline, quinophthalone, anthraquinone (flavatron), azomethine, xanthene and the like.
- Orange diketopyrrolopyrrole, perylene, anthraquinone, perinone, quinacridone, etc.
- Red Anthraquinone, quinacridone, diketopyrrolopyrrole, perylene, indigoid and the like.
- the inorganic pigment for example, the following pigments can be used.
- White zinc white, lead white, lithopone, titanium dioxide, precipitated barium sulfate, barite powder, etc.
- Red Lead red, iron oxide red, etc.
- Yellow yellow lead, zinc yellow (Zinc Yellow 1 type, Zinc Yellow 2 type) and the like.
- Blue Ultramarine blue, prussian blue (potassium ferrocyanide), etc.
- Black Carbon black or the like.
- the content of the pigment based on the total mass of the adhesive layer 13 is preferably 1% by mass or more and more preferably 5% by mass or more because higher reliability is obtained. Moreover, since the outstanding adhesiveness is acquired, it is preferable that it is 50 mass% or less, and it is more preferable that it is 20 mass% or less.
- Metal foil layer 14 examples of the metal foil layer 14 include various metal foils such as aluminum and stainless steel, and the metal foil layer 14 is preferably an aluminum foil from the viewpoint of workability such as moisture resistance and spreadability, and cost.
- the aluminum foil may be a general soft aluminum foil, but is preferably an aluminum foil containing iron from the viewpoint of excellent pinhole resistance and extensibility during molding.
- the iron content is preferably 0.1 to 9.0% by mass, more preferably 0.5 to 2.0% by mass (for example, Aluminum foil made of 8021 material and 8079 material in the JIS standard).
- the iron content is 0.1% by mass or more, it is possible to obtain the exterior material 10 having more excellent pinhole resistance and spreadability.
- the iron content is 9.0% by mass or less, it is possible to obtain the exterior material 10 having more flexibility.
- a soft aluminum foil subjected to an annealing treatment is more preferable from the viewpoint of imparting the extensibility during desired molding.
- the metal foil used for the metal foil layer 14 is preferably subjected to a degreasing treatment, for example, in order to obtain a desired electrolytic solution resistance.
- the metal foil is preferably one whose surface is not etched.
- a degreasing process for example, a wet type degreasing process or a dry type degreasing process can be used, but a dry type degreasing process is preferable from the viewpoint of simplifying the manufacturing process.
- Examples of the dry-type degreasing treatment include a method of performing a degreasing treatment by increasing a treatment time in a step of annealing a metal foil. In the annealing treatment performed to soften the metal foil, sufficient electrolytic solution resistance can be obtained even with the degreasing treatment performed simultaneously.
- the dry type degreasing treatment treatments such as a frame treatment and a corona treatment which are treatments other than the annealing treatment may be used. Further, as the dry type degreasing treatment, for example, a degreasing treatment in which contaminants are oxidatively decomposed and removed by active oxygen generated when the metal foil is irradiated with ultraviolet rays having a specific wavelength may be used.
- the wet type degreasing treatment for example, acid degreasing treatment, alkali degreasing treatment or the like can be used.
- the acid used for the acid degreasing treatment include inorganic acids such as sulfuric acid, nitric acid, hydrochloric acid, and hydrofluoric acid. These acids may be used individually by 1 type, and may use 2 or more types together.
- an alkali used for an alkali degreasing process sodium hydroxide with a high etching effect can be used, for example.
- the wet type degreasing treatment described above can be performed, for example, by an immersion method or a spray method.
- the thickness of the metal foil layer 14 is preferably 9 to 200 ⁇ m, more preferably 15 to 150 ⁇ m, and further preferably 15 to 100 ⁇ m, from the viewpoint of barrier properties, pinhole resistance and workability. preferable.
- the thickness of the metal foil layer 14 is 9 ⁇ m or more, the metal foil layer 14 is hardly broken even when stress is applied by molding.
- the thickness of the metal foil layer 14 is 200 ⁇ m or less, an increase in mass of the exterior material can be reduced, and a decrease in weight energy density of the electricity storage device can be suppressed.
- the corrosion prevention treatment layers 15a and 15b serve to suppress the corrosion of the metal foil layer 14 due to the electrolytic solution or hydrofluoric acid generated by the reaction between the electrolytic solution and moisture.
- the corrosion prevention treatment layer 15 a plays a role of increasing the adhesion between the metal foil layer 14 and the adhesive layer 13.
- the corrosion prevention treatment layer 15 b plays a role of increasing the adhesion between the metal foil layer 14 and the sealant adhesive layer 16.
- the corrosion prevention treatment layer 15a and the corrosion prevention treatment layer 15b may be layers having the same configuration or different configurations.
- Corrosion prevention treatment layers 15a and 15b are, for example, coating agents having a degreasing treatment, a hydrothermal alteration treatment, an anodizing treatment, a chemical conversion treatment, and a corrosion prevention ability for a layer that is a base material of the corrosion prevention treatment layers 15a and 15b. It can be formed by carrying out a coating-type corrosion prevention treatment in which coating is applied, or a corrosion prevention treatment combining these treatments.
- degreasing treatment, hydrothermal modification treatment, anodizing treatment, particularly hydrothermal modification treatment and anodizing treatment are performed by dissolving the surface of the metal foil (aluminum foil) with a treating agent and having excellent corrosion resistance.
- This is a treatment for forming an aluminum compound (boehmite, anodized).
- such a treatment may be included in the definition of chemical conversion treatment in order to obtain a structure in which a co-continuous structure is formed from the metal foil layer 14 to the corrosion prevention treatment layers 15a and 15b.
- Degreasing treatment includes acid degreasing and alkali degreasing.
- the acid degreasing include a method using acid degreasing obtained by mixing inorganic acids such as sulfuric acid, nitric acid, hydrochloric acid, and hydrofluoric acid as described above alone or by mixing them.
- an acid degreasing agent in which a fluorine-containing compound such as monosodium ammonium difluoride is dissolved with the above-described inorganic acid is used, so that not only the degreasing effect of the metal foil layer 14 but also a passive metal fluoride is obtained. This is effective in terms of resistance to hydrofluoric acid.
- the alkaline degreasing include a method using sodium hydroxide and the like.
- hydrothermal modification treatment for example, boehmite treatment obtained by immersing the metal foil layer 14 in boiling water to which triethanolamine is added can be used.
- anodizing treatment for example, an alumite treatment can be used.
- chemical conversion treatment for example, chromate treatment, zirconium treatment, titanium treatment, vanadium treatment, molybdenum treatment, calcium phosphate treatment, strontium hydroxide treatment, cerium treatment, ruthenium treatment, or a combination of two or more of these is used. be able to.
- These hydrothermal modification treatment, anodizing treatment, and chemical conversion treatment are preferably performed in advance with the above-described degreasing treatment.
- the chemical conversion treatment is not limited to a wet method, and for example, a treatment agent used for these treatments may be mixed with a resin component and applied.
- a treatment agent used for these treatments may be mixed with a resin component and applied.
- coating type chromate process is preferable from a viewpoint of a waste liquid process.
- the coating agent used in the coating type corrosion prevention treatment for coating the coating agent having the corrosion prevention performance contains at least one selected from the group consisting of rare earth oxide sols, anionic polymers, and cationic polymers.
- a coating agent is mentioned.
- a method using a coating agent containing a rare earth element oxide sol is preferable.
- the method using the coating agent containing the rare earth element oxide sol is a pure coating type corrosion prevention treatment. By using this method, a corrosion prevention effect is imparted to the metal foil layer 14 even by a general coating method. It is possible. Moreover, the layer formed using the rare earth element oxide sol has a corrosion prevention effect (inhibitor effect) of the metal foil layer 14 and is also a material suitable from the environmental aspect.
- rare earth element oxide fine particles for example, particles having an average particle diameter of 100 nm or less
- examples of rare earth element oxides include cerium oxide, yttrium oxide, neodymium oxide, and lanthanum oxide. Of these, cerium oxide is preferable. Thereby, the adhesiveness between the metal foil layers 14 can be further improved.
- various solvents such as water, alcohol solvents, hydrocarbon solvents, ketone solvents, ester solvents, ether solvents and the like can be used. Of these, water is preferred.
- the rare earth element oxides contained in the corrosion prevention treatment layers 15a and 15b can be used singly or in combination of two or more.
- rare earth element oxide sols are used as dispersion stabilizers, such as inorganic acids such as nitric acid, hydrochloric acid and phosphoric acid, and organic substances such as acetic acid, malic acid, ascorbic acid and lactic acid. It is preferable to contain acids, salts thereof and the like. Of these dispersion stabilizers, it is particularly preferable to use phosphoric acid or phosphate.
- condensed phosphoric acid such as trimetaphosphoric acid, tetrametaphosphoric acid, hexametaphosphoric acid, and ultrametaphosphoric acid, or alkali metal salts and ammonium salts thereof are preferable for the functional expression as a power storage device exterior material.
- dry film-forming properties drying capacity, heat quantity
- the phosphate a water-soluble salt is preferable.
- the phosphoric acid or phosphate contained in the corrosion prevention treatment layers 15a and 15b can be used alone or in combination of two or more.
- the blending amount of phosphoric acid or a salt thereof in the rare earth element oxide sol is preferably 1 part by mass or more and more preferably 5 parts by mass or more with respect to 100 parts by mass of the rare earth element oxide.
- the upper limit of the phosphoric acid or salt thereof added to 100 parts by mass of the rare earth element oxide may be in a range not accompanied by a decrease in the function of the rare earth element oxide sol, and is 100 parts by mass or less with respect to 100 parts by mass of the rare earth element oxide.
- 50 parts by mass or less is more preferable, and 20 parts by mass or less is more preferable.
- the layer formed from the rare earth element oxide sol described above is an aggregate of inorganic particles, the cohesive force of the layer itself is low even after the drying curing process. Therefore, in order to supplement the cohesive force of this layer, it is preferable to make a composite with an anionic polymer.
- anionic polymer examples include a polymer having a carboxy group, and examples thereof include poly (meth) acrylic acid (or a salt thereof) or a copolymer obtained by copolymerizing poly (meth) acrylic acid as a main component.
- the copolymer component of the copolymer includes alkyl (meth) acrylate monomers (alkyl groups include methyl, ethyl, n-propyl, i-propyl, n-butyl, i-butyl, t-butyl group, 2-ethylhexyl group, cyclohexyl group, etc.); (meth) acrylamide, N-alkyl (meth) acrylamide, N, N-dialkyl (meth) acrylamide (alkyl groups include methyl, ethyl, n-propyl group, i-propyl group, n-butyl group, i-butyl group, t-butyl group, 2-ethylhexyl group, cyclohexyl group, etc.), N-alkoxy (meth) acrylamide, N, N- Dialkoxy (meth) acrylamide (alkoxy groups include methoxy, ethoxy
- vinylidene, ethylene, propylene, vinyl chloride, vinyl acetate, and butadiene examples include vinylidene, ethylene, propylene, vinyl chloride, vinyl acetate, and butadiene.
