WO2018097329A1 - Matériau d'encapsulation pour batteries, son procédé de production, et batterie - Google Patents

Matériau d'encapsulation pour batteries, son procédé de production, et batterie Download PDF

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Publication number
WO2018097329A1
WO2018097329A1 PCT/JP2017/042691 JP2017042691W WO2018097329A1 WO 2018097329 A1 WO2018097329 A1 WO 2018097329A1 JP 2017042691 W JP2017042691 W JP 2017042691W WO 2018097329 A1 WO2018097329 A1 WO 2018097329A1
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WIPO (PCT)
Prior art keywords
layer
packaging material
adhesive layer
battery packaging
adhesive
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PCT/JP2017/042691
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English (en)
Japanese (ja)
Inventor
かおる 津森
山下　力也
山下　孝典
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大日本印刷株式会社
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Application filed by 大日本印刷株式会社 filed Critical 大日本印刷株式会社
Priority to CN201780014270.XA priority Critical patent/CN108701780B/zh
Priority to JP2018553026A priority patent/JP6958567B2/ja
Publication of WO2018097329A1 publication Critical patent/WO2018097329A1/fr

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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
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • 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
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/34—Layered products comprising a layer of synthetic resin comprising polyamides
    • 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
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/36—Layered products comprising a layer of synthetic resin comprising polyesters
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/78—Cases; Housings; Encapsulations; Mountings
    • 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
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/105—Pouches or flexible bags
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to a packaging material for a battery, a manufacturing method thereof, and a battery.
  • a polyamide film may be used as a base material.
  • a polyamide film is used as the base material, if the electrolytic solution adheres to the surface of the battery packaging material containing the battery element in the battery manufacturing process, the outer surface is eroded and whitened, resulting in a defective product.
  • a polyester film may be used as a base material.
  • the polyester film has a problem that it is hard and inferior in moldability as compared with the polyamide film.
  • a battery packaging material that uses a laminate of a polyester film and a polyamide film as a base material and has improved chemical moldability and electrolyte solution resistance (see Patent Document 1). ).
  • battery packaging materials are required to further improve moldability.
  • the polyester film and the polyamide film It is considered necessary to ensure sufficient adhesion and adhesion between the base material and the barrier layer, and to relieve stress applied during molding and to prevent the barrier layer from breaking during molding.
  • the main object of the present invention is to provide a technique for improving the moldability of a battery packaging material in which the base material layer has at least a polyester film layer and a polyamide film layer.
  • the present inventors have provided a battery packaging material using a laminate of a polyester film and a polyamide film as a base material, an adhesive layer between the base material layer and the barrier layer, and the polyester film and the polyamide.
  • a battery packaging material with significantly superior moldability compared to conventional battery packaging materials can be provided.
  • the present invention provides a battery packaging material composed of a laminate including at least a base material layer, an adhesive layer, a barrier layer, and a heat-fusible resin layer in this order.
  • the base material layer is a polyester film layer.
  • a first adhesive layer between the first adhesive layer and the polyamide film layer, and each of the adhesive layer and the first adhesive layer has a hardness measured by a nanoindentation method of 50 MPa or less. It was found that the moldability was excellent despite having the layer.
  • the present invention has been completed by further studies based on these findings.
  • Item 1 It is composed of a laminate comprising at least a base material layer, an adhesive layer, a barrier layer, and a heat-fusible resin layer in this order, In the base material layer, a first adhesive layer is provided between the polyester film layer and the polyamide film layer, Each of the adhesive layer and the first adhesive layer is a battery packaging material having a hardness measured by a nanoindentation method of 50 MPa or less.
  • Item 2. Item 2. The battery packaging material according to Item 1, wherein the ratio of the thickness of the polyester film layer to the thickness of the polyamide film layer is in the range of 1: 1 to 1: 5.
  • Item 4. Item 4. The battery packaging material according to any one of Items 1 to 3, wherein the thickness of the first adhesive layer is 3 ⁇ m or less.
  • the adhesive layer is formed of a polyurethane adhesive, a polyacrylic adhesive, a modified polypropylene adhesive, an adhesive containing a silane coupling agent, or an adhesive containing a titanate coupling agent. 5.
  • the first adhesive layer is formed of a resin composition containing a modified thermoplastic resin graft-modified with an unsaturated carboxylic acid or an unsaturated carboxylic acid derivative component. Battery packaging material.
  • Item 7. The battery packaging material according to any one of Items 1 to 6, wherein an acid-resistant film is provided on at least the surface of the barrier layer on the heat-fusible resin layer side.
  • Item 8. Item 8. The battery packaging material according to Item 7, wherein the acid-resistant film contains at least one element selected from the group consisting of phosphorus, chromium, and cerium.
  • Item 9. Item 8. The battery packaging material according to Item 7, wherein the acid-resistant film contains at least one selected from the group consisting of phosphates, chromates, fluorides, and triazine thiol compounds.
  • Item 10. Item 8. The battery packaging material according to Item 7, wherein the acid-resistant film contains a cerium compound.
  • Item 11. Item 8.
  • Item 12 A battery, wherein a battery element comprising at least a positive electrode, a negative electrode, and an electrolyte is housed in a package formed of the battery packaging material according to any one of Items 1 to 11.
  • a method for producing a battery packaging material comprising a step of obtaining a laminate by laminating at least a base material layer, an adhesive layer, a barrier layer, and a heat-fusible resin layer in this order,
  • the base material layer includes a first adhesive layer between the polyester film layer and the polyamide film layer,
  • the method for producing a battery packaging material wherein the adhesive layer and the first adhesive layer each have a hardness measured by a nanoindentation method of 50 MPa or less.
  • the present invention is composed of a laminate including at least a base material layer, an adhesive layer, a barrier layer, and a heat-fusible resin layer in this order.
  • a polyester film layer and a polyamide film layer In the base material layer, a polyester film layer and a polyamide film layer
  • the first adhesive layer is provided between the first adhesive layer and the adhesive layer and the first adhesive layer each having a hardness measured by the nanoindentation method of 50 MPa or less.
  • Packaging materials can be provided.
  • the battery packaging material of the present invention is composed of a laminate including at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order.
  • the polyester film layer and A first adhesive layer is provided between the polyamide film layer, and each of the adhesive layer and the first adhesive layer has a hardness measured by a nanoindentation method of 50 MPa or less.
  • the numerical range indicated by “to” means “above” or “below”.
  • the notation of 2 to 15 mm means 2 mm or more and 15 mm or less.
  • the battery packaging material 10 of the present invention comprises a base material layer 1, an adhesive layer 2, a barrier layer 3, and a heat-fusible resin layer 4 in this order. It is comprised from the laminated body provided.
  • the base material layer 1 is the outermost layer side
  • the heat-fusible resin layer 4 is the innermost layer. That is, when the battery is assembled, the battery element is sealed by heat-sealing the heat-fusible resin layers 4 positioned at the periphery of the battery element to seal the battery element.
  • the base material layer 1 includes a first adhesive layer 13 between the polyester film layer 11 and the polyamide film layer 12. From the viewpoint of increasing the electrolytic solution resistance on the outer surface of the battery packaging material, the polyamide film layer 12, the first adhesive layer 13, and the polyester film layer 11 are laminated in this order from the barrier layer 3 side.
  • the battery packaging material of the present invention is provided with a second adhesive layer between the barrier layer 3 and the heat-fusible resin layer 4 for the purpose of enhancing the adhesion between them. 5 may be provided.
  • the surface coating layer 6 etc. may be provided in the outer side (opposite side to the heat-fusible resin layer 4) of the base material layer 1 as needed.
  • the thickness of the laminate constituting the battery packaging material of the present invention is not particularly limited, but is preferably about 160 ⁇ m or less from the viewpoint of exhibiting high insulation while reducing the thickness of the laminate as much as possible. More preferred is about 35 to 155 ⁇ m, still more preferred is about 45 to 120 ⁇ m. Even when the thickness of the laminate constituting the battery packaging material of the present invention is as thin as 160 ⁇ m or less, for example, the present invention can exhibit excellent insulation. For this reason, the packaging material for batteries of this invention can contribute to the improvement of the energy density of a battery.
  • the base material layer 1 is a layer located on the outermost layer side.
  • a first adhesive layer 13 is provided between the polyester film layer 11 and the polyamide film layer 12. That is, the base material layer 1 has at least the polyester film layer 11, the first adhesive layer 13, and the polyamide film layer 12 in this order.
  • polyester constituting the polyester film layer 11 include copolymerized polyesters mainly composed of polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, polyethylene isophthalate, and ethylene terephthalate. And a copolyester mainly composed of butylene terephthalate as a repeating unit.
  • the copolymer polyester mainly composed of ethylene terephthalate is a copolymer polyester that polymerizes with ethylene isophthalate mainly composed of ethylene terephthalate (hereinafter, polyethylene (terephthalate / isophthalate)).
  • polyethylene terephthalate / isophthalate
  • polyethylene terephthalate / adipate
  • polyethylene terephthalate / sodium sulfoisophthalate
  • polyethylene terephthalate / sodium isophthalate
  • polyethylene terephthalate / phenyl-dicarboxylate
  • polyethylene terephthalate / decanedicarboxylate
  • polyester mainly composed of butylene terephthalate as a repeating unit
  • a copolymer polyester that polymerizes with butylene isophthalate having butylene terephthalate as a repeating unit hereinafter referred to as polybutylene (terephthalate / isophthalate).
  • polybutylene (terephthalate / adipate) polybutylene (terephthalate / sebacate), polybutylene (terephthalate / decanedicarboxylate), polybutylene naphthalate and the like.
  • These polyesters may be used individually by 1 type, and may be used in combination of 2 or more type.
  • Polyester has the advantage of being excellent in electrolytic solution resistance and less likely to cause whitening due to the adhesion of the electrolytic solution, and is suitably used as a material for forming the base material layer 1.
  • the polyester film layer 11 is preferably composed of a biaxially stretched polyester film, particularly a biaxially stretched polyethylene terephthalate film.
  • the thickness of the polyester film layer 11 is not particularly limited, but is preferably about 20 ⁇ m or less, more preferably about 1 to 15 ⁇ m, more preferably from the viewpoint of exhibiting excellent moldability while reducing the thickness of the battery packaging material. Is about 3 to 12 ⁇ m.
  • polyamide constituting the polyamide film layer 12 include aliphatic systems such as nylon 6, nylon 66, nylon 610, nylon 12, nylon 46, and a copolymer of nylon 6 and nylon 66.
  • Polyamides containing aromatics such as acid copolymerized polyamides and polyamides MXD6 (polymetaxylylene adipamide); Alicyclic polyamides such as polyaminomethylcyclohexyl adipamide (PACM6); and lactam components and 4,4′-diphenylmethane -Diisocyanate, etc.
  • Polyamides obtained by copolymerizing the isocyanate component, copolymerized polyamide and polyester and polyalkylene ether glycol with a polyester amide copolymer is a copolymer of or polyetheresteramide copolymers; copolymers thereof, and the like.
  • polyamides may be used individually by 1 type, and may be used in combination of 2 or more type.
  • the stretched polyamide film is excellent in stretchability, can prevent whitening due to resin cracking of the base material layer 1 during molding, and is suitably used as a material for forming the base material layer 1.
  • the polyamide film layer 12 is preferably composed of a biaxially stretched polyamide film, particularly a biaxially stretched nylon film.
  • the thickness of the polyamide film layer 12 is not particularly limited, but is preferably 30 ⁇ m or less, more preferably about 1 to 25 ⁇ m, more preferably from the viewpoint of achieving excellent moldability while reducing the thickness of the battery packaging material.
  • An example is about 10 to 25 ⁇ m.
  • the ratio of the thickness of the polyester film layer 11 to the thickness of the polyamide film layer 12 (the thickness of the polyester film layer 11: the thickness of the polyamide film layer 12) in the base material layer 1 is 1 It is preferably in the range of about 1: 1 to 1: 5, and more preferably in the range of about 1: 1.2 to 1: 4.
  • the base material layer 1 as a lamination order of the polyester film layer 11 and the polyamide film layer 12, from the viewpoint of improving the electrolytic solution resistance of the battery packaging material, the polyamide film layer 12, The first adhesive layer 13 and the polyester film layer 11 are laminated in this order.
  • the hardness measured by the nanoindentation method of the first adhesive layer 13 is 50 MPa or less.
  • the first adhesive layer 13 has a hardness of 50 MPa or less, and an adhesive layer 2 described later positioned between the base material layer 1 and the barrier layer 3.
  • the hardness measured by the nanoindentation method is 50 MPa or less, excellent moldability can be exhibited.
  • this mechanism for example, it can be considered as follows. That is, since the hardness of these adhesive layers is designed to be smaller than that of a normal adhesive, the base layer 1 at the time of molding is formed even though the base layer 1 has the polyester film layer 11. It is effective that the adhesive layer 2 and the first adhesive layer 13 appropriately suppress the deformation of the barrier layer 3 due to the deformation, and as a result, cracks and pinholes are effectively generated in the barrier layer 3. It is thought to be suppressed.
  • the hardness of the first adhesive layer 13 is preferably about 10 to 50 MPa, more preferably about 15 to 40 MPa.
  • the hardness measured by the nanoindentation method of the adhesive layer 2 and the first adhesive layer 13 is a value measured as follows.
  • a nanoindenter (“TriboIndenter TI950” manufactured by HYSITRON (Heiditron) Co., Ltd.) is used.
  • the indenter is placed on the surface of the adhesive layer 2 of the battery packaging material (the surface on which the adhesive layer 2 is exposed, the direction perpendicular to the stacking direction of the layers).
  • the adhesive used for forming the first adhesive layer 13 is preferably a resin composition containing a modified thermoplastic resin graft-modified with an unsaturated carboxylic acid or unsaturated carboxylic acid derivative component.
  • the modified thermoplastic resin preferably includes a resin obtained by modifying a polyolefin resin, a styrene elastomer, a polyester elastomer or the like with an unsaturated carboxylic acid derivative component.
  • the said resin may be used individually by 1 type, and may be used in combination of 2 or more types.
  • the unsaturated carboxylic acid derivative component include unsaturated carboxylic acid anhydrides and unsaturated carboxylic acid esters. As the unsaturated carboxylic acid derivative component, one kind may be used alone, or two or more kinds may be used in combination.
  • polyolefin resin in the modified thermoplastic resin examples include low density polyethylene, medium density polyethylene, high density polyethylene; ethylene- ⁇ olefin copolymer; homo, block or random polypropylene; propylene- ⁇ olefin copolymer; Examples include copolymers obtained by copolymerizing polar molecules such as acrylic acid and methacrylic acid; polymers such as crosslinked polyolefins, and the like.
  • One type of polyolefin resin may be used alone, or two or more types of combinations may be used.
  • styrenic elastomer in the modified thermoplastic resin examples include a copolymer of styrene (hard segment) and butadiene or isoprene or a hydrogenated product (soft segment) thereof.
  • One type of polyolefin resin may be used alone, or two or more types of combinations may be used.
  • polyester elastomer in the modified thermoplastic resin examples include a copolymer of crystalline polyester (hard segment) and polyalkylene ether glycol (soft segment).
  • hard segment crystalline polyester
  • soft segment polyalkylene ether glycol
  • One type of polyolefin resin may be used alone, or two or more types of combinations may be used.
  • Examples of the unsaturated carboxylic acid in the modified thermoplastic resin include acrylic acid, methacrylic acid, maleic acid, fumaric acid, itaconic acid, citraconic acid, tetrahydrophthalic acid, bicyclo [2,2,1] hept-2-ene- Examples include 5,6-dicarboxylic acid.
  • Examples of unsaturated carboxylic acid anhydrides include maleic anhydride, itaconic anhydride, citraconic anhydride, tetrahydrophthalic anhydride, bicyclo [2,2,1] hept-2-ene-5,6- And dicarboxylic acid anhydride.
  • Examples of the unsaturated carboxylic acid ester include methyl acrylate, methyl methacrylate, ethyl methacrylate, butyl methacrylate, dimethyl maleate, monomethyl maleate, diethyl fumarate, dimethyl itaconate, diethyl citraconic acid, tetrahydro And esters of unsaturated carboxylic acids such as dimethyl phthalic anhydride and dimethyl bicyclo [2,2,1] hept-2-ene-5,6-dicarboxylate.
  • modified thermoplastic resin with respect to 100 parts by mass of the base thermoplastic resin, about 0.2 to 100 parts by mass of the unsaturated carboxylic acid derivative component is heated and reacted in the presence of a radical initiator. Can be obtained.
  • the reaction temperature is preferably about 50 to 250 ° C, more preferably about 60 to 200 ° C.