- the anionic polymer plays a role of improving the stability of the corrosion prevention treatment layers 15a and 15b (oxide layers) obtained using the rare earth element oxide sol. This is due to the effect of protecting the hard and brittle oxide layer with an acrylic resin component and the effect of capturing ion contamination (especially sodium ions) derived from phosphate contained in the rare earth oxide sol (cation catcher). Achieved. That is, when the corrosion prevention treatment layers 15a and 15b obtained using the rare earth element oxide sol contain alkali metal ions or alkaline earth metal ions such as sodium in particular, starting from the place containing the ions. The corrosion prevention treatment layers 15a and 15b are liable to deteriorate. Therefore, the resistance of the corrosion prevention treatment layers 15a and 15b is improved by fixing sodium ions and the like contained in the rare earth oxide sol by the anionic polymer.
- the corrosion prevention treatment layers 15a and 15b combined with the anionic polymer and the rare earth element oxide sol have the same corrosion prevention performance as the corrosion prevention treatment layers 15a and 15b formed by subjecting the metal foil layer 14 to the chromate treatment.
- the anionic polymer preferably has a structure in which a polyanionic polymer that is essentially water-soluble is crosslinked.
- the crosslinking agent used for forming the structure include compounds having an isocyanate group, a glycidyl group, a carboxy group, and an oxazoline group.
- Examples of the compound having an isocyanate group include diisocyanates such as tolylene diisocyanate, xylylene diisocyanate or hydrogenated products thereof, hexamethylene diisocyanate, 4,4′-diphenylmethane diisocyanate or hydrogenated products thereof, and isophorone diisocyanate compounds. Or adducts obtained by reacting these isocyanates with polyhydric alcohols such as trimethylolpropane, bures obtained by reacting with water, or isocyanurates which are trimers. Isocyanates; or block polyisocyanates obtained by blocking these polyisocyanates with alcohols, lactams, oximes, and the like.
- diisocyanates such as tolylene diisocyanate, xylylene diisocyanate or hydrogenated products thereof, hexamethylene diisocyanate, 4,4′-diphenylmethane diisocyanate or hydrogenated products thereof, and isophorone diis
- Examples of the compound having a glycidyl group include ethylene glycol, diethylene glycol, triethylene glycol, polyethylene glycol, propylene glycol, dipropylene glycol, tripropylene glycol, polypropylene glycol, 1,4-butanediol, 1,6-hexanediol, Epoxy hydrin was reacted with polyhydric alcohols such as epoxy compounds, glycerin, polyglycerin, trimethylolpropane, pentaerythritol, sorbyl, etc., which were reacted with glycols such as neopentyl glycol and epiquinol hydrin.
- Examples thereof include an epoxy compound, an epoxy compound obtained by reacting a dicarboxylic acid such as phthalic acid, terephthalic acid, oxalic acid, and adipic acid with epichlorohydrin.
- Examples of the compound having a carboxy group include various aliphatic or aromatic dicarboxylic acids, and it is also possible to use poly (meth) acrylic acid and alkali (earth) metal salts of poly (meth) acrylic acid. is there.
- the compound having an oxazoline group for example, a low molecular compound having two or more oxazoline units, or a polymerizable monomer such as isopropenyl oxazoline, (meth) acrylic acid, (meth) acrylic acid alkyl ester And a compound obtained by copolymerizing an acrylic monomer such as hydroxyalkyl (meth) acrylate.
- silane coupling agents include ⁇ -glycidoxypropyl-trimethoxysilane, ⁇ -glycidoxypropyltriethoxysilane, ⁇ - (3,4-epoxycyclohexyl) ethyltrimethoxysilane, ⁇ -chloropropylmethoxysilane, Vinyltrichlorosilane, ⁇ -mercaptopropyltrimethoxysilane, ⁇ -aminopropyltriethoxysilane, N- ⁇ (aminoethyl) - ⁇ -aminopropyltrimethoxysilane, ⁇ -isocyanatopropyltriethoxysilane, and particularly anions
- epoxy silane, amino silane, and isocyanate silane are preferable.
- the blending amount of the crosslinking agent is preferably 1 to 50 parts by mass and more preferably 10 to 20 parts by mass with respect to 100 parts by mass of the anionic polymer.
- the ratio of the crosslinking agent is 1 part by mass or more with respect to 100 parts by mass of the anionic polymer, a crosslinked structure is easily formed.
- the ratio of the crosslinking agent is 50 parts by mass or less with respect to 100 parts by mass of the anionic polymer, the pot life of the coating liquid is improved.
- the method of crosslinking the anionic polymer is not limited to the above-mentioned crosslinking agent, and may be a method of forming ionic crosslinking using a titanium or zirconium compound. Moreover, you may apply the coating composition which forms the corrosion prevention process layer 15a to these materials.
- the corrosion prevention treatment layers 15a and 15b by chemical conversion treatment represented by chromate treatment are formed with an inclined structure with the metal foil layer 14, and in particular, hydrofluoric acid, hydrochloric acid, nitric acid. Then, the metal foil layer 14 is treated using a chemical conversion treatment agent containing sulfuric acid or a salt thereof, and then a chemical conversion treatment layer is formed on the metal foil layer 14 by the action of a chromium-based or non-chromium-based compound.
- the said chemical conversion treatment uses the acid for a chemical conversion treatment agent, it is accompanied by deterioration of a working environment and corrosion of a coating apparatus.
- the coating-type corrosion prevention treatment layers 15a and 15b described above do not require an inclined structure to be formed on the metal foil layer 14. Therefore, the properties of the coating agent are not subject to restrictions such as acidity, alkalinity, and neutrality, and a good working environment can be realized.
- the chromate treatment using a chromium compound is preferably the coating-type corrosion prevention treatment layers 15a and 15b from the viewpoint that an alternative is required for environmental hygiene.
- the corrosion prevention treatment layers 15a and 15b may have a laminated structure in which a cationic polymer is further laminated as necessary.
- a cationic polymer examples include polyethyleneimine, an ionic polymer complex composed of polyethyleneimine and a polymer having a carboxylic acid, a primary amine-grafted acrylic resin in which a primary amine is graphed on an acrylic main skeleton, polyallylamine, or derivatives thereof. And aminophenol resins.
- Examples of the “polymer having a carboxylic acid” forming an ionic polymer complex include polycarboxylic acid (salt), a copolymer in which a comonomer is introduced into polycarboxylic acid (salt), a polysaccharide having a carboxy group, and the like. It is done.
- Examples of the polycarboxylic acid (salt) include polyacrylic acid or an ionic salt thereof.
- Examples of the polysaccharide having a carboxy group include carboxymethyl cellulose or an ionic salt thereof.
- Examples of the ionic salt include alkali metal salts and alkaline earth metal salts.
- the primary amine graph acrylic resin is a resin obtained by graphing a primary amine on an acrylic main skeleton.
- the acrylic main skeleton include various monomers used in the above-described acrylic polyol, such as poly (meth) acrylic acid.
- the primary amine graphed on the acrylic main skeleton include ethyleneimine.
- polyallylamine or derivatives thereof homopolymers or copolymers of allylamine, allylamine amide sulfate, diallylamine, dimethylallylamine, etc. can be used. Furthermore, these amines can be free amines or acetic acid or hydrochloric acid. Stabilized products can also be used. Further, maleic acid, sulfur dioxide or the like can be used as a copolymer component. Furthermore, it is possible to use a type in which a primary amine is partially methoxylated to impart thermal crosslinkability. These cationic polymers may be used alone or in combination of two or more. Among the above, the cationic polymer is preferably at least one selected from the group consisting of polyallylamine and derivatives thereof.
- the cationic polymer is preferably used in combination with a crosslinking agent having a functional group capable of reacting with an amine / imine such as a carboxy group or a glycidyl group.
- a crosslinking agent used in combination with the cationic polymer a polymer having a carboxylic acid that forms an ionic polymer complex with polyethyleneimine can also be used.
- a polycarboxylic acid (salt) such as polyacrylic acid or an ionic salt thereof, or the like
- a copolymer having a carboxy group such as carboxymethylcellulose or an ionic salt thereof.
- the cationic polymer is also described as one component constituting the corrosion prevention treatment layers 15a and 15b.
- the cationic polymer itself also has electrolyte solution resistance and hydrofluoric acid resistance. This is because it was found to be a compound capable of imparting. This factor is presumed to be because the metal foil layer 14 is prevented from being damaged by capturing fluorine ions with a cationic group (anion catcher).
- the cationic polymer is also very preferable in terms of improving the adhesion between the corrosion prevention treatment layer 15 b and the sealant adhesive layer 16.
- the cationic polymer is water-soluble like the anionic polymer described above, the water resistance can be improved by forming a crosslinked structure using the above-mentioned crosslinking agent.
- a crosslinked structure can be formed even if a cationic polymer is used, when a rare earth oxide sol is used for forming the corrosion prevention treatment layers 15a and 15b, an anionic polymer is used as the protective layer. Instead, a cationic polymer may be used.
- examples of combinations of the above-described coating type corrosion prevention treatments are as follows: (1) only rare earth oxide sol, (2) only anionic polymer, (3) only cationic polymer, (4) rare earth oxide Sol + anionic polymer (laminated composite), (5) rare earth oxide sol + cationic polymer (laminated composite), (6) (rare earth oxide sol + anionic polymer: laminated composite) / cationic polymer ( (Multilayered), (7) (rare earth oxide sol + cationic polymer: laminated composite) / anionic polymer (multilayered), and the like. Of these, (1) and (4) to (7) are preferable, and (4) to (7) are more preferable.
- the corrosion prevention treatment layer 15a (6) is particularly preferable because the corrosion prevention effect and the anchor effect (adhesion improvement effect) can be further realized.
- the corrosion prevention treatment layer 15b (6) and (7) are particularly preferable because the resistance to the electrolyte solution on the sealant layer 17 side can be more easily maintained.
- the present embodiment is not limited to the above combination.
- the cationic polymer is a very preferable material in that it has a good adhesiveness with the modified polyolefin resin mentioned in the description of the sealant adhesive layer 16 described later.
- the layer 16 is composed of a modified polyolefin resin, it is possible to design such that a cationic polymer is provided on the surface in contact with the sealant adhesive layer 16 (for example, configurations (5) and (6)).
- the corrosion prevention treatment layers 15a and 15b are not limited to the layers described above.
- it may be formed using an agent in which phosphoric acid and a chromium compound are blended in a resin binder (aminophenol resin or the like), such as a coating chromate that is a known technique. If this processing agent is used, it becomes possible to form a layer having both a corrosion prevention function and adhesion.
- the chemical conversion treatment layer a layer formed by degreasing treatment, hydrothermal modification treatment, anodizing treatment, chemical conversion treatment, or a combination of these treatments
- the cationic property described above is used.
- Corrosion treatment layer 15a per unit area of the 15b mass preferably in the range of 0.005 ⁇ 0.200g / m 2, more preferably in the range of 0.010 ⁇ 0.100g / m 2. If it is 0.005 g / m 2 or more, the metal foil layer 14 is easily imparted with a corrosion prevention function. Even if the mass per unit area exceeds 0.200 g / m 2 , the corrosion prevention function is saturated and no further effect can be expected. On the other hand, when the rare earth oxide sol is used, if the coating film is thick, curing due to heat at the time of drying becomes insufficient, and there is a possibility that the cohesive force is lowered. In addition, although it described with the mass per unit area in the said content, if specific gravity is known, it is also possible to convert thickness from there.
- the thickness of the corrosion prevention treatment layers 15a and 15b is preferably 10 nm to 5 ⁇ m, and more preferably 20 to 500 nm, from the viewpoint of the corrosion prevention function and the function as an anchor.
- the sealant adhesive layer 16 is a layer that bonds the metal foil layer 14 on which the corrosion prevention treatment layer 15 b is formed and the sealant layer 17.
- the exterior material 10 is roughly divided into a thermal laminate configuration and a dry laminate configuration depending on the adhesive component that forms the sealant adhesive layer 16.
- the adhesive component for forming the sealant adhesive layer 16 in the heat laminate configuration is preferably an acid-modified polyolefin resin obtained by graft-modifying a polyolefin resin with an acid. Since the acid-modified polyolefin-based resin has a polar group introduced in a part of the non-polar polyolefin-based resin, the acid-modified polyolefin-based resin has a polarity with the sealant layer 17 formed of a non-polar polyolefin-based resin film or the like. In many cases, it can be firmly adhered to both of the corrosion prevention treatment layers 15b.
- the use of the acid-modified polyolefin resin improves the resistance of the exterior material 10 to the contents such as the electrolyte, and even if hydrofluoric acid is generated inside the battery, the adhesive strength is reduced due to deterioration of the sealant adhesive layer 16. It is easy to prevent.
- polyolefin resin of the acid-modified polyolefin resin examples include low density, medium density and high density polyethylene; ethylene- ⁇ olefin copolymer; polypropylene; and propylene- ⁇ olefin copolymer.
- the polyolefin resin in the case of a copolymer may be a block copolymer or a random copolymer.
- a copolymer obtained by copolymerizing a polar molecule such as acrylic acid or methacrylic acid with the above-described one, or a polymer such as a crosslinked polyolefin can be used as the polyolefin resin.
- Examples of the acid that modifies the polyolefin resin include carboxylic acid, epoxy compound, and acid anhydride, and maleic anhydride is preferable.
- the acid-modified polyolefin resin used for the sealant adhesive layer 16 may be one type or two or more types.
- the sealant adhesive layer 16 having a heat laminate structure can be formed by extruding the adhesive component with an extrusion device.
- the thickness of the heat-bonded sealant adhesive layer 16 is preferably 8 to 50 ⁇ m.
- Examples of the adhesive component for forming the sealant adhesive layer 16 having a dry laminate structure include the same adhesives as those mentioned for the adhesive layer 13.
- the composition of the adhesive may be designed so that it is a main component of a skeleton that is difficult to hydrolyze and that can improve the crosslinking density. preferable.
- dimer fatty acid is an acid obtained by dimerizing various unsaturated fatty acids, and examples of the structure include acyclic, monocyclic, polycyclic and aromatic ring types.
- the fatty acid that is the starting material for the dimer fatty acid is not particularly limited. Moreover, you may introduce
- curing agent with respect to the main ingredient which comprises the sealant contact bonding layer 16 it is possible to use the isocyanate compound which can be used also as a chain extender of a polyester polyol, for example.
- the crosslinking density of the adhesive coating film increases, leading to improvements in solubility and swelling, and an increase in the urethane group concentration can also be expected to improve substrate adhesion.
- the sealant adhesive layer 16 having a dry laminate structure has a highly hydrolyzable bonding portion such as an ester group and a urethane group
- a heat laminate structure is used as the sealant adhesive layer 16 for applications requiring higher reliability. It is preferable to use the adhesive component.
- the above-mentioned various curing agents are blended in a coating liquid obtained by dissolving or dispersing an acid-modified polyolefin resin in a solvent such as toluene or methylcyclohexane (MCH), and then applied and dried.
- a sealant adhesive layer 16 is formed.
- the sealant adhesive layer 16 having a dry laminate structure may include a compound having a covalent bond with the corrosion prevention treatment layer 15b.
- the curing agent used in that case include at least one compound selected from the group consisting of polyfunctional isocyanate compounds, glycidyl compounds, compounds having a carboxy group, and compounds having an oxazoline group.
- the adhesive resin is easily oriented in the MD direction (extrusion direction) due to stress generated during the extrusion molding.
- an elastomer may be blended in the sealant adhesive layer 16 in order to relax the anisotropy of the sealant adhesive layer 16.
- blended with the sealant contact bonding layer 16 an olefin-type elastomer, a styrene-type elastomer, etc. can be used, for example.
- the average particle size of the elastomer is preferably a particle size that can improve the compatibility between the elastomer and the adhesive resin and can improve the effect of relaxing the anisotropy of the sealant adhesive layer 16.
- the average particle diameter of the elastomer is preferably 200 nm or less, for example.
- the average particle size of the elastomer can be obtained, for example, by taking a photograph of an enlarged cross section of the elastomer composition with an electron microscope and then measuring the average particle size of the dispersed crosslinked rubber component by image analysis. .
- the said elastomer may be used individually by 1 type, and may be used in combination of 2 or more type.
- the amount of the elastomer added to the sealant adhesive layer 16 (100% by mass) is, for example, preferably 1 to 25% by mass, and more preferably 10 to 20% by mass.
- the blending amount of the elastomer is 1% by mass or more, the compatibility with the adhesive resin is improved, and the effect of relaxing the anisotropy of the sealant adhesive layer 16 tends to be improved.
- sealant adhesive layer 16 for example, a dispersion type adhesive resin liquid in which an adhesive resin is dispersed in an organic solvent may be used.
- the thickness of the sealant adhesive layer 16 is preferably 8 to 50 ⁇ m and more preferably 20 to 40 ⁇ m in the case of a thermal laminate configuration. When the thickness of the sealant adhesive layer 16 is 8 ⁇ m or more, sufficient adhesive strength between the metal foil layer 14 and the sealant layer 17 can be easily obtained. It is possible to easily reduce the amount of moisture entering.
- the thickness of the sealant adhesive layer 16 is preferably 1 to 5 ⁇ m in the case of a dry laminate configuration. When the thickness of the sealant adhesive layer 16 is 1 ⁇ m or more, sufficient adhesion strength between the metal foil layer 14 and the sealant layer 17 is easily obtained, and when the thickness is 5 ⁇ m or less, the sealant adhesive layer 16 is not cracked. Can be suppressed.
- the sealant layer 17 is a layer that imparts a sealing property to the exterior material 10 by heat sealing, and is a layer that is arranged on the inner side and thermally fused when the power storage device is assembled.
- the sealant layer 17 include a polyolefin resin or a resin film made of an acid-modified polyolefin resin obtained by graft-modifying an acid such as maleic anhydride to a polyolefin resin.
- a polyolefin-based resin that improves the barrier property of water vapor and can form the electricity storage device without being excessively crushed by heat sealing is preferable, and polypropylene is particularly preferable.
- polystyrene resin examples include low density, medium density and high density polyethylene; ethylene- ⁇ olefin copolymer; polypropylene; and propylene- ⁇ olefin copolymer.
- the polyolefin resin in the case of a copolymer may be a block copolymer or a random copolymer. These polyolefin resin may be used individually by 1 type, and may use 2 or more types together.
- the sealant layer 17 is preferably a polyolefin-based resin that improves the barrier property of water vapor and can form the electricity storage device without being crushed excessively by heat sealing, and polypropylene is particularly preferable.
- each of the above-mentioned types of polypropylene that is, random polypropylene, homopolypropylene, and block polypropylene, includes a low crystalline ethylene-butene copolymer, a low crystalline propylene-butene copolymer, ethylene, butene, and propylene.
- a terpolymer made of a component copolymer, silica, zeolite, an antiblocking agent (AB agent) such as acrylic resin beads, a fatty acid amide slip agent, or the like may be added.
- Examples of the acid-modified polyolefin resin include the same as those mentioned in the sealant adhesive layer 16.
- the sealant layer 17 may be a single layer film or a multilayer film, and may be selected according to a required function.
- a multilayer film in which a resin such as an ethylene-cycloolefin copolymer and polymethylpentene is interposed can be used.
- sealant layer 17 may contain various additives such as a flame retardant, a slip agent, an antiblocking agent, an antioxidant, a light stabilizer and a tackifier.
- sealant layer 17 When a heat-weldable film formed by extrusion molding is used as the sealant layer 17, there is an orientation tendency in the extrusion direction of the heat-weldable film. For this reason, an elastomer may be blended in the heat-weldable film from the viewpoint of relaxing the anisotropy of the sealant layer 17 due to orientation. Thereby, it can suppress that the sealant layer 17 whitens when cold-molding the exterior
- the same material as the material exemplified as the elastomer constituting the sealant adhesive layer 16 can be used.
- the sealant layer 17 has a multilayer film structure
- at least one of the plurality of layers constituting the multilayer film structure may include an elastomer.
- the sealant layer 17 has a three-layer laminated structure composed of laminated random polypropylene layer / block polypropylene layer / random polypropylene layer
- the elastomer may be blended only in the block polypropylene layer or only in the random polypropylene layer. You may mix
- a lubricant may be included in order to impart slipperiness to the sealant layer 17.
- the sealant layer 17 contains the lubricant
- the content of the lubricant in the sealant layer 17 (100% by mass) is preferably 0.001 to 0.5% by mass.
- the content of the lubricant in the sealant layer 17 is preferably 0.001 to 0.5% by mass.
- There exists a tendency which can suppress more that the sealant layer 17 whitens at the time of cold molding as content of a lubricant is 0.001 mass% or more.
- there exists a tendency which can suppress the fall of the adhesive strength between the surfaces of the other layer which contacts the surface of the sealant layer 17 as content of a lubricant is 0.5 mass% or less.
- the thickness of the sealant layer 17 is preferably 10 to 100 ⁇ m, and more preferably 20 to 60 ⁇ m. When the thickness of the sealant layer 17 is 20 ⁇ m or more, sufficient heat seal strength can be obtained, and when it is 90 ⁇ m or less, the amount of water vapor entering from the edge of the exterior material can be reduced.
- Step S11 A step of forming the corrosion prevention treatment layer 15a on one surface of the metal foil layer 14 and the corrosion prevention treatment layer 15b on the other surface of the metal foil layer 14.
- Step S12 A step of bonding the surface of the corrosion prevention treatment layer 15a opposite to the metal foil layer 14 and the base material layer 11 via the adhesive layer 13.
- Process S13 The process of forming the base-material protective layer 12 in the surface on the opposite side to the contact bonding layer 13 of the base material layer 11.
- FIG. Step S14 A step of forming a sealant layer 17 via a sealant adhesive layer 16 on the surface of the corrosion prevention treatment layer 15b opposite to the metal foil layer 14.
- step S11 the corrosion prevention treatment layer 15a is formed on one surface of the metal foil layer 14, and the corrosion prevention treatment layer 15b is formed on the other surface of the metal foil layer 14.
- the corrosion prevention treatment layers 15a and 15b may be formed separately, or both may be formed at once.
- a corrosion prevention treatment agent base material of the corrosion prevention treatment layer
- 15a and 15b are formed at once.