  • the reaction time depends on the production method, in the case of a melt graft reaction by a twin screw extruder, it is preferably about 2 to 30 minutes, more preferably about 5 to 10 minutes, which is within the residence time of the extruder.
  • the denaturation reaction can be carried out under both normal pressure and pressurized conditions.
  • the radical initiator used in the modification reaction includes organic peroxides.
  • Various materials can be selected as the organic peroxide depending on temperature conditions and reaction time.
  • alkyl peroxides aryl peroxides, acyl peroxides, ketone peroxides, peroxyketals, peroxycarbonates, peroxides. Examples thereof include oxyesters and hydroperoxides.
  • alkyl peroxides, peroxyketals and peroxyesters are preferable, and di-t-butyl peroxide, 2,5-dimethyl-2,5-di-t- It is more preferable to use butylperoxy-hexyne-3, dicumyl peroxide.
  • the hardness of the first adhesive layer 13 is not limited to the type of resin contained in the adhesive, but by adjusting the molecular weight of the resin, the number of crosslinking points, the modification rate, the stretch rate, the stretch temperature, and the like. It can be adjusted to be a value of.
  • the thickness of the first adhesive layer 13 is preferably about 0.1 to 5 ⁇ m, more preferably about 0.5 to 3 ⁇ m.
  • the hardness of the polyester film layer 11 measured by the nanoindentation method is preferably about 300 to 400 MPa, more preferably about 300 to 350 MPa.
  • the hardness of the polyamide film layer 12 measured by the nanoindentation method is preferably about 200 to 400 MPa, more preferably about 200 to 350 MPa.
  • the hardness measured by the nanoindentation method of the polyester film layer 11 and the polyamide film layer 12 is a measuring object of hardness in the measuring method of the hardness in the above-mentioned 1st contact bonding layer 13, respectively. Can be measured in the same manner as the first adhesive layer 13 except that the polyester film layer 11 or the polyamide film layer 12 is used and the indentation load is 100 ⁇ N.
  • the base material layer 1 may further include other layers in addition to the polyester film layer 11, the first adhesive layer 13, and the polyamide film layer 12.
  • the material for forming the other layers is not particularly limited as long as it has insulating properties. Examples of the material forming the other layer include polyester, polyamide, epoxy resin, acrylic resin, fluorine resin, polyurethane, silicon resin, phenol resin, polyetherimide, polyimide, and a mixture or copolymer thereof. It is done.
  • the thickness of the other layers is preferably about 0.1 to 20 ⁇ m, more preferably about 0.5 to 10 ⁇ m.
  • a lubricant is preferably attached to the surface of the base material layer 1 from the viewpoint of improving the moldability of the battery packaging material.
  • a lubricant Preferably the amide type lubricant illustrated in the below-mentioned heat-meltable resin layer is mentioned.
  • the amount of the lubricant is not particularly limited, but is preferably about 3 mg / m 2 or more, more preferably 4 to 15 mg / m 2 in an environment of a temperature of 24 ° C. and a relative humidity of 60%.
  • about m 2 more preferably about 5 to 14 mg / m 2 is mentioned.
  • the thickness of the base material layer 1 is preferably about 4 ⁇ m or more, more preferably about 10 to 75 ⁇ m from the viewpoint of making the battery packaging material excellent in insulation while reducing the total thickness of the battery packaging material. More preferably, about 10 to 50 ⁇ m is mentioned.
  • the adhesive layer 2 is a layer provided between the base material layer 1 and the barrier layer 3 in order to firmly bond them.
  • the adhesive layer 2 is formed of an adhesive capable of bonding the base material layer 1 and the barrier layer 3 together.
  • the hardness of the adhesive layer 2 measured by the nanoindentation method is 50 MPa or less.
  • the hardness measured by the nanoindentation method of the first adhesive layer 13 and the adhesive layer 2 is both 50 MPa or less, and thus exhibits excellent moldability. It becomes possible to do.
  • the method for measuring the hardness of the adhesive layer 2 is as described above.
  • the hardness of the adhesive layer 2 is preferably about 10 to 50 MPa, more preferably about 20 to 40 MPa.
  • the adhesive used for forming the adhesive layer 2 is not particularly limited as long as it has the above-mentioned hardness after the adhesive layer 2 is formed, and may be a two-component curable adhesive. Also, a one-component curable adhesive may be used. Furthermore, the bonding mechanism of the adhesive used for forming the adhesive layer 2 is not particularly limited, and may be any of a chemical reaction type, a solvent volatilization type, a heat melting type, a hot pressure type, and the like.
  • adhesive components that can be used to form the adhesive layer 2 include polyester resins such as polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, polyethylene isophthalate, and copolyester; polyethers Polyurethane adhesive; epoxy resin; phenolic resin; polyamide resin such as nylon 6, nylon 66, nylon 12, copolymer polyamide; polyolefin resin such as polyolefin, carboxylic acid modified polyolefin, metal modified polyolefin , Polyvinyl acetate resin; cellulose adhesive; (meth) acrylic resin; polyimide resin; polycarbonate; amino resin such as urea resin and melamine resin; chloroprene rubber, nitrile rubber, styrene - rubbers such as butadiene rubber, silicone-based resins. These adhesive components may be used individually by 1 type, and may be used in combination of 2 or more type. Among these adhesive components, a polyurethane
  • the polyurethane adhesive is a polyurethane adhesive containing a main component containing a polyol component (A) and a curing agent containing a polyisocyanate component (B), and the polyol component (A) is a polyester polyol (A1). ), And the polyester polyol (A1) is a polyester polyol having a number average molecular weight of about 5,000 to 50,000, which is composed of a polybasic acid component and a polyhydric alcohol component, and is aromatic in 100 mol% of the polybasic acid component.
  • the polybasic acid component is contained in an amount of about 45 to 95 mol%, and the tensile stress at 100% elongation of the adhesive layer is about 100 kg / cm 2 or more and about 500 kg / cm 2 or less.
  • a polyurethane adhesive for battery packaging materials containing a main agent and a polyisocyanate curing agent, wherein the main agent comprises 5 to 50% by weight of a polyester polyol (A1) having a glass transition temperature of 40 ° C. or higher and a glass transition temperature.
  • the equivalent ratio [NCO] / ([OH] + [COOH]) of isocyanate groups contained in the agent is about 1 to 30.
  • the adhesive containing resin containing either ((A) or (B)) is mentioned. That is, a polyacrylic adhesive, a modified polypropylene adhesive, an adhesive containing a silane coupling agent, an adhesive containing a titanate coupling agent, and the like can be suitably used.
  • the hardness of the adhesive layer 2 is not only the type of resin contained in the adhesive, but also the molecular weight of the resin and the number of crosslinking points, the ratio of the main agent and the curing agent, the dilution ratio of the main agent and the curing agent, the drying temperature, By adjusting the aging temperature, the aging time, etc., it is possible to adjust to the above values.
  • the thickness of the adhesive layer 2 is not particularly limited as long as it exhibits a function as an adhesive layer, and may be, for example, about 1 to 10 ⁇ m, preferably about 2 to 5 ⁇ m.
  • the barrier layer 3 is a layer that functions as a barrier layer for preventing water vapor, oxygen, light, and the like from entering the battery, in addition to improving the strength of the battery packaging material.
  • the metal constituting the barrier layer 3 include aluminum, stainless steel, and titanium, and preferably aluminum.
  • the barrier layer 3 can be formed of a metal foil, a metal vapor-deposited film, an inorganic oxide vapor-deposited film, a carbon-containing inorganic oxide vapor-deposited film, a film provided with these vapor-deposited films, or the like, and preferably formed of a metal foil. More preferably, it is formed of an aluminum foil.
  • annealed aluminum JIS H4160: 1994 A8021H-O, JIS H4160: 1994 A8079H-O.
  • a soft aluminum foil for example, annealed aluminum (JIS H4160: 1994 A8021H-O, JIS H4160: 1994 A8079H-O).
  • the thickness of the barrier layer 3 is not particularly limited as long as it functions as a barrier layer such as water vapor, but can be, for example, about 10 to 80 ⁇ m, preferably about 10 to 50 ⁇ m, more preferably about 10 to 45 ⁇ m. .
  • the barrier layer 3 is preferably subjected to chemical conversion treatment on at least one side, preferably both sides, in order to stabilize adhesion, prevent dissolution and corrosion, and the like.