- drying, curing, and baking are sequentially performed to form the corrosion prevention treatment layer 15 a, the same is applied to the other surface of the metal foil layer 14.
- the corrosion prevention treatment layer 15b may be formed.
- the order in which the corrosion prevention treatment layers 15a and 15b are formed is not particularly limited. Further, different corrosion prevention treatment agents may be used for the corrosion prevention treatment layer 15a and the corrosion prevention treatment layer 15b, or the same one may be used.
- As said corrosion prevention processing agent the corrosion prevention processing agent for coating type chromate processing etc. can be used, for example.
- the coating method of the corrosion inhibitor is not particularly limited. For example, gravure coating method, gravure reverse coating method, roll coating method, reverse roll coating method, die coating method, bar coating method, kiss coating method, comma coating method, small diameter gravure A method such as a coating method can be used.
- an untreated metal foil layer may be used, or a metal foil layer subjected to degreasing treatment by wet type degreasing treatment or dry type degreasing treatment may be used.
- step S12 In step S ⁇ b> 12, the surface of the corrosion prevention treatment layer 15 a opposite to the metal foil layer 14 and the base material layer 11 are bonded together by a technique such as dry lamination using an adhesive that forms the adhesive layer 13. At this time, in order to impart designability to the exterior material 10, the above-described pigment may be added to the adhesive.
- an aging treatment may be performed in the range of room temperature to 100 ° C. in order to promote adhesion. The aging time is, for example, 1 to 10 days.
- step S ⁇ b> 13 the base material protective layer 12 is formed on the surface of the base material layer 11 opposite to the adhesive layer 13.
- a material (coating solution) prepared by dissolving a raw material (polyester resin or acrylic resin) for forming the base material protective layer 12 in a solvent is prepared.
- a polyisocyanate and other curing agents are blended.
- various stabilizers such as a leveling agent and an antifoaming agent may be blended.
- Various catalysts may be blended to prevent blocking after coating, and to promote the reaction of the coating liquid.
- blend a reaction retarder for example, acetylacetone for pot life control of a coating liquid.
- this coating liquid is applied onto the base material layer 11 using a known method, and is heated and dried.
- a coating method include gravure direct, gravure reverse (direct, kiss), bar coater, and small-diameter gravure coating method.
- the slurry in which the filler is dispersed in the solvent in advance may be mixed with the varnished resin, or the filler may be directly dispersed in the already varnished resin coating liquid. Good. It is also possible to add other additives such as a curing agent to these filler compounding liquids.
- the timing which forms the base material protective layer 12 is not limited to this Embodiment.
- Step S14 After step S13, the base material protective layer 12, the base material layer 11, the adhesive layer 13, the corrosion prevention treatment layer 15a, the metal foil layer 14, and the corrosion prevention treatment layer 15b are laminated in this order on the corrosion prevention treatment layer 15b of the laminate.
- a sealant layer 17 is formed on the surface opposite to the metal foil layer 14 via a sealant adhesive layer 16.
- the sealant layer 17 may be laminated by dry lamination, sandwich lamination, or the like, or may be laminated together with the sealant adhesive layer 16 by a coextrusion method. From the viewpoint of improving adhesiveness, the sealant layer 17 is preferably laminated by, for example, sandwich lamination, or is preferably laminated by the coextrusion method together with the sealant adhesive layer 16, and more preferably by the coextrusion method.
- the exterior material 10 is obtained through the steps S11 to S14 described above. Note that the process sequence of the manufacturing method of the packaging material 10 is not limited to the method of sequentially performing the above steps S11 to S14. For example, the order of steps to be performed may be changed as appropriate, such as step S11 after step S12.
- the electricity storage device includes a battery element 1 including an electrode, a lead 2 extending from the electrode, and a container that houses the battery element 1, and the container is formed from an exterior material 10 for the electricity storage device, and a sealant layer 17 is disposed inside. Formed to be.
- the container may be obtained by stacking two exterior materials with the sealant layers 17 facing each other, and heat-sealing the peripheral edge of the overlaid exterior material 10, or by folding back one exterior material. It may be obtained by overlapping and similarly heat-sealing the peripheral portion of the exterior material 10.
- the electricity storage device may include the exterior material 20 as a container.
- the exterior material of this embodiment can be used in various power storage devices. Examples of such an electricity storage device include secondary batteries such as lithium ion batteries, nickel metal hydride batteries, and lead acid batteries, and electrochemical capacitors such as electric double layer capacitors.
- the lead 2 is sandwiched and sealed by an exterior material 10 that forms a container with the sealant layer 17 inside.
- the lead 2 may be clamped by the exterior material 10 via a tab sealant.
- FIG. 2 is a view showing the embossed type exterior member 30.
- FIGS. 3A to 3D are perspective views showing a manufacturing process of a one-side molded battery using the exterior material 10.
- the secondary battery 40 is a double-sided molded battery that is manufactured by bonding two exterior materials such as the embossed type exterior material 30 and bonding the exterior materials together while adjusting the alignment. Also good. Further, the embossed type exterior material 30 may be formed using the exterior material 20.
- the secondary battery 40 which is a one-side molded battery, can be manufactured, for example, by the following steps S21 to S26.
- Step S21 A step of preparing the outer packaging material 10, the battery element 1 including the electrodes, and the leads 2 extending from the electrodes.
- Step S22 A step of forming a recess 32 for disposing the battery element 1 on one side of the exterior material 10 (see FIGS. 3A and 3B).
- Step S23 The battery element 1 is arranged in the molding processing area (recessed portion 32) of the embossed-type exterior member 30, and the embossed-type exterior member 30 is folded and overlapped so that the lid portion 34 covers the recessed portion 32, and extends from the battery element 1.
- Step S24 Leave one side other than the side sandwiching the lead 2 and pressurize and melt the other side, then inject the electrolyte from the remaining side and pressurize and heat-bond the remaining side in a vacuum state Step (see FIG. 3C).
- Step S25 a step of performing chemical change (chemical conversion) by charging / discharging the current value, voltage value, environmental temperature, and the like under predetermined conditions.
- Step S26 a step of cutting the end of the press-fusing side other than the side sandwiching the lead 2 and bending it to the side of the molding area (recess 32) (see FIG. 3D).
- step S21 the exterior material 10, the battery element 1 including the electrodes, and the leads 2 extending from the electrodes are prepared.
- the exterior material 10 is prepared based on the above-described embodiment. There is no restriction
- a recess 32 for disposing the battery element 1 on the sealant layer 17 side of the exterior material 10 is formed.
- the planar shape of the recess 32 is a shape that matches the shape of the battery element 1, for example, a rectangular shape in plan view.
- the recess 32 is formed, for example, by pressing a pressing member having a rectangular pressure surface against a part of the exterior material 10 in the thickness direction. Further, the pressing position, that is, the recess 32 is formed at a position deviated from the center of the exterior material 10 cut into a rectangle toward one end in the longitudinal direction of the exterior material 10. Thereby, the other end part side which does not form the recessed part 32 after a shaping
- a method of forming the recess 32 includes a molding process using a mold (deep drawing molding).
- a molding method a female mold and a male mold disposed so as to have a gap larger than the thickness of the exterior material 10 are used, and the male mold is pushed into the female mold together with the exterior material 10. Is mentioned.
- the embossed type exterior material 30 is obtained by forming the recess 32 in the exterior material 10.
- the embossed type exterior member 30 has a shape as shown in FIG. 2, for example.
- FIG. 2 (a) is a perspective view of the embossed type exterior member 30, and
- FIG. 2 (b) is a longitudinal section along the line bb of the embossed type exterior member 30 shown in FIG. 2 (a).
- step S23 In step S ⁇ b> 23, the battery element 1 including the positive electrode, the separator, the negative electrode, and the like is disposed in the molding processing area (recess 32) of the embossed type exterior material 30. Further, the lead 2 extending from the battery element 1 and bonded to the positive electrode and the negative electrode, respectively, is drawn out from the molding area (recess 32). Thereafter, the embossed type exterior member 30 is folded back at substantially the center in the longitudinal direction, and the sealant layers 17 are stacked so as to be inside, and one side of the embossed type exterior member 30 sandwiching the lead 2 is subjected to pressure heat fusion.
- the pressure heat fusion is controlled by three conditions of temperature, pressure, and time, and is appropriately set. The temperature of the pressure heat fusion is preferably equal to or higher than the temperature at which the sealant layer 17 is melted.
- the thickness of the sealant layer 17 before heat sealing is preferably 40% or more and 80% or less with respect to the thickness of the lead 2.
- the thickness of the sealant layer 17 is equal to or greater than the lower limit value, the heat-sealing resin tends to sufficiently fill the end portion of the lead 2, and when the thickness is equal to or less than the upper limit value, The thickness of the end can be moderately suppressed, and the amount of moisture permeating from the end of the exterior material 10 can be reduced.
- step S24 one side other than the side sandwiching the lead 2 is left and the other side is subjected to pressure heat fusion. Thereafter, an electrolytic solution is injected from the remaining side, and the remaining side is pressurized and heat-sealed in a vacuum state. The conditions for the pressure heat fusion are the same as in step S23.
- Step S25 the secondary battery 40 obtained up to step S23 is charged and discharged to cause a chemical change (chemical conversion: 40 ° C. environment for 3 days). Then, in order to remove the gas generated by the chemical conversion or to replenish the electrolyte, the secondary battery 40 is opened once, and then final sealing is performed. This step S25 can be omitted.
- Step S26 Edge edges of the peripheral pressure heat-sealing side other than the sides sandwiching the lead 2 are cut, and the sealant layer 17 protruding from the ends is removed. Then, the secondary battery 40 is obtained by folding the peripheral pressure heat-sealed portion toward the molding area 32 and forming the folded portion 42.
- the present invention will be described more specifically based on examples.
- the lithium ion battery exterior material is taken up as an example of the electrical storage device exterior material, the present invention is not limited to the following examples.
- Example A1 the exterior material 10 for lithium ion batteries was produced by the following method. First, as the metal foil layer 14, a soft aluminum foil 8079 material (manufactured by Toyo Aluminum Co., Ltd.) having a thickness of 35 ⁇ m was prepared. Subsequently, sodium polyphosphate-stabilized cerium oxide sol (corrosion prevention treatment agent) was applied to both surfaces of the metal foil layer 14 by gravure coating using distilled water as a solvent and adjusting the solid content concentration to 10% by mass. At this time, phosphoric acid was 10 mass parts with respect to 100 mass parts of cerium oxide.
- a soft aluminum foil 8079 material manufactured by Toyo Aluminum Co., Ltd.
- sodium polyphosphate-stabilized cerium oxide sol corrosion prevention treatment agent
- a baking treatment is sequentially performed to form a corrosion prevention treatment layer 15a on one surface of the metal foil layer 14 and corrosion prevention on the other surface.
- a treatment layer 15b was formed.
- the baking conditions were a temperature of 150 ° C. and a processing time of 30 seconds.
- a polyurethane-based adhesive was applied as an adhesive layer 13 on the surface of the metal foil layer 14 opposite to the metal foil layer 14 of the corrosion prevention treatment layer 15a.
- the metal foil layer 14 and the corona-treated surface of the base material layer 11 were bonded via the adhesive layer 13 by a dry laminating method. Thereafter, the structure composed of the base material layer 11, the adhesive layer 13, the corrosion prevention treatment layer 15a, the metal foil layer 14, and the corrosion prevention treatment layer 15b is left in an atmosphere at a temperature of 60 ° C. for 6 days, thereby aging. Processed.
- a base material protective layer forming coating solution was prepared, applied to the surface of the base material layer 11 opposite to the adhesive layer 13, and dried to form a base material protective layer 12 having a thickness of 3 ⁇ m.
- the coating liquid for base-material protective layer formation was adjusted as follows. That is, a curing agent (adduct of hexamethylene diisocyanate as an isocyanate other than alicyclic isocyanate (HDI-A) and isophorone diisocyanate as an alicyclic isocyanate in a coating solution of a varnished resin (polyester polyol). 99/1 mixture with isocyanurate body).
- the blending amount of the curing agent was set so that the ratio ([B] / [A]) of the number of moles [B] of the reactive group of the curing agent to the number of moles [A] of the hydroxyl group of the polyester resin was 50.
- a maleic anhydride-modified polypropylene (trade name: Admer, manufactured by Mitsui Chemicals) as a base material and a sealant layer 17 as a sealant adhesive layer 16 are used.
- Admer sold by Mitsui Chemicals
- a sealant layer 17 as a sealant adhesive layer 16
- polypropylene was coextruded and bonded (heat-pressed) at 180 ° C. (pattern 2).
- the thickness of the sealant adhesive layer 16 was 15 ⁇ m
- the thickness of the sealant layer 17 was 20 ⁇ m. And thereby, the exterior material 10 for lithium ion batteries was produced.
- a lithium ion battery exterior material 10 was produced in the same manner as in Example A1, except that the base material protective layer composition and the composition pattern shown in Tables 1 and 2 were adopted.
- the end “-A” in the curing agent type indicates that it is an adduct, and the end “—N” indicates that it is an isocyanurate.
- the procedure was changed as follows to prepare exterior materials. (Examples A12 to A14, A16 and A18) A filler was blended into the varnished resin.
- Examples A17 and A18 A polyurethane-based adhesive prepared by mixing polyisocyanate with acid-modified polyolefin dissolved in a mixed solvent of toluene and methylcyclohexane was applied to the surface of the corrosion prevention treatment layer 15b opposite to the metal foil layer. Next, by a dry laminating method, a polyolefin film having a thickness of 30 ⁇ m (a film obtained by corona-treating the surface of the non-stretched polypropylene film on the side of the sealant adhesive layer 16) and the metal foil layer 14 through the sealant adhesive layer 16. And were adhered.
- the structure composed of the base material layer 11, the adhesive layer 13, the corrosion prevention treatment layer 15a, the metal foil layer 14, the corrosion prevention treatment layer 15b, the sealant adhesion layer 16, and the sealant layer 17 is placed in an atmosphere having a temperature of 40 ° C. Aging treatment was carried out by leaving it for 6 days. Except this, a lithium ion battery exterior material 10 was produced in the same manner as in Example A1 (Pattern 1).
- Tables 1 and 2 The meanings of terms in Tables 1 and 2 are as follows.
- HDI Hexamethylene diisocyanate
- TDI Tolylene diisocyanate
- IPDI Isophorone diisocyanate
- Pattern 1 Dry laminate configuration
- Pattern 2 Thermal laminate configuration
- Ceria Corrosion prevention treatment with sodium polyphosphate stabilized cerium oxide sol
- Chromium Corrosion prevention treatment with chromate
- A The strength was 6 N / 15 mm or more, and the peeled surface was between PSA / Al.
- the molding depth in which deep drawing molding is possible was evaluated with the following method.
- the exterior material 10 for lithium ion batteries was arrange
- the molding depth of the molding apparatus was set to 1.0 to 7.0 mm every 0.5 mm, and cold molding was performed in an environment of room temperature 23 ° C. and dew point temperature ⁇ 35 ° C.
- the punch mold has a rectangular cross section of 70 mm ⁇ 80 mm, has a punch radius (RP) of 1.00 mm on the bottom, and a punch corner radius (RCP) of 1.00 mm on the side. It was used.
- a die mold having a 1.00 mm diradius (RD) on the upper surface of the opening was used.
- C The difference is more than 1.25 compared to the case where there is no base material protective layer.
- Reference Example B1 In Reference Example B1, the following method was used. First, as the metal foil layer 14, a soft aluminum foil 8079 material (manufactured by Toyo Aluminum Co., Ltd.) having a thickness of 35 ⁇ m was prepared. Subsequently, sodium polyphosphate-stabilized cerium oxide sol (corrosion prevention treatment agent) was applied to both surfaces of the metal foil layer 14 by gravure coating using distilled water as a solvent and adjusting the solid content concentration to 10% by mass. At this time, phosphoric acid was 10 mass parts with respect to 100 mass parts of cerium oxide.
- sodium polyphosphate-stabilized cerium oxide sol corrosion prevention treatment agent
- a baking treatment is sequentially performed to form a corrosion prevention treatment layer 15a on one surface of the metal foil layer 14 and corrosion prevention on the other surface.
- a treatment layer 15b was formed.
- the baking conditions were a temperature of 150 ° C. and a processing time of 30 seconds.
- a polyurethane-based adhesive was applied as an adhesive layer 13 on the surface of the metal foil layer 14 opposite to the metal foil layer 14 of the corrosion prevention treatment layer 15a.
- the metal foil layer 14 and the corona-treated surface of the base material layer 11 were bonded via the adhesive layer 13 by a dry laminating method. Thereafter, the structure composed of the base material layer 11, the adhesive layer 13, the corrosion prevention treatment layer 15a, the metal foil layer 14, and the corrosion prevention treatment layer 15b is left in an atmosphere at a temperature of 60 ° C. for 6 days, thereby aging. Processed.
- a base material protective layer forming coating solution was prepared, applied to the surface of the base material layer 11 opposite to the adhesive layer 13, and dried to form a base material protective layer 12 having a thickness of 3 ⁇ m.
- the coating liquid for base-material protective layer formation was adjusted as follows. That is, a curing agent (tolylene diisocyanate adduct (TDI-A) as an aromatic isocyanate compound) was blended in a coating solution of a varnished resin (polyester polyol).
- a maleic anhydride-modified polypropylene (trade name: Admer, manufactured by Mitsui Chemicals) as a base material and a sealant layer 17 as a sealant adhesive layer 16 are used.
- Admer sold by Mitsui Chemicals
- a sealant layer 17 as a sealant adhesive layer 16
- polypropylene was coextruded and bonded (heat-pressed) at 180 ° C. (pattern 2).
- the thickness of the sealant adhesive layer 16 was 15 ⁇ m
- the thickness of the sealant layer 17 was 20 ⁇ m. And thereby, the exterior material 10 for lithium ion batteries was produced.
- a lithium ion battery exterior material 10 was produced in the same manner as in Reference Example B1, except that the base material protective layer composition and the configuration pattern shown in Tables 5 and 6 were adopted.
- the suffix “-A” in the curing agent type indicates an adduct, and the suffix “—N” indicates an isocyanurate.
- the procedure was changed as follows to prepare exterior materials. (Examples B32 to B34, B36 and B38) A filler was blended into the varnished resin.
- Examples B37 and B38 A polyurethane-based adhesive prepared by mixing polyisocyanate with acid-modified polyolefin dissolved in a mixed solvent of toluene and methylcyclohexane was applied to the surface of the corrosion prevention treatment layer 15b opposite to the metal foil layer. Next, by a dry laminating method, a polyolefin film having a thickness of 30 ⁇ m (a film obtained by corona-treating the surface of the non-stretched polypropylene film on the side of the sealant adhesive layer 16) and the metal foil layer 14 through the sealant adhesive layer 16. And were adhered.
- the structure composed of the base material layer 11, the adhesive layer 13, the corrosion prevention treatment layer 15a, the metal foil layer 14, the corrosion prevention treatment layer 15b, the sealant adhesion layer 16, and the sealant layer 17 is placed in an atmosphere having a temperature of 40 ° C. Aging treatment was carried out by leaving it for 6 days. Except this, a lithium ion battery exterior material 10 was produced in the same manner as in Example B1 (Pattern 1).
- A The strength was 6 N / 15 mm or more, and the peeled surface was between PSA / Al.
- the molding depth in which deep drawing molding is possible was evaluated with the following method.
- the exterior material 10 for lithium ion batteries was arrange
- the molding depth of the molding apparatus was set to 1.0 to 7.0 mm every 0.25 mm, and cold molding was performed in an environment of a room temperature of 23 ° C. and a dew point temperature of ⁇ 35 ° C.
- the punch mold has a rectangular cross section of 70 mm ⁇ 80 mm, has a punch radius (RP) of 1.00 mm on the bottom, and a punch corner radius (RCP) of 1.00 mm on the side. It was used.
- a die mold having a 1.00 mm diradius (RD) on the upper surface of the opening was used.
- C The difference is more than 1.25 compared to the case where there is no base material protective layer.
- the insulating property was evaluated when the base material and the base material protective layer were formed on one surface of the metal foil layer and the corrosion prevention treatment layer was exposed on the other surface.
- a dielectric strength / insulation resistance tester manufactured by KIKUSUI, “TOS9201” was used for the evaluation of insulation. The measurement was performed by fixing one electrode on the corrosion prevention treatment layer side, dropping water on the surface of the base material protective layer, bringing the other electrode into contact with the dropped region, and applying a voltage of 100V.
- S A resistance of 20000 M ⁇ or more was obtained.
- A A resistance of 10000 M ⁇ or more to less than 20000 M ⁇ was obtained.
- B A resistance of 2000 M ⁇ to 10000 M ⁇ was obtained.
- C A resistance of less than 2000 M ⁇ was obtained.
- the exterior materials of the reference examples or Examples B1 to B38 have deep drawability, delamination resistance, electrolytic solution resistance, and alcohol resistance, and are adhesive. It was confirmed that the tape had adhesion and insulating properties. Compared to Reference Examples B1 to B3, Comparative Example B1 having no base material protective layer was found to be inferior in electrolytic solution resistance, alcohol resistance, and insulation.
- Example B20 by using an isocyanate other than the alicyclic isocyanate as an adduct or buret of an aliphatic isocyanate, good electrolytic solution resistance and alcohol resistance can be obtained.
- the polyester resin or the acrylic resin has a hydroxyl value of 5 to 100 KOHmg / g, so that the base material protective layer has high base material adhesion.
- the base material protective layer thickness is 1 When the ratio of the thickness of the base material protective layer to the thickness of the base material layer was 35% or less, high delamination resistance could be obtained.
- SYMBOLS 1 Battery element, 2 ... Lead, 10 ... Exterior material (exterior material for electrical storage devices), 11 ... Base material layer, 12 ... Base material protective layer, 13 ... Adhesive layer, 14 ... Metal foil layer, 15a, 15b ... Corrosion Prevention treatment layer, 16 ... sealant adhesive layer, 17 ... sealant layer, 30 ... embossed type exterior material, 32 ... molding process area (concave part), 34 ... lid part, 40 ... secondary battery.