  • the chemical conversion treatment refers to a treatment for forming an acid-resistant film on the surface of the barrier layer.
  • chromic acid compounds such as chromium nitrate, chromium fluoride, chromium sulfate, chromium acetate, chromium oxalate, chromium biphosphate, chromic acetyl acetate, chromium chloride, potassium sulfate chromium, etc.
  • X represents a hydrogen atom, a hydroxyl group, an alkyl group, a hydroxyalkyl group, an allyl group or a benzyl group.
  • R 1 and R 2 are the same or different and each represents a hydroxyl group, an alkyl group, or a hydroxyalkyl group.
  • examples of the alkyl group represented by X, R 1 and R 2 include a methyl group, an ethyl group, an n-propyl group, an isopropyl group, an n-butyl group, an isobutyl group, Examples thereof include a linear or branched alkyl group having 1 to 4 carbon atoms such as a tert-butyl group.
  • Examples of the hydroxyalkyl group represented by X, R 1 and R 2 include a hydroxymethyl group, a 1-hydroxyethyl group, a 2-hydroxyethyl group, a 1-hydroxypropyl group, a 2-hydroxypropyl group, 3- C1-C4 straight or branched chain in which one hydroxyl group such as hydroxypropyl group, 1-hydroxybutyl group, 2-hydroxybutyl group, 3-hydroxybutyl group, 4-hydroxybutyl group is substituted
  • An alkyl group is mentioned.
  • the alkyl group and hydroxyalkyl group represented by X, R 1 and R 2 may be the same or different.
  • X is preferably a hydrogen atom, a hydroxyl group or a hydroxyalkyl group.
  • the number average molecular weight of the aminated phenol polymer having a repeating unit represented by the general formulas (1) to (4) is preferably, for example, 500 to 1,000,000, more preferably about 1,000 to 20,000. preferable.
  • a phosphoric acid is coated with a metal oxide such as aluminum oxide, titanium oxide, cerium oxide, tin oxide, or barium sulfate fine particles dispersed therein.
  • a method of forming a corrosion-resistant treatment layer on the surface of the barrier layer 3 by performing a baking treatment at about 150 ° C. or higher is mentioned.
  • a resin layer obtained by crosslinking a cationic polymer with a crosslinking agent may be further formed on the corrosion-resistant treatment layer.
  • examples of the cationic polymer include polyethyleneimine, an ionic polymer complex composed of a polymer having polyethyleneimine and a carboxylic acid, a primary amine graft acrylic resin obtained by graft polymerization of a primary amine on an acrylic main skeleton, and polyallylamine. Or the derivative, aminophenol, etc. are mentioned.
  • these cationic polymers only one type may be used, or two or more types may be used in combination.
  • examples of the crosslinking agent include a compound having at least one functional group selected from the group consisting of an isocyanate group, a glycidyl group, a carboxyl group, and an oxazoline group, and a silane coupling agent. As these crosslinking agents, only one type may be used, or two or more types may be used in combination.
  • At least the surface on the inner layer side of the aluminum alloy foil is firstly immersed in an alkali soaking method, electrolytic cleaning method, acid cleaning method, electrolytic acid cleaning method.
  • Treatment liquid (aqueous solution) mainly composed of a mixture of metal salts, or treatment liquid (aqueous solution) principally composed of a non-metallic phosphate and a mixture of these non-metallic salts, or these and an acrylic resin
  • a treatment liquid (aqueous solution) composed of a mixture with a water-based synthetic resin such as a phenol resin or a urethane resin is applied by a known coating method such as a roll coating method, a gravure printing method, or a dipping method.
  • the acid-resistant coating it is possible to form the acid-resistant coating.
  • a chromium phosphate salt treatment solution when treated with a chromium phosphate salt treatment solution, it becomes an acid-resistant film made of chromium phosphate, aluminum phosphate, aluminum oxide, aluminum hydroxide, aluminum fluoride, etc., and treated with a zinc phosphate salt treatment solution.
  • an acid-resistant film made of zinc phosphate hydrate, aluminum phosphate, aluminum oxide, aluminum hydroxide, aluminum fluoride or the like is obtained.
  • an acid-resistant film for example, at least the surface on the inner layer side of the aluminum foil, first, an alkali dipping method, an electrolytic cleaning method, an acid cleaning method, an electrolytic acid cleaning method, an acid activity
  • An acid-resistant film can be formed by performing a degreasing process by a known processing method such as a chemical conversion method and then performing a known anodizing process on the degreasing surface.
  • acid-resistant films include phosphate-based and chromic acid-based films.
  • phosphate-based and chromic acid-based films examples include zinc phosphate, iron phosphate, manganese phosphate, calcium phosphate, and chromium phosphate.
  • chromic acid system examples include chromium chromate.
  • an acid-resistant film by forming an acid-resistant film such as phosphate, chromate, fluoride, triazine thiol compound, between the aluminum and the base material layer at the time of embossing molding
  • an acid-resistant film such as phosphate, chromate, fluoride, triazine thiol compound
  • hydrogen fluoride generated by the reaction between electrolyte and moisture prevents dissolution and corrosion of the aluminum surface, especially the dissolution and corrosion of aluminum oxide present on the aluminum surface, and adhesion of the aluminum surface This improves the wettability and prevents delamination between the base material layer and aluminum at the time of heat sealing.
  • embossed type it shows the effect of preventing delamination between the base material layer and aluminum at the time of press molding.
  • an aqueous solution composed of three components of a phenol resin, a chromium (III) fluoride compound, and phosphoric acid is applied to the aluminum surface, and the dry baking treatment is good.
  • the acid-resistant film includes a layer having cerium oxide, phosphoric acid or phosphate, an anionic polymer, and a crosslinking agent that crosslinks the anionic polymer, and the phosphoric acid or phosphate is 1 to 100 parts by mass may be blended with 100 parts by mass of cerium oxide. It is preferable that the acid-resistant film has a multilayer structure further including a layer having a cationic polymer and a crosslinking agent for crosslinking the cationic polymer.
  • the anionic polymer is poly (meth) acrylic acid or a salt thereof, or a copolymer containing (meth) acrylic acid or a salt thereof as a main component.
  • the said crosslinking agent is at least 1 sort (s) chosen from the group which has a functional group in any one of an isocyanate group, a glycidyl group, a carboxyl group, and an oxazoline group, and a silane coupling agent.
  • the phosphoric acid or phosphate is preferably condensed phosphoric acid or condensed phosphate.
  • chemical conversion treatment only one type of chemical conversion treatment may be performed, or two or more types of chemical conversion processing may be performed in combination. Furthermore, these chemical conversion treatments may be carried out using one kind of compound alone, or may be carried out using a combination of two or more kinds of compounds.
  • chemical conversion treatments chromic acid chromate treatment, chromate treatment combining a chromic acid compound, a phosphoric acid compound, and an aminated phenol polymer are preferable.
  • the acid-resistant film include those containing at least one of phosphates, chromates, fluorides, and triazine thiol compounds.
  • An acid resistant film containing a cerium compound is also preferable.
  • cerium compound cerium oxide is preferable.
  • the acid resistant film examples include a phosphate film, a chromate film, a fluoride film, and a triazine thiol compound film.
  • a phosphate film examples include a phosphate film, a chromate film, a fluoride film, and a triazine thiol compound film.
  • an acid-resistant film one of these may be used, or a plurality of combinations may be used.
  • a treatment liquid composed of a mixture of a metal phosphate and an aqueous synthetic resin, or a mixture of a non-metal phosphate and an aqueous synthetic resin It may be formed with a treatment liquid.
  • the composition of the acid resistant film can be analyzed using, for example, time-of-flight secondary ion mass spectrometry.
  • time-of-flight secondary ion mass spectrometry for example, a peak derived from at least one of Ce + and Cr + is detected.
  • phosphoric acid or phosphate is used for the acid-resistant film, for example, a peak derived from PO 3 ⁇ is detected.
  • the surface of the aluminum alloy foil is provided with an acid resistant film containing at least one element selected from the group consisting of phosphorus, chromium and cerium.
  • the acid-resistant film on the surface of the aluminum alloy foil of the battery packaging material contains at least one element selected from the group consisting of phosphorus, chromium, and cerium using X-ray photoelectron spectroscopy.
  • the heat-fusible resin layer, the adhesive layer, and the like laminated on the aluminum alloy foil are physically peeled off.