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Abstract
Description
図1は、本発明の蓄電デバイス用外装材の一実施形態を模式的に表す断面図である。図1に示すように、本実施形態の外装材(蓄電デバイス用外装材)10は、基材層11と、該基材層11の一方の面側に設けられた基材保護層12と、該基材層11の基材保護層12とは反対側に設けられた接着層13と、該接着層13の基材層11とは反対側に設けられた、両面に腐食防止処理層15a,15bを有する金属箔層14と、該金属箔層14の接着層13とは反対側に設けられたシーラント接着層16と、該シーラント接着層16の金属箔層14とは反対側に設けられたシーラント層17と、が積層された積層体である。ここで、腐食防止処理層15aは金属箔層14の接着層13側の面に、腐食防止処理層15bは金属箔層14のシーラント接着層16側の面に、それぞれ設けられている。外装材10は、基材保護層12が最外層、シーラント層17が最内層である。すなわち、外装材10は、基材保護層12を蓄電デバイスの外部側、シーラント層17を蓄電デバイスの内部側に向けて使用される。以下、各層について説明する。
基材層11は、蓄電デバイスを製造する際のシール工程における耐熱性を付与し、成型加工や流通の際に起こりうるピンホールの発生を抑制する役割を果たす。特に大型用途の蓄電デバイスの外装材の場合等は、耐擦傷性、耐薬品性、絶縁性等も付与できる。
基材保護層12は、基材層11の一方の面側に設けられる層であって、ポリエステル樹脂又はアクリル樹脂と、硬化剤とを用いて形成される層である。すなわち、基材保護層12は、ポリエステル樹脂又はアクリル樹脂と、硬化剤とを含む原料の硬化物である。
接着層13は、基材層11と金属箔層14とを接着する層である。接着層13は、基材層11と金属箔層14とを強固に接着するために必要な密着力を有すると共に、冷間成型する際において、基材層11によって金属箔層14が破断されることを抑制するための追随性(部材が変形・伸縮したとしても、剥離することなく部材上に接着層13を確実に形成するための性能)も有する。
黄色:イソインドリノン、イソインドリン、キノフタロン、アントラキノン(フラバトロン)、アゾメチン、キサンテン等。
橙色:ジケトピロロピロール、ペリレン、アントラキノン、ペリノン、キナクリドン等。
赤色:アントラキノン、キナクリドン、ジケトピロロピロール、ペリレン、インジゴイド等。
紫色:オキサジン(ジオキサジン)、キナクリドン、ペリレン、インジゴイド、アントラキノン、キサンテン、ベンツイミダゾロン、ビオランスロン等。
青色:フタロシアニン、アントラキノン、インジゴイド等。
緑色:フタロシアニン、ペリレン、アゾメチン等。
白色:亜鉛華、鉛白、リトポン、二酸化チタン、沈降性硫酸バリウム、バライト粉等。
赤色:鉛丹、酸化鉄赤等。
黄色:黄鉛、亜鉛黄(亜鉛黄1種、亜鉛黄2種)等。
青色:ウルトラマリン青、プロシア青(フェロシアン化鉄カリウム)等。
黒色:カーボンブラック等。
金属箔層14としては、アルミニウム及びステンレス鋼等の各種金属箔が挙げられ、防湿性及び延展性等の加工性、並びにコストの面から、金属箔層14はアルミニウム箔であることが好ましい。アルミニウム箔は一般の軟質アルミニウム箔であってもよいが、耐ピンホール性及び成形時の延展性に優れる点から、鉄を含むアルミニウム箔であることが好ましい。
腐食防止処理層15a,15bは、電解液、又は、電解液と水分の反応により発生するフッ酸による金属箔層14の腐食を抑制する役割を果たす。また、腐食防止処理層15aは、金属箔層14と接着層13との密着力を高める役割を果たす。また、腐食防止処理層15bは、金属箔層14とシーラント接着層16との密着力を高める役割を果たす。腐食防止処理層15a及び腐食防止処理層15bは、同一の構成の層であってもよく、異なる構成の層であってもよい。
シーラント接着層16は、腐食防止処理層15bが形成された金属箔層14とシーラント層17を接着する層である。外装材10は、シーラント接着層16を形成する接着成分によって、熱ラミネート構成とドライラミネート構成に大きく分けられる。
シーラント層17は、外装材10に対し、ヒートシールによる封止性を付与する層であり、蓄電デバイスの組み立て時に内側に配置されて熱融着される層である。シーラント層17としては、ポリオレフィン系樹脂、又はポリオレフィン系樹脂に無水マレイン酸等の酸をグラフト変性させた酸変性ポリオレフィン系樹脂からなる樹脂フィルムが挙げられる。中でも、水蒸気のバリア性を向上させ、ヒートシールによって過度に潰れることなく蓄電デバイスの形態を構成可能なポリオレフィン系樹脂が好ましく、ポリプロピレンが特に好ましい。
次に、外装材10の製造方法について説明する。なお、外装材10の製造方法は以下の方法に限定されない。
工程S11:金属箔層14の一方の面上に腐食防止処理層15aを形成し、金属箔層14の他方の面上に腐食防止処理層15bを形成する工程。
工程S12:腐食防止処理層15aの金属箔層14とは反対側の面と、基材層11とを、接着層13を介して貼り合わせる工程。
工程S13:基材層11の接着層13とは反対側の面に基材保護層12を形成する工程。
工程S14:腐食防止処理層15bの金属箔層14とは反対側の面上に、シーラント接着層16を介してシーラント層17を形成する工程。
工程S11では、金属箔層14の一方の面上に腐食防止処理層15aを形成し、金属箔層14の他方の面上に腐食防止処理層15bを形成する。腐食防止処理層15a及び15bは、それぞれ別々に形成されてもよく、両方が一度に形成されてもよい。具体的には、例えば、金属箔層14の両方の面に腐食防止処理剤(腐食防止処理層の母材)を塗布し、その後、乾燥、硬化、焼付けを順次行うことで、腐食防止処理層15a及び15bを一度に形成する。また、金属箔層14の一方の面に腐食防止処理剤を塗布し、乾燥、硬化、焼き付けを順次行って腐食防止処理層15aを形成した後、金属箔層14の他方の面に同様にして腐食防止処理層15bを形成してもよい。腐食防止処理層15a及び15bの形成順序は特に制限されない。また、腐食防止処理剤は、腐食防止処理層15aと腐食防止処理層15bとで異なるものを用いてもよく、同じのものを用いてもよい。上記腐食防止処理剤としては、例えば、塗布型クロメート処理用の腐食防止処理剤等を用いることができる。腐食防止処理剤の塗布方法は、特に限定されないが、例えば、グラビアコート法、グラビアリバースコート法、ロールコート法、リバースロールコート法、ダイコート法、バーコート法、キスコート法、コンマコート法、小径グラビアコート法等の方法を用いることができる。なお、金属箔層14として、未処理の金属箔層を用いてもよいし、ウェットタイプの脱脂処理又はドライタイプの脱脂処理により、脱脂処理を施した金属箔層を用いてもよい。
工程S12では、腐食防止処理層15aの金属箔層14とは反対側の面と、基材層11とが、接着層13を形成する接着剤を用いてドライラミネーション等の手法で貼り合わせられる。このとき、外装材10に意匠性を付与するために、接着剤に上記顔料を配合してもよい。工程S13では、接着性の促進のため、室温~100℃の範囲でエージング(養生)処理を行ってもよい。エージング時間は、例えば、1~10日である。
工程S13では、基材層11の接着層13とは反対側の面に基材保護層12を形成する。まず、基材保護層12を形成するための原料(ポリエステル樹脂又はアクリル樹脂)を溶剤に溶かしたもの(塗液)を準備する。これに、ポリイソシアネート及びその他の硬化剤を配合する。塗工安定性を付与するために、レベリング剤、消泡剤等の各種安定剤を配合してもよい。また、塗工後のブロッキングを防止するために、また、塗液の反応促進のために、各種触媒を配合してもよい。また、塗液のポットライフ制御のために、反応遅延剤(例えばアセチルアセトン)を配合してもよい。
工程S13後、基材保護層12、基材層11、接着層13、腐食防止処理層15a、金属箔層14及び腐食防止処理層15bがこの順に積層された積層体の腐食防止処理層15bの金属箔層14とは反対側の面上に、シーラント接着層16を介してシーラント層17が形成される。シーラント層17は、ドライラミネーション及びサンドイッチラミネーション等によって積層されてもよく、シーラント接着層16とともに共押出し法によって積層されてもよい。シーラント層17は、接着性向上の点から、例えばサンドイッチラミネーションによって積層される、又は、シーラント接着層16とともに共押出し法によって積層されることが好ましく、共押出し法によって積層されることがより好ましい。
次に、外装材10を容器として備える蓄電デバイスについて説明する。蓄電デバイスは、電極を含む電池要素1と、上記電極から延在するリード2と、電池要素1を収容する容器とを備え、上記容器は蓄電デバイス用外装材10から、シーラント層17が内側となるように形成される。上記容器は、2つの外装材をシーラント層17同士を対向させて重ね合わせ、重ねられた外装材10の周縁部を熱融着して得られてもよく、また、1つの外装材を折り返して重ね合わせ、同様に外装材10の周縁部を熱融着して得られてもよい。また、蓄電デバイスは、外装材20を容器として備えていてもよい。本実施形態の外装材は、様々な蓄電デバイスにおいて使用可能である。そのような蓄電デバイスとしては、例えば、リチウムイオン電池、ニッケル水素電池、及び鉛蓄電池等の二次電池、並びに電気二重層キャパシタ等の電気化学キャパシタが挙げられる。
次に、上述した外装材10を用いて蓄電デバイスを製造する方法について説明する。なお、ここでは、エンボスタイプ外装材30を用いて二次電池40を製造する場合を例に挙げて説明する。図2は上記エンボスタイプ外装材30を示す図である。図3の(a)~(d)は、外装材10を用いた片側成型加工電池の製造工程を示す斜視図である。二次電池40としては、エンボスタイプ外装材30のような外装材を2つ設け、このような外装材同士を、アライメントを調整しつつ、貼り合わせて製造される、両側成型加工電池であってもよい。また、エンボスタイプ外装材30は、外装材20を用いて形成されてもよい。
工程S21:外装材10、電極を含む電池要素1、並びに上記電極から延在するリード2を準備する工程。
工程S22:外装材10の片面に電池要素1を配置するための凹部32を形成する工程(図3(a)及び図3(b)参照)。
工程S23:エンボスタイプ外装材30の成型加工エリア(凹部32)に電池要素1を配置し、凹部32を蓋部34が覆うようにエンボスタイプ外装材30を折り返し重ねて、電池要素1から延在するリード2を挟持するようにエンボスタイプ外装材30の一辺を加圧熱融着する工程(図3(b)及び図3(c)参照)。
工程S24:リード2を挟持する辺以外の一辺を残し、他の辺を加圧熱融着し、その後、残った一辺から電解液を注入し、真空状態で残った一辺を加圧熱融着する工程(図3(c)参照)。
工程S25:電流値や電圧値、環境温度などを所定の条件にして充放電を行い、化学変化を起こさせる(化成)工程。
工程S26:リード2を挟持する辺以外の加圧熱融着辺端部をカットし、成型加工エリア(凹部32)側に折り曲げる工程(図3(d)参照)。
工程S21では、外装材10、電極を含む電池要素1、並びに上記電極から延在するリード2を準備する。外装材10は、上述した実施形態に基づき準備する。電池要素1及びリード2としては特に制限はなく、公知の電池要素1及びリード2を用いることができる。
工程S22では、外装材10のシーラント層17側に電池要素1を配置するための凹部32が形成される。凹部32の平面形状は、電池要素1の形状に合致する形状、例えば平面視矩形状とされる。凹部32は、例えば矩形状の圧力面を有する押圧部材を、外装材10の一部に対してその厚み方向に押圧することで形成される。また、押圧する位置、すなわち凹部32は、長方形に切り出した外装材10の中央より、外装材10の長手方向の一方の端部に偏った位置に形成する。これにより、成型加工後に凹部32を形成していないもう片方の端部側を折り返し、蓋(蓋部34)とすることができる。
工程S23では、エンボスタイプ外装材30の成型加工エリア(凹部32)内に、正極、セパレータ及び負極等から構成される電池要素1が配置され。また、電池要素1から延在し、正極と負極にそれぞれ接合されたリード2が成型加工エリア(凹部32)から外に引き出される。その後、エンボスタイプ外装材30は、長手方向の略中央で折り返され、シーラント層17同士が内側となるように重ねられ、エンボスタイプ外装材30のリード2を挟持する一辺が加圧熱融着される。加圧熱融着は、温度、圧力及び時間の3条件で制御され、適宜設定される。加圧熱融着の温度は、シーラント層17を融解する温度以上であることが好ましい。
工程S24では、リード2を挟持する辺以外の一辺を残し、他の辺の加圧熱融着が行われる。その後、残った一辺から電解液を注入し、残った一辺が真空状態で加圧熱融着される。加圧熱融着の条件は工程S23と同様である。
工程S25では、工程S23までに得られた二次電池40に対して充放電を行い、化学変化を起こさせる(化成:40℃環境にて3日間)。そして、化成によって発生したガスの除去や電解液の補充のため、二次電池40を一度開封し、その後最終シールを行う。なお、この工程S25は省略することができる。
リード2を挟持する辺以外の周縁加圧熱融着辺端部がカットされ、端部からははみだしたシーラント層17が除去される。その後、周縁加圧熱融着部を成型加工エリア32側に折り返し、折り返し部42を形成することで、二次電池40が得られる。
実施例A1では、以下の手法により、リチウムイオン電池用外装材10を作製した。始めに、金属箔層14として、厚さ35μmの軟質アルミニウム箔8079材(東洋アルミニウム株式会社製)を準備した。次いで、金属箔層14の両面に、グラビアコートにより、溶媒として蒸留水を使用し、かつ固形分濃度10質量%に調整したポリリン酸ナトリウム安定化酸化セリウムゾル(腐食防止処理剤)を塗布した。このとき、酸化セリウム100質量部に対して、リン酸は10質量部とした。
表1、表2に示す基材保護層組成及び構成パターンを採用したこと以外は、実施例A1と同様にしてリチウムイオン電池用外装材10を作製した。表1、表2中、硬化剤タイプにおける末尾「-A」はアダクト体であることを示し、末尾「-N」はイソシアヌレート体であることを示す。なお、一部の実施例については、以下のとおり手順を変更して外装材を作製した。
(実施例A12~A14,A16及びA18)
ワニス化された樹脂に対して、フィラーを配合した。
・「シリカ」:7.8質量%、平均粒径2.7μm
・「ウレタン」:7.0質量%、平均粒径3μm
・「アクリル」:7.0質量%、平均粒径6μm
(実施例A15~A18)
ポリリン酸ナトリウム安定化酸化セリウムゾルを用いて腐食防止処理層15a及び15bを形成する代わりに、金属箔層14の両面にフェノール樹脂、フッ化クロム化合物、及びリン酸からなる処理液を塗布して被膜を形成し、焼付けすることによりクロメート処理を行って腐食防止処理層15a及び15bを形成した。このこと以外は実施例A1と同様にして、リチウムイオン電池用外装材10を作製した。
(実施例A17及びA18)
腐食防止処理層15bの金属箔層14とは反対側の面に、トルエン及びメチルシクロヘキサンの混合溶媒に溶解させた酸変性ポリオレフィンにポリイソシアネートを配合したポリウレタン系接着剤を塗布した。次いで、ドライラミネート法により、シーラント接着層16を介して、シーラント層17となる厚さ30μmのポリオレフィンフィルム(無延伸ポリプロピレンフィルムのシーラント接着層16側の面をコロナ処理したフィルム)と金属箔層14とを接着させた。その後、基材層11、接着層13、腐食防止処理層15a、金属箔層14、腐食防止処理層15b、シーラント接着層16、及びシーラント層17からなる構造体を、温度が40℃の雰囲気中で6日間放置することで、エージング処理した。このこと以外は、実施例A1と同様にして、リチウムイオン電池用外装材10を作製した(パターン1)。
HDI:ヘキサメチレンジイソシアネート
TDI:トリレンジイソシアネート
IPDI:イソホロンジイソシアネート
パターン1:ドライラミネート構成
パターン2:熱ラミネート構成
セリア:ポリリン酸ナトリウム安定化酸化セリウムゾルを用いた腐食防止処理
クロム:クロメートによる腐食防止処理
基材保護層が上面になるように、外装材をアクリル板で固定した。基材保護層側に長さ100mm、幅15mmのPSA(pressure sensitive adhesive)テープと、長さ100mm、幅25mmの剥離試験用の支持アルミニウム箔とを、加重1kgのローラーで固定した。これを室温で12時間静置した後、外装材とPSAテープとのラミネート強度(180度剥離、剥離速度は50mm/分)を測定し、どの界面で剥離したかについても確認した。結果を表3、表4に示す。
A:強度が6N/15mm以上、かつ、剥離面がPSA/Al間であった。
B:強度が6N/15mm以上、かつ、剥離面がPSA/Al以外の面であった。
C:強度が6N/15mm未満であった。
各例で得られた外装材の被覆層に、電解液(エチレンカーボネート/ジメチルカーボネート/ジエチルカーボネート=1:1:1wt%、LiPF6、1M)を滴下し、規定時間経過後にイソプロピルアルコールで拭き取った。その後、滴下箇所の外観を以下の基準に従って評価した。結果を表3、表4に示す。
A:15分経過後に電解液を滴下した箇所が認識できなかった。
B:10分経過後に電解液を滴下した箇所が認識できなかったが、15分経過後には輪郭が発生した。
C:5分経過後に電解液を滴下した箇所が認識できなかったが、10分経過後には輪郭が発生した。
各例で得られた外装材の被覆層に、エタノールを染み込ませた1cm四方のコットンを当て、その上から500gの加重をかけ一定速度でラビングした(アルコールラビング法)。そして、規定回数ラビングを繰り返した後、塗膜に剥がれがないかを以下の基準に従って評価した。結果を表3、表4に示す。
A:20回以上繰り返しても剥がれが発生しなかった。
B:15回繰り返し後には剥がれが発生しなかったが、20回繰り返し後には剥がれが発生した。
C:10回繰り返し後には剥がれが発生しなかったが、15回繰り返し後には剥がれが発生した。
各例で得られた外装材について、基材層11と基材保護層12との間の密着性を以下の方法で評価した。試験面にカッターナイフを用いて、素地に達する切り傷の間隔が1mmになるように11本の切り傷をつけ100個の碁盤目を作る。碁盤目部分にセロハンテープを強く圧着させ、テープの端を90°の角度で一気に引き剥がし、100個の碁盤目から目視にて塗膜が剥離していない個数をカウントして評価した。結果を表3、表4に示す。
A:100個OK
B:90~80個OK
C:80個未満OK
各例で得られた外装材について、深絞り成型が可能な成型深度を以下の方法で評価した。まず、リチウムイオン電池用外装材10を、シーラント層17が上方を向くように成型装置内に配置した。成型装置の成型深さを0.5mmごとに1.0~7.0mmに設定し、室温23℃、露点温度-35℃の環境下で冷間成型した。なお、パンチ金型には、70mm×80mmの長方形の横断面を有し、底面に1.00mmのパンチラジアス(RP)を有し、側面に1.00mmのパンチコーナーラジアス(RCP)を有するものを使用した。また、ダイ金型には、開口部上面に1.00mmのダイラジアス(RD)を有するものを使用した。冷間成型を行った部分の破断及びピンホールの有無を、外装材にライトを照射しながら目視にて確認し、破断及びピンホールのいずれも生じることなく深絞り成型できた成型深度の最大値を求めた。また、成型深度について以下の基準に従って評価した。結果を表3、表4に示す。
A:基材保護層がない場合(比較例A1)と比較して、差が0.75mm以下。
B:基材保護層がない場合と比較して、差が0.75mm超1.25mm以下。
C:基材保護層がない場合と比較して、差が1.25超。
・脂環式イソシアネート以外のイソシアネートの重量[a]と脂環式イソシアネートの重量[b]との比([a]/[b])が99/1~80/20であると、PSA密着性、耐電解液性、耐アルコール性に優れる。
・成型性向上のためには、ポリエステルポリオールの水酸基のモル数[A]に対する硬化剤の反応性基のモル数[B]の比([B]/[A])が80未満であることが好ましい(実施例A2と実施例A6との比較)。
・フィラーを配合すると、成型性が向上する傾向にある(実施例A2と実施例A12~A14との比較)。
参考例B1では、以下の手法に作製した。始めに、金属箔層14として、厚さ35μmの軟質アルミニウム箔8079材(東洋アルミニウム株式会社製)を準備した。次いで、金属箔層14の両面に、グラビアコートにより、溶媒として蒸留水を使用し、かつ固形分濃度10質量%に調整したポリリン酸ナトリウム安定化酸化セリウムゾル(腐食防止処理剤)を塗布した。このとき、酸化セリウム100質量部に対して、リン酸は10質量部とした。
表5、表6に示す基材保護層組成及び構成パターンを採用したこと以外は、参考例B1と同様にしてリチウムイオン電池用外装材10を作製した。表5及び表6中、硬化剤タイプにおける末尾「-A」はアダクト体であることを示し、末尾「-N」はイソシアヌレート体であることを示す。なお、一部の実施例については、以下のとおり手順を変更して外装材を作製した。
(実施例B32~B34,B36及びB38)
ワニス化された樹脂に対して、フィラーを配合した。
・「シリカ」:7.8質量%、平均粒径2.7μm
・「ウレタン」:7.0質量%、平均粒径 3μm
・「アクリル」:7.0質量%、平均粒径 6μm
(実施例B35~B38)