  • the aluminum alloy foil is placed in an electric furnace at about 300 ° C. for about 30 minutes to remove organic components present on the surface of the aluminum alloy foil. Thereafter, the surface of the aluminum alloy foil is confirmed to contain these elements using X-ray photoelectron spectroscopy.
  • the amount of the acid-resistant film to be formed on the surface of the barrier layer 3 in the chemical conversion treatment is not particularly limited.
  • a chromic acid compound is present per 1 m 2 of the surface of the barrier layer 3.
  • the thickness of the acid-resistant film is not particularly limited, but is preferably about 1 nm to 20 ⁇ m, more preferably about 1 to 100 nm, from the viewpoint of the cohesive strength of the film and the adhesive strength with the barrier layer and the heat-fusible resin layer. More preferably, about 1 to 50 nm is mentioned.
  • the thickness of the acid-resistant film can be measured by observation with a transmission electron microscope, or a combination of observation with a transmission electron microscope and energy dispersive X-ray spectroscopy or electron energy loss spectroscopy.
  • a solution containing a compound used for forming an acid-resistant film is applied to the surface of the barrier layer by a bar coating method, a roll coating method, a gravure coating method, a dipping method, etc., and then the temperature of the barrier layer is 70. It is performed by heating to about 200 ° C.
  • the barrier layer may be previously subjected to a degreasing treatment by an alkali dipping method, an electrolytic cleaning method, an acid cleaning method, an electrolytic acid cleaning method, or the like. By performing the degreasing process in this manner, it is possible to more efficiently perform the chemical conversion process on the surface of the barrier layer.
  • the heat-fusible resin layer 4 corresponds to the innermost layer, and is a layer that heat-fuses the heat-fusible resin layers and seals the battery element when the battery is assembled.
  • the resin component used in the heat-fusible resin layer 4 is not particularly limited as long as it can be heat-sealed, and examples thereof include polyolefins, cyclic polyolefins, carboxylic acid-modified polyolefins, and carboxylic acid-modified cyclic polyolefins. It is done. That is, the heat-fusible resin layer 4 may include a polyolefin skeleton, and preferably includes a polyolefin skeleton. The fact that the heat-fusible resin layer 4 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited.
  • a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • the peak may be small and may not be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • polystyrene resin examples include polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, and linear low density polyethylene; homopolypropylene, polypropylene block copolymer (for example, block copolymer of propylene and ethylene), polypropylene And a random copolymer (eg, a random copolymer of propylene and ethylene); an ethylene-butene-propylene terpolymer; and the like.
  • polyethylene and polypropylene are preferable.
  • the cyclic polyolefin is a copolymer of an olefin and a cyclic monomer
  • examples of the olefin that is a constituent monomer of the cyclic polyolefin include ethylene, propylene, 4-methyl-1-pentene, styrene, butadiene, and isoprene.
  • Examples of the cyclic monomer that is a constituent monomer of the cyclic polyolefin include cyclic alkenes such as norbornene; specifically, cyclic dienes such as cyclopentadiene, dicyclopentadiene, cyclohexadiene, and norbornadiene.
  • cyclic alkene is preferable, and norbornene is more preferable.
  • the carboxylic acid-modified polyolefin is a polymer modified by block polymerization or graft polymerization of the polyolefin with carboxylic acid.
  • Examples of the carboxylic acid used for modification include maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride, itaconic anhydride and the like.
  • the carboxylic acid-modified cyclic polyolefin is obtained by copolymerizing a part of the monomer constituting the cyclic polyolefin in place of the ⁇ , ⁇ -unsaturated carboxylic acid or its anhydride, or by ⁇ , ⁇ with respect to the cyclic polyolefin.
  • the cyclic polyolefin to be modified with carboxylic acid is the same as described above.
  • the carboxylic acid used for modification is the same as that used for modification of the polyolefin.
  • carboxylic acid-modified polyolefin is preferable; carboxylic acid-modified polypropylene is more preferable.
  • the heat-fusible resin layer 4 may be formed of one kind of resin component alone or may be formed of a blend polymer in which two or more kinds of resin components are combined. Furthermore, the heat-fusible resin layer 4 may be formed of only one layer, but may be formed of two or more layers using the same or different resin components.
  • the heat-fusible resin layer 4 may contain a lubricant or the like as necessary.
  • the lubricant is not particularly limited, and a known lubricant can be used, and examples thereof include those exemplified in the base material layer 1 described above.
  • One type of lubricant may be used alone, or two or more types may be used in combination.
  • the amount of lubricant present on the surface of the heat-fusible resin layer 4 is not particularly limited. From the viewpoint of improving the moldability of the electronic packaging material, it is preferably 10 to 10 at a temperature of 24 ° C. and a relative humidity of 60%. About 50 mg / m 2 , more preferably about 15 to 40 mg / m 2 is mentioned.
  • the thickness of the heat-fusible resin layer 4 is not particularly limited as long as it functions as a heat-fusible resin layer.
  • the thickness is about 100 ⁇ m or less, preferably about 85 ⁇ m or less, more preferably 15 to 85 ⁇ m.
  • the thickness of the second adhesive layer 5 described later is about 10 ⁇ m or more
  • the thickness of the heat-fusible resin layer 4 is preferably about 60 ⁇ m or less, more preferably about 15 to 45 ⁇ m.
  • the thickness of the heat-fusible resin layer 4 is preferably about 20 ⁇ m or more. More preferably, the thickness is about 35 to 85 ⁇ m.
  • the second adhesive layer 5 is a layer provided between the barrier layer 3 and the heat-fusible resin layer 4 as necessary in order to firmly bond the barrier layer 3 and the heat-fusible resin layer 4.
  • the second adhesive layer 5 is formed of a resin capable of bonding the barrier layer 3 and the heat-fusible resin layer 4.
  • the resin used for forming the second adhesive layer 5 the adhesive mechanism, the kind of adhesive component, and the like can be the same as the adhesive exemplified in the adhesive layer 2.
  • the resin used for forming the second adhesive layer 5 include polyolefin resins such as polyolefin, cyclic polyolefin, carboxylic acid-modified polyolefin, and carboxylic acid-modified cyclic polyolefin exemplified in the above-mentioned heat-fusible resin layer 4. Can be used.
  • the polyolefin is preferably a carboxylic acid-modified polyolefin, and particularly preferably a carboxylic acid-modified polypropylene.
  • the second adhesive layer 5 may include a polyolefin skeleton, and preferably includes a polyolefin skeleton.
  • the fact that the second adhesive layer 5 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited.
  • a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • the peak may be small and may not be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • the second adhesive layer 5 is a resin composition containing an acid-modified polyolefin and a curing agent. It may be a cured product.
  • Preferred examples of the acid-modified polyolefin include the same carboxylic acid-modified polyolefin and carboxylic acid-modified cyclic polyolefin exemplified in the heat-fusible resin layer 4.
  • the curing agent is not particularly limited as long as it can cure the acid-modified polyolefin.
  • the curing agent include an epoxy curing agent, a polyfunctional isocyanate curing agent, a carbodiimide curing agent, and an oxazoline curing agent.
  • the epoxy curing agent is not particularly limited as long as it is a compound having at least one epoxy group.
  • examples of the epoxy curing agent include epoxy resins such as bisphenol A diglycidyl ether, modified bisphenol A diglycidyl ether, novolac glycidyl ether, glycerin polyglycidyl ether, and polyglycerin polyglycidyl ether.
  • the polyfunctional isocyanate curing agent is not particularly limited as long as it is a compound having two or more isocyanate groups.
  • Specific examples of the polyfunctional isocyanate-based curing agent include isophorone diisocyanate (IPDI), hexamethylene diisocyanate (HDI), tolylene diisocyanate (TDI), diphenylmethane diisocyanate (MDI), those obtained by polymerizing or nurating these, Examples thereof include mixtures and copolymers with other polymers.
  • the carbodiimide curing agent is not particularly limited as long as it is a compound having at least one carbodiimide group (—N ⁇ C ⁇ N—).
  • a polycarbodiimide compound having at least two carbodiimide groups is preferable.
  • the oxazoline-based curing agent is not particularly limited as long as it is a compound having an oxazoline skeleton.
  • Specific examples of the oxazoline-based curing agent include Epocros series manufactured by Nippon Shokubai Co., Ltd.
  • the curing agent may be composed of two or more kinds of compounds.
  • the content of the curing agent in the resin composition forming the second adhesive layer 5 is preferably in the range of about 0.1 to 50% by mass, and more preferably in the range of about 0.1 to 30% by mass. Preferably, it is in the range of about 0.1 to 10% by mass.