ポリリン酸ナトリウム安定化酸化セリウムゾルを用いて腐食防止処理層15a及び15bを形成する代わりに、金属箔層14の両面にフェノール樹脂、フッ化クロム化合物、及びリン酸からなる処理液を塗布して被膜を形成し、焼付けすることによりクロメート処理を行って腐食防止処理層15a及び15bを形成した。このこと以外は参考例B1と同様にして、リチウムイオン電池用外装材10を作製した。
(実施例B37及びB38)
腐食防止処理層15bの金属箔層14とは反対側の面に、トルエン及びメチルシクロヘキサンの混合溶媒に溶解させた酸変性ポリオレフィンにポリイソシアネートを配合したポリウレタン系接着剤を塗布した。次いで、ドライラミネート法により、シーラント接着層16を介して、シーラント層17となる厚さ30μmのポリオレフィンフィルム(無延伸ポリプロピレンフィルムのシーラント接着層16側の面をコロナ処理したフィルム)と金属箔層14とを接着させた。その後、基材層11、接着層13、腐食防止処理層15a、金属箔層14、腐食防止処理層15b、シーラント接着層16、及びシーラント層17からなる構造体を、温度が40℃の雰囲気中で6日間放置することで、エージング処理した。このこと以外は、実施例B1と同様にして、リチウムイオン電池用外装材10を作製した(パターン1)。
HDI―A:ヘキサメチレンジイソシアネートのアダクト体
TDI―A:トリレンジイソシアネートのアダクト体
IPDI―N:イソホロンジイソシアネートのヌレート体
パターン1:ドライラミネート構成
パターン2:熱ラミネート構成
セリア:ポリリン酸ナトリウム安定化酸化セリウムゾルを用いた腐食防止処理
クロム:クロメートによる腐食防止処理
基材保護層が上面になるように、外装材をアクリル板で固定した。基材保護層側に長さ100mm、幅15mmのPSA(pressure sensitive adhesive)テープと、長さ100mm、幅25mmの剥離試験用の支持アルミニウム箔とを、加重2kgのローラーで固定した。これを室温で12時間静置した後、外装材とPSAテープとのラミネート強度(180度剥離、剥離速度は50mm/分)を測定し、どの界面で剥離したかについても確認した。結果を表7、表8に示す。
A:強度が6N/15mm以上、かつ、剥離面がPSA/Al間であった。
B:強度が6N/15mm以上、かつ、剥離面がPSA/Al以外の面であった。
C:強度が6N/15mm未満であった。
各例で得られた外装材の被覆層に、電解液(エチレンカーボネート/ジメチルカーボネート/ジエチルカーボネート=1:1:1wt%、LiPF6、1M)を滴下し、規定時間経過後にイソプロピルアルコールで拭き取った。その後、滴下箇所の外観を以下の基準に従って評価した。結果を表1に示す。
S:20分経過後に電解液を滴下した箇所が認識できなかった。
A:15分経過後に電解液を滴下した箇所が認識できなかった。
B:10分経過後に電解液を滴下した箇所が認識できなかったが、15分経過後には輪郭が発生した。
C:5分経過後に電解液を滴下した箇所が認識できなかったが、10分経過後には輪郭が発生した。
各例で得られた外装材の被覆層に、エタノールを染み込ませた1cm四方のコットンを当て、その上から500gの加重をかけ一定速度でラビングした(アルコールラビング法)。そして、規定回数ラビングを繰り返した後、塗膜に剥がれがないかを以下の基準に従って評価した。結果を表1に示す。
A:20回以上繰り返しても剥がれが発生しなかった。
B:15回繰り返し後には剥がれが発生しなかったが、20回繰り返し後には剥がれが発生した。
C:10回繰り返し後には剥がれが発生しなかったが、15回繰り返し後には剥がれが発生した。
各例で得られた外装材について、基材層11と基材保護層12との間の密着性を以下の方法で評価した。試験面にカッターナイフを用いて、素地に達する切り傷の間隔が1mmになるように11本の切り傷をつけ100個の碁盤目を作る。碁盤目部分にセロハンテープを強く圧着させ、テープの端を90°の角度で一気に引き剥がし、100個の碁盤目から目視にて塗膜が剥離していない個数をカウントして評価した。結果を表1に示す。
A:100個OK
B:90~80個OK
C:80個未満OK
各例で得られた外装材について、深絞り成型が可能な成型深度を以下の方法で評価した。まず、リチウムイオン電池用外装材10を、シーラント層17が上方を向くように成型装置内に配置した。成型装置の成型深さを0.25mmごとに1.0~7.0mmに設定し、室温23℃、露点温度-35℃の環境下で冷間成型した。なお、パンチ金型には、70mm×80mmの長方形の横断面を有し、底面に1.00mmのパンチラジアス(RP)を有し、側面に1.00mmのパンチコーナーラジアス(RCP)を有するものを使用した。また、ダイ金型には、開口部上面に1.00mmのダイラジアス(RD)を有するものを使用した。冷間成型を行った部分の破断及びピンホールの有無を、外装材にライトを照射しながら目視にて確認し、破断及びピンホールのいずれも生じることなく深絞り成型できた成型深度の最大値を求めた。また、成型深度について以下の基準に従って評価した。結果を表1に示す。
A:基材保護層がない場合(比較例B1)と比較して、差が0.75mm以下。
B:基材保護層がない場合と比較して、差が0.75mm超1.25mm以下。
C:基材保護層がない場合と比較して、差が1.25超。
各例で得られた外装材について、成型装置の成型深さを3.5mmで固定したこと以外は、成型深度の評価と同様にして冷間成型した。このような冷間成型体を各例について10サンプル準備し高温水環境(50℃温水)に一週間放置した。そして、各環境毎に、基材層11及び金属箔層間においてデラミネーションが発生したサンプル数をカウントし、以下の基準に従って評価した。結果を表1に示す。
A:0サンプル。
B:1~3サンプル。
C:4~10サンプル。
金属箔層の一方の面に基材及び基材保護層が形成され、他方の面に腐食防止処理層が露出している段階で、絶縁性の評価を行った。絶縁性の評価には耐電圧・絶縁抵抗試験器(KIKUSUI製、「TOS9201」)を用いた。測定は、腐食防止処理層側に一方の電極を固定し、基材保護層表面に水を滴下し、滴下した領域に他方の電極を接触させて、100Vの電圧を印加して行った。
S:20000MΩ以上の抵抗を得た。
A:10000MΩ以上~20000MΩ未満の抵抗を得た。
B:2000MΩ以上~10000MΩ未満の抵抗を得た。
C:2000MΩ未満の抵抗を得た。
各実験例で使用したポリオールにトルエンを加え、マグネチックスターラーで一定時間攪拌し、ポリオールの溶解性を以下の基準に従って評価した。
A:1分後にポリオールが溶解した。
B:1分後に未溶解のポリオールが残るものの、5分後にはポリオールが溶解した。
C:5分を越えても未溶解のポリオールが残った。
なお、上記評価においては、いずれもB以上を合格基準とする。
Claims (12)
- 少なくとも基材保護層、基材層、接着層、金属箔層、シーラント接着層、及びシーラント層がこの順で積層された構造を備え、
前記基材保護層は、ポリエステル樹脂又はアクリル樹脂と、硬化剤とを含む原料の硬化物であり、
前記ポリエステル樹脂又は前記アクリル樹脂は、前記硬化剤と反応する反応性基を末端もしくは側鎖、又はその両方に有し、
前記硬化剤は、脂環式イソシアネート以外のイソシアネートと、脂環式イソシアネートとを含み、
前記脂環式イソシアネート以外のイソシアネートの重量[a]と脂環式イソシアネートの重量[b]との比([a]/[b])が99/1~80/20である、蓄電デバイス用外装材。 - 前記ポリエステル樹脂又は前記アクリル樹脂の反応性基のモル数[A]に対する前記硬化剤の反応性基のモル数[B]の比([B]/[A])が5~60である、請求項1記載の蓄電デバイス用外装材。
- 前記ポリエステル樹脂又は前記アクリル樹脂の反応性基のモル数[A]に対する前記硬化剤の反応性基のモル数[B]の比([B]/[A])が5~20である、請求項2記載の蓄電デバイス用外装材。
- 最外部分に水が付着した状態で、前記基材保護層と金属箔層との間に100Vの定電圧を3分間印加したとき、その電気抵抗が2000MΩ以上となる、請求項1~3のいずれか一項記載の蓄電デバイス用外装材。
- 前記ポリエステル樹脂又は前記アクリル樹脂の反応性基がいずれも水酸基であり、
前記ポリエステル樹脂又は前記アクリル樹脂の水酸基価が5~70KOHmg/gである、請求項1~4のいずれか一項記載の蓄電デバイス用外装材。 - 前記脂環式イソシアネート以外のイソシアネートが、脂肪族イソシアネートのアダクト体又はビューレット体である、請求項1~5のいずれか一項記載の蓄電デバイス用外装材。
- 前記ポリエステル樹脂又は前記アクリル樹脂の数平均分子量が2000~30000である、請求項1~6のいずれか一項記載の蓄電デバイス用外装材。
- 前記基材保護層のガラス転移温度(Tg)が60~140℃である、請求項1~7のいずれか一項記載の蓄電デバイス用外装材。
- 前記基材保護層がさらにフィラーを含む、請求項1~8のいずれか一項記載の蓄電デバイス用外装材。
- 前記基材保護層の厚さが1~5μmであり、前記基材層の厚さに対する前記基材保護層の厚さの割合が35%以下である、請求項1~9のいずれか一項記載の蓄電デバイス用外装材。
- 金属箔層の一方の面に、接着層を介して基材層を貼り合わせる工程、
前記基材層の前記接着層とは反対側の面に基材保護層を形成する工程、及び
前記金属箔層の前記接着層とは反対側の面に、シーラント接着層を介してシーラント層を形成する工程、を備え、
前記基材保護層は、ポリエステル樹脂又はアクリル樹脂と、硬化剤とを含む原料の硬化物であり、
前記ポリエステル樹脂又はアクリル樹脂は、前記硬化剤と反応する反応性基を末端もしくは側鎖、又はその両方に有し、
前記硬化剤は、脂環式イソシアネート以外のイソシアネートと、脂環式イソシアネートとを含み、
前記脂環式イソシアネート以外のイソシアネートの重量[a]と脂環式イソシアネートの重量[b]との比([a]/[b])が99/1~80/20である、
蓄電デバイス用外装材の製造方法。 - 基材層の一方の面に基材保護層を形成する工程、
前記基材層の基材保護層とは反対側の面に、接着層を介して金属箔層の一方の面を貼り合わせる工程、及び
前記金属箔層の前記接着層とは反対側の面に、シーラント接着層を介してシーラント層を形成する工程、を備え、
前記基材保護層は、ポリエステル樹脂又はアクリル樹脂と、硬化剤とを含む原料の硬化物であり、
前記ポリエステル樹脂又はアクリル樹脂は、前記硬化剤と反応する反応性基を末端もしくは側鎖、又はその両方に有し、
前記硬化剤は、脂環式イソシアネート以外のイソシアネートと、脂環式イソシアネートとを含み、
前記脂環式イソシアネート以外のイソシアネートの重量[a]と脂環式イソシアネートの重量[b]との比([a]/[b])が99/1~80/20である、
蓄電デバイス用外装材の製造方法。
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