  • the second adhesive layer 5 can also be suitably formed using an adhesive.
  • the adhesive for example, a non-crystalline polyolefin resin (A) having a carboxyl group, a polyfunctional isocyanate compound (B), and a tertiary amine having no functional group that reacts with the polyfunctional isocyanate compound (B) ( C), the polyfunctional isocyanate compound (B) is contained in an amount of 0.3 to 10 mol of the isocyanate group with respect to 1 mol of the total carboxyl groups, and 1 mol of the total carboxyl groups. And the one formed from the adhesive composition containing the tertiary amine (C) in the range of 1 to 10 mol.
  • a styrene-type thermoplastic elastomer (A), a tackifier (B), and a polyisocyanate (C) are contained, a styrene-type thermoplastic elastomer (A), a tackifier ( And 20) to 90% by weight of the styrenic thermoplastic elastomer (A) and 10 to 80% by weight of the tackifier (B) in a total of 100% by weight of the styrene thermoplastic elastomer (A).
  • the thickness of the second adhesive layer 5 is not particularly limited as long as it functions as an adhesive layer.
  • the adhesive exemplified in the adhesive layer 2 it is preferably about 2 to 10 ⁇ m, more preferably 2 to 5 ⁇ m may be mentioned.
  • the resin exemplified in the heat-fusible resin layer 4 it is preferably about 2 to 50 ⁇ m, more preferably about 10 to 40 ⁇ m.
  • a cured product of an acid-modified polyolefin and a curing agent it is preferably about 30 ⁇ m or less, more preferably about 0.1 to 20 ⁇ m, and still more preferably about 0.5 to 5 ⁇ m.
  • the thickness after drying and curing is about 1 to 30 g / m 2 .
  • the second adhesive layer 5 is a cured product of a resin composition containing an acid-modified polyolefin and a curing agent, the second adhesive layer 5 is formed by applying the resin composition and curing it by heating or the like. be able to.
  • the base material layer 1 (barrier layer of the base material layer 1) is optionally formed. If necessary, a surface coating layer 6 may be provided on the side opposite to (3).
  • the surface coating layer 6 is a layer located in the outermost layer when the battery is assembled.
  • the surface coating layer 6 can be formed of, for example, polyvinylidene chloride, polyester resin, urethane resin, acrylic resin, epoxy resin, or the like. Of these, the surface coating layer 6 is preferably formed of a two-component curable resin. Examples of the two-component curable resin for forming the surface coating layer 6 include a two-component curable urethane resin, a two-component curable polyester resin, and a two-component curable epoxy resin. Moreover, you may mix
  • Examples of the additive include fine particles having a particle size of about 0.5 nm to 5 ⁇ m.
  • the material of the additive is not particularly limited, and examples thereof include metals, metal oxides, inorganic substances, and organic substances.
  • the shape of the additive is not particularly limited, and examples thereof include a spherical shape, a fibrous shape, a plate shape, an indeterminate shape, and a balloon shape.
  • Specific additives include talc, silica, graphite, kaolin, montmorilloid, montmorillonite, synthetic mica, hydrotalcite, silica gel, zeolite, aluminum hydroxide, magnesium hydroxide, zinc oxide, magnesium oxide, aluminum oxide, Neodymium oxide, antimony oxide, titanium oxide, cerium oxide, calcium sulfate, barium sulfate, calcium carbonate, calcium silicate, lithium carbonate, calcium benzoate, calcium oxalate, magnesium stearate, alumina, carbon black, carbon nanotubes, high Melting
  • money, aluminum, copper, nickel etc. are mentioned.
  • additives may be used individually by 1 type, and may be used in combination of 2 or more type.
  • silica, barium sulfate, and titanium oxide are preferably used from the viewpoints of dispersion stability and cost.
  • the surface of the additive may be subjected to various surface treatments such as insulation treatment and high dispersibility treatment.
  • the method for forming the surface coating layer 6 is not particularly limited, and examples thereof include a method of applying a two-component curable resin for forming the surface coating layer 6 on one surface of the base material layer 1.
  • the additive may be added to the two-component curable resin, mixed, and then applied.
  • the thickness of the surface coating layer 6 is not particularly limited as long as the above function as the surface coating layer 6 is exhibited.
  • the thickness is about 0.5 to 10 ⁇ m, preferably about 1 to 5 ⁇ m.
  • the production method of the battery packaging material of the present invention is not particularly limited as long as a laminate in which layers of a predetermined composition are laminated is obtained. That is, in the method for producing a battery packaging material of the present invention, at least a step of obtaining a laminate by laminating a base layer, an adhesive layer, a barrier layer, and a heat-fusible resin layer in this order.
  • the base material layer is provided with a first adhesive layer between a polyester film layer and a polyamide film layer, and the adhesive layer and the first adhesive layer are: A method in which the hardness measured by the nanoindentation method is 50 MPa or less, respectively.
  • a laminate in which the base material layer 1, the adhesive layer 2, and the barrier layer 3 are laminated in this order (hereinafter also referred to as “laminate A”) is formed.
  • the laminate A is formed by applying an adhesive used for forming the adhesive layer 2 on the base layer 1 or the barrier layer 3 whose surface is subjected to a chemical conversion treatment, if necessary, a gravure coating method, After applying and drying by a coating method such as a roll coating method, the barrier layer 3 or the base material layer 1 can be laminated and the adhesive layer 2 can be cured by a dry laminating method.
  • the second adhesive layer 5 and the heat-fusible resin layer 4 are laminated on the barrier layer 3 of the laminate A in this order.
  • an adhesive for forming the second adhesive layer 5 is laminated by extrusion method, solution coating, drying at high temperature or baking, etc., and a film is formed on the second adhesive layer 5 in advance.
  • the surface coating layer 6 When the surface coating layer 6 is provided, the surface coating layer 6 is laminated on the surface of the base material layer 1 opposite to the barrier layer 3.
  • the surface coating layer 6 can be formed by, for example, applying the above-described resin for forming the surface coating layer 6 to the surface of the base material layer 1.
  • the order of the step of laminating the barrier layer 3 on the surface of the base material layer 1 and the step of laminating the surface coating layer 6 on the surface of the base material layer 1 are not particularly limited.
  • the barrier layer 3 may be formed on the surface of the base material layer 1 opposite to the surface coating layer 6.
  • a hot roll contact type a hot air type
  • each layer constituting the laminate improves or stabilizes film forming properties, lamination processing, suitability for final processing (pouching, embossing), etc., as necessary. Therefore, surface activation treatment such as corona treatment, blast treatment, oxidation treatment, ozone treatment may be performed.
  • the battery packaging material of the present invention is used in a package for sealing and housing battery elements such as a positive electrode, a negative electrode, and an electrolyte. That is, a battery element including at least a positive electrode, a negative electrode, and an electrolyte can be accommodated in a package formed of the battery packaging material of the present invention to obtain a battery.
  • a battery element including at least a positive electrode, a negative electrode, and an electrolyte is formed using the battery packaging material of the present invention, with the metal terminals connected to each of the positive electrode and the negative electrode protruding outward.
  • a flange portion region where the heat-fusible resin layers are in contact with each other
  • heat-sealing the heat-fusible resin layers of the flange portion to seal the battery
  • a battery using the packaging material is provided.
  • the battery packaging material of the present invention may be used for either a primary battery or a secondary battery, but is preferably a secondary battery.
  • the type of secondary battery to which the battery packaging material of the present invention is applied is not particularly limited.
  • a lithium ion battery, a lithium ion polymer battery, a lead storage battery, a nickel-hydrogen storage battery, a nickel-cadmium storage battery, a nickel- Examples include iron storage batteries, nickel / zinc storage batteries, silver oxide / zinc storage batteries, metal-air batteries, multivalent cation batteries, capacitors, capacitors, and the like.
  • lithium ion batteries and lithium ion polymer batteries are suitable applications for the battery packaging material of the present invention.
  • Example 1 As a base material layer, a polyethylene terephthalate film and a nylon film were laminated by coextrusion, and a biaxially stretched laminated film was prepared.
  • a modified thermoplastic resin graft-modified with an unsaturated carboxylic acid derivative component is contained between the (biaxially stretched) polyethylene terephthalate film (thickness 5 ⁇ m) and the (biaxially stretched) nylon film (thickness 20 ⁇ m). It adhere
  • a barrier layer made of an aluminum foil (JIS H4160: 1994 A8021H-O, thickness 40 ⁇ m) which is subjected to a chemical conversion treatment on both surfaces and has an acid-resistant film on the surface of the (biaxially stretched) nylon film side is a dry laminating method.
  • a two-component polyurethane adhesive polyol compound and aromatic isocyanate compound
  • an adhesive layer is formed on the barrier layer. Formed.
  • Measuring device Time-of-flight secondary ion mass spectrometer TOF.
  • SIMS5 Measurement conditions Primary ion: Double charged ion of Bismuth cluster (Bi 3 ++ ) Primary ion acceleration voltage: 30 kV Mass range (m / z): 0-1500 Measurement range: 100 ⁇ m ⁇ 100 ⁇ m Number of scans: 16 scan / cycle Number of pixels (one side): 256 pixels Etching ions: Ar gas cluster ion beam (Ar-GCIB) Etching ion acceleration voltage: 5.0 kV
  • an amorphous polyolefin resin having a carboxyl group and an adhesive containing a polyfunctional isocyanate compound are applied and dried at 100 ° C., the barrier layer side of the obtained laminate, an unstretched random polypropylene film (
  • the second adhesive layer / heat-sealable resin layer was laminated on the metal foil by passing between two rolls having a thickness of 80 ⁇ m) set to 60 ° C. and bonding them.
  • the obtained laminate was cured (aged) at 40 ° C. for 1 day and at 40 ° C.
  • Comparative Example 1 In the same manner as in Example 1, a laminated film in which a (biaxially stretched) polyethylene terephthalate film (thickness 5 ⁇ m) and a (biaxially stretched) nylon film (thickness 20 ⁇ m) were laminated by coextrusion was prepared as a base material layer. . Next, a barrier layer made of an aluminum foil (JIS H4160: 1994 A8021H-O, thickness 40 ⁇ m) which is subjected to a chemical conversion treatment on both surfaces and has an acid-resistant film on the surface of the (biaxially stretched) nylon film side is a dry laminating method. Was laminated.
  • a barrier layer made of an aluminum foil JIS H4160: 1994 A8021H-O, thickness 40 ⁇ m
  • a urethane-based adhesive was applied to one surface of an aluminum foil provided with an acid-resistant film, and an adhesive layer (thickness 3 ⁇ m) was formed on the barrier layer.
  • an aging treatment is performed at 40 ° C. for 24 hours, thereby (biaxially stretched) polyethylene terephthalate film.
  • a laminate of / first adhesive layer / (biaxially stretched) nylon film / adhesive layer / barrier layer was produced.
  • the hardness of the (biaxially stretched) polyethylene terephthalate film, the first adhesive layer, the (biaxially stretched) nylon film, and the adhesive layer is as shown in Table 2.
  • the aluminum foil used as a barrier layer is provided with an acid resistant film containing chromium oxide and phosphate.
  • the analysis of the acid-resistant film on the barrier layer was performed using time-of-flight secondary ion mass spectrometry as in Example 1. As a result, secondary ions such as Cr + and PO 3 ⁇ were detected from the acid-resistant film.
  • maleic anhydride-modified polypropylene (thickness 40 ⁇ m) as a second adhesive layer and random polypropylene (thickness 40 ⁇ m) as a heat-fusible resin layer are coextruded on the barrier layer of the obtained laminate.
  • the second adhesive layer / heat-fusible resin layer was laminated on the barrier layer.
  • the obtained laminate was aged in a temperature environment of 80 ° C. for 24 hours, and finally heated at 190 ° C. for 2 minutes, whereby (biaxial stretching) polyethylene terephthalate film (5 ⁇ m) / first adhesive layer (1 ⁇ m) ) / (Biaxially stretched) nylon film (20 ⁇ m) / adhesive layer (3 ⁇ m) / barrier layer (40 ⁇ m) / maleic anhydride modified polypropylene (40 ⁇ m) / random polypropylene and (40 ⁇ m) laminated in this order Obtained material.
  • Table 1 shows the layer structure of the battery packaging material.
  • Example 2 and Comparative Example 2-3 As the base material layer, a laminated film in which a biaxially stretched polyethylene terephthalate film (thickness 12 ⁇ m) and a biaxially stretched nylon film (thickness 15 ⁇ m) were laminated by a dry lamination method was prepared. In the laminated film, the biaxially stretched polyethylene terephthalate film and the biaxially stretched nylon film are bonded with a urethane adhesive using a polyol and an isocyanate curing agent.
  • a barrier layer made of an aluminum foil (JIS H4160: 1994 A8021H-O, thickness 40 ⁇ m) subjected to chemical conversion treatment on both sides was laminated on the surface of the biaxially stretched nylon film side by a dry laminating method.
  • a two-component urethane adhesive (a polyol compound and an aromatic isocyanate compound) was applied to one surface of the aluminum foil, and an adhesive layer (thickness 3 ⁇ m) was formed on the barrier layer.
  • the biaxially stretched polyethylene terephthalate film / first adhesive is performed by performing an aging treatment at 40 ° C. for 24 hours.
  • a laminate of layer / biaxially stretched nylon film / adhesive layer / barrier layer was produced.
  • the hardnesses of the biaxially stretched polyethylene terephthalate film, the first adhesive layer, the biaxially stretched nylon film, and the adhesive layer are as shown in Table 2, respectively.
  • the aluminum foil used as a barrier layer is provided with an acid resistant film containing chromium oxide and phosphate.
  • the analysis of the acid-resistant film on the barrier layer was performed using time-of-flight secondary ion mass spectrometry as in Example 1. As a result, secondary ions such as Cr + and PO 3 ⁇ were detected from the acid-resistant film.
  • Example 3 In Comparative Example 2 described above, after laminating the adhesive layer on the barrier layer and the biaxially stretched nylon film side of the base material layer, instead of the aging treatment of “24 hours at 40 ° C.”, “12 at 40 ° C. The biaxially stretched polyethylene terephthalate film (12 ⁇ m) / first adhesive layer (3 ⁇ m) / biaxially stretched nylon film (15 ⁇ m) / adhesive layer in the same manner as in Comparative Example 2 except that the aging process of “time” was performed.
  • a battery packaging material in which (3 ⁇ m) / barrier layer (40 ⁇ m) / maleic anhydride-modified polypropylene (40 ⁇ m) / random polypropylene and (40 ⁇ m) were laminated in this order was obtained.
  • Table 1 shows the layer structure of the battery packaging material. The hardnesses of the biaxially stretched polyethylene terephthalate film, the first adhesive layer, the biaxially stretched nylon film, and the adhesive layer are as shown in Table 2, respectively.
  • Example 4 In Example 1, except that a stainless steel foil (SUS304, thickness 20 ⁇ m) provided with an acid-resistant film by performing chemical conversion treatment (same chemical conversion treatment as in Example 1) on both sides was used as the barrier layer.
  • a stainless steel foil SUS304, thickness 20 ⁇ m
  • 1 (biaxial stretching) polyethylene terephthalate film (5 ⁇ m) / first adhesive layer (1 ⁇ m) / (biaxial stretching) nylon film (20 ⁇ m) / adhesive layer (3 ⁇ m) / barrier layer (20 ⁇ m) /
  • Table 1 shows the layer structure of the battery packaging material. The hardness of the (biaxially stretched) polyethylene terephthalate film, the first adhesive layer, the (biaxially stretched) nylon film, and the adhesive layer is as shown in Table 2.
  • Example 5 In Example 3, except that a stainless steel foil (SUS304, thickness 20 ⁇ m) provided with an acid-resistant film by performing chemical conversion treatment (same chemical conversion treatment as in Example 1) on both surfaces was used as the barrier layer. 3.
  • Table 1 shows the layer structure of the battery packaging material. The hardnesses of the biaxially stretched polyethylene terephthalate film, the first adhesive layer, the biaxially stretched nylon film, and the adhesive layer are as shown in Table 2, respectively.
  • Comparative Example 4 In Comparative Example 2, as a barrier layer, a comparative example was used except that a stainless steel foil (SUS304, thickness 20 ⁇ m) provided with an acid-resistant coating by performing chemical conversion treatment on both surfaces (chemical conversion treatment similar to Example 1) was used. 2 biaxially stretched polyethylene terephthalate film (12 ⁇ m) / first adhesive layer (3 ⁇ m) / biaxially stretched nylon film (15 ⁇ m) / adhesive layer (3 ⁇ m) / barrier layer (20 ⁇ m) / maleic anhydride modified A battery packaging material in which polypropylene (40 ⁇ m) / random polypropylene and (40 ⁇ m) were laminated in this order was obtained. Table 1 shows the layer structure of the battery packaging material. The hardnesses of the biaxially stretched polyethylene terephthalate film, the first adhesive layer, the biaxially stretched nylon film, and the adhesive layer are as shown in Table 2, respectively.
  • the numerical value in parentheses in the layer structure means thickness ( ⁇ m).
  • PET is a biaxially stretched polyethylene terephthalate film
  • Ny is a biaxially stretched nylon film
  • AD is a first adhesive layer formed by coextrusion
  • DL is a first adhesive layer formed by a dry laminating method (Example 2).
  • ALM is aluminum foil
  • SUS stainless steel Steel foil
  • CPP is a heat-fusible resin layer formed from unstretched polypropylene
  • PPa is a second adhesive layer formed from maleic anhydride-modified polypropylene (Examples 2, 3, 5, Comparative Examples 1-4)
  • PP means a heat-fusible resin layer formed of random polypropylene.
  • a nanoindenter (“TriboIndenter TI950” manufactured by HYSITRON (Heiditron) Co., Ltd.) is used. In an environment of 0 ° C., the indenter is applied to the surface of the adhesive layer of the battery packaging material (the surface on which the adhesive layer is exposed and perpendicular to the stacking direction of each layer) for 10 seconds.
  • the indenter was pushed into the adhesive layer to a load of 40 ⁇ N, held in that state for 5 seconds, and then unloaded for 10 seconds.Maximum load P max ( ⁇ N) and contact projected area A at the maximum depth ( ⁇ m 2 ) and the indentation hardness (MPa) was calculated from P max / A
  • the hardness of the first adhesive layer was the same as that of the adhesive layer except that the load was 10 ⁇ N.
  • the surface into which the indenter was pushed was cut in the thickness direction so as to pass through the center of the battery packaging material.
  • the cross-section of the adhesive layer, etc. obtained in this way is exposed, and the cutting was performed using a commercially available rotary microtome or the like.
  • Each of the battery packaging materials obtained above was cut into a rectangle having a length (MD) of 90 mm and a width (TD) of 150 mm to obtain a test sample.
  • the MD of the battery packaging material corresponds to the rolling direction (RD) of the aluminum alloy foil
  • the TD of the battery packaging material corresponds to the TD of the aluminum alloy foil.
  • This sample was formed into a rectangular mold having a diameter of 31.6 mm (MD) and a width of 54.5 mm (TD) (female mold, the surface is JIS B 0659-1: 2002 Annex 1 (reference))
  • the maximum height roughness (nominal value of Rz) specified in Table 2 of the surface roughness standard piece is 3.2 ⁇ m (corner R2.0 mm, ridgeline R1.0 mm), and the corresponding molding die (Male type, surface is JIS B 0659-1: 2002, Annex 1 (Reference)
  • the maximum height roughness (nominal value of Rz) specified in Table 2 of the comparative surface roughness standard piece is 1.6 ⁇ m.
  • the molding depth was changed in units of 0.5mm from the molding depth of 0.5mm at a pressing pressure (surface pressure) of 0.25MPa, and 10 pieces each.
  • the test sample was placed on the female mold and molded so that the heat-fusible resin layer side was positioned on the male mold side.
  • the clearance between the male mold and the female mold was 0.3 mm.
  • light was irradiated with the penlight in the dark room, and it was confirmed whether the pinhole and the crack had arisen in the aluminum foil by permeation
  • Amm is the deepest forming depth where pinholes and cracks do not occur in all 10 samples of aluminum foil, and B is the number of samples where pinholes are generated at the shallowest forming depth where pinholes are generated in aluminum foil.
  • the value calculated by the following formula was rounded off to the second decimal place to obtain the limit molding depth of the battery packaging material. The results are shown in Table 2.
  • Limit forming depth Amm + (0.5mm / 10) x (10-B)
  • PET means a biaxially stretched polyethylene terephthalate film
  • Ny means a biaxially stretched nylon film
  • the battery packaging material (using aluminum foil as the barrier layer) has a molding depth of 7.3 mm or more, and Examples 4 and 5 (using stainless steel foil as the barrier layer) have a molding depth of 3.2 mm. As described above, the moldability was excellent.
  • Comparative Example 1 in which at least one of the hardnesses measured by the nanoindentation method of the adhesive layer and the first adhesive layer exceeds 50 MPa, although the laminated structure is common to Example 1-5.
  • the battery packaging material No.-4 was inferior in moldability as compared with Example 1-5. That is, when Example 1 using aluminum foil as a barrier layer is compared with Comparative Example 1, Example 1 is 0.5 mm better in formability than Comparative Example 1, and when Examples 2 and 3 are compared with Comparative Example 2. Examples 2 and 3 are superior to Comparative Example 3 in moldability by 0.6 mm, and when Examples 2 and 3 are compared with Comparative Example 3, Examples 2 and 3 are superior to Comparative Example 3 in moldability by 0.3 mm. It was. Further, when Examples 4 and 5 using stainless steel foil as a barrier layer were compared with Comparative Example 4, Examples 4 and 5 were superior to Comparative Example 4 in formability by 0.4 to 0.8 mm.

Landscapes

  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Sealing Battery Cases Or Jackets (AREA)
  • Laminated Bodies (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)

Abstract

L'invention concerne un matériau d'encapsulation pour batteries, qui possède une excellente formabilité. Un matériau d'encapsulation pour batteries, qui est configuré à partir d'un stratifié qui comprend séquentiellement au moins une couche de matériau de base, une couche adhésive, une couche barrière et une couche de résine thermofusible dans cet ordre, et qui est configuré de telle sorte que: la couche de matériau de base comprend une première couche de liaison entre une couche de film de polyester et une couche de film de polyamide; et la couche adhésive et la première couche de liaison présentent des duretés de 50 MPa ou moins, telle que déterminée par un procédé de nanoindentation.
PCT/JP2017/042691 2016-11-28 2017-11-28 Matériau d'encapsulation pour batteries, son procédé de production, et batterie WO2018097329A1 (fr)

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WO2020085463A1 (fr) * 2018-10-24 2020-04-30 大日本印刷株式会社 Matériau de conditionnement pour dispositif de stockage d'énergie, son procédé de production et dispositif de stockage d'énergie
WO2020204185A1 (fr) * 2019-04-04 2020-10-08 大日本印刷株式会社 Matériau d'emballage externe pour dispositifs de stockage d'électricité, son procédé de production, et dispositif de stockage d'électricité
WO2020235387A1 (fr) * 2019-05-17 2020-11-26 大日本印刷株式会社 Dispositif de fabrication et procédé de fabrication
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JPWO2020085464A1 (ja) * 2018-10-24 2021-02-15 大日本印刷株式会社 蓄電デバイス用外装材、その製造方法、及び蓄電デバイス
WO2021090950A1 (fr) * 2019-11-08 2021-05-14 大日本印刷株式会社 Film adhésif pour borne métallique ainsi que procédé de fabrication de celui-ci, borne métallique avec film adhésif pour borne métallique, dispositif de stockage électrique mettant en œuvre ce film adhésif pour borne métallique, et procédé de fabrication de dispositif de stockage électrique
CN112912982A (zh) * 2018-10-24 2021-06-04 大日本印刷株式会社 蓄电器件用外装材料、其制造方法和蓄电器件
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CN113348081B (zh) * 2019-01-23 2023-06-02 大日本印刷株式会社 蓄电器件用外包装材料、蓄电器件用外包装材料的制造方法和蓄电器件
WO2020153459A1 (fr) * 2019-01-23 2020-07-30 大日本印刷株式会社 Matériau extérieur pour dispositif de stockage d'énergie, procédé de fabrication de matériau extérieur pour dispositif de stockage d'énergie, et dispositif de stockage d'énergie
WO2021020583A1 (fr) * 2019-08-01 2021-02-04 大日本印刷株式会社 Matériau extérieur pour dispositif de stockage d'électricité, son procédé de fabrication et dispositif de stockage d'électricité
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JP7104137B2 (ja) 2018-10-24 2022-07-20 大日本印刷株式会社 蓄電デバイス用外装材、その製造方法、及び蓄電デバイス
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CN108701780A (zh) 2018-10-23
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