JP2014110114A - External packaging body for electrochemical element - Google Patents

External packaging body for electrochemical element Download PDF

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JP2014110114A
JP2014110114A JP2012263054A JP2012263054A JP2014110114A JP 2014110114 A JP2014110114 A JP 2014110114A JP 2012263054 A JP2012263054 A JP 2012263054A JP 2012263054 A JP2012263054 A JP 2012263054A JP 2014110114 A JP2014110114 A JP 2014110114A
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safety valve
exterior
electrochemical element
exterior body
metal sheet
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JP5969368B2 (en
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Kensuke Nagata
健祐 永田
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Resonac Packaging Corp
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Showa Denko Packaging Co Ltd
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Priority to JP2012263054A priority Critical patent/JP5969368B2/en
Priority to KR1020130142715A priority patent/KR102076372B1/en
Priority to CN201310628166.3A priority patent/CN103855332B/en
Priority to CN201320774834.9U priority patent/CN203850342U/en
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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 of a single cell or a single battery
    • H01M50/116—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material
    • H01M50/124—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material having a layered structure
    • 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 of a single cell or a single battery
    • H01M50/116—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material
    • H01M50/124—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material having a layered structure
    • H01M50/126—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material having a layered structure comprising three or more layers
    • H01M50/129—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material having a layered structure comprising three or more layers with two or more layers of only organic material
    • 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
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material 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
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/12—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by using adhesives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-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
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-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
    • H01G11/80—Gaskets; Sealings
    • 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 of a single cell or a single battery
    • H01M50/102—Primary casings, jackets or wrappings of a single cell or a single battery characterised by their shape or physical structure
    • H01M50/105—Pouches or flexible bags
    • 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 of a single cell or a single battery
    • H01M50/172—Arrangements of electric connectors penetrating the casing
    • H01M50/174—Arrangements of electric connectors penetrating the casing adapted for the shape of the cells
    • H01M50/178—Arrangements of electric connectors penetrating the casing adapted for the shape of the cells for pouch or flexible bag cells
    • 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 of a single cell or a single battery
    • H01M50/183—Sealing members
    • 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
    • H01M50/30—Arrangements for facilitating escape of gases
    • H01M50/317—Re-sealable arrangements
    • 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
    • H01M50/30—Arrangements for facilitating escape of gases
    • H01M50/342—Non-re-sealable arrangements
    • H01M50/3425—Non-re-sealable arrangements in the form of rupturable membranes or weakened parts, e.g. pierced with the aid of a sharp member
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/552—Terminals characterised by their shape
    • H01M50/553—Terminals adapted for prismatic, pouch or rectangular cells
    • H01M50/557—Plate-shaped terminals
    • 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
    • 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

Abstract

PROBLEM TO BE SOLVED: To provide a lamination type external packaging body for an electrochemical element, to which a porous metal sheet as a safety valve can be attached with sufficient strength.SOLUTION: The present invention relates to a lamination type external packaging body for an electrochemical element, in which two sheets of external packaging films 11 each having a sealant layer comprising a polymer compound on one face side are laminated while the sealant layers face each other and the outer peripheral edge part of the layered external packaging films 11 is sealed. A safety valve 2 for preventing internal pressure from rising comprises a porous metal sheet 21, and is fixed to the sealant layer of the external packaging films 11 via an adhesion layer 3 containing a polymer compound while the safety valve 2 is interposed between corresponding outside edge parts in the two sheets of laminated external packaging films 11 so that one end side of the safety valve 2 is disposed at the inside and the other end side is disposed at the outside.

Description

この発明は、内部で発生したガスを外部に逃がすための内圧上昇防止用の安全弁が取り付けられているリチウムイオン電池や、リチウムイオンキャパシタ等のラミネート型の電気化学素子用外装体およびその関連技術に関する。   TECHNICAL FIELD The present invention relates to a lithium ion battery, a laminate type electrochemical element exterior body such as a lithium ion capacitor, and a related technology to which a safety valve for preventing an increase in internal pressure for escaping gas generated inside is attached. .

従来より、ビデオカメラ、ノートパソコン、タブレットパソコン、携帯電話、多機能携帯電話等の電子機器においては、ポータブル化、小型軽量化の要望が強く、それに伴い、これらの電子機器の電源用の電池として用いられるリチウムイオン２次電池においても、小型軽量化、高性能化が強く求められている。   Conventionally, electronic devices such as video cameras, laptop computers, tablet computers, mobile phones, and multifunctional mobile phones have been strongly requested to be portable and small and light, and as a result, as batteries for power supplies of these electronic devices. The lithium ion secondary battery used is also strongly required to be small and light and to have high performance.

また最近では、リチウムイオン２次電池を電気自動車やハイブリッド車の車載電源用に適用すべく、リチウムイオン２次電池の大型化も検討されている。   In recent years, an increase in size of a lithium ion secondary battery has been studied in order to apply the lithium ion secondary battery to an in-vehicle power source of an electric vehicle or a hybrid vehicle.

リチウムイオン２次電池の中でも、アルミラミネートフィルムを使用したラミネート型の薄型電池は、重量やコストの面で優位性が高く、近年注目を集めている。   Among lithium ion secondary batteries, a laminate-type thin battery using an aluminum laminate film is highly advantageous in terms of weight and cost, and has attracted attention in recent years.

ラミネート型のリチウムイオン２次電池は、重ね合わされた２枚の外装フィルムの外周縁部が封止された袋状の外装体を備え、その外装体の内部に発電要素としての電池本体が収容されている。このような電池は、過充電時や過昇温時に電池本体においてガスが発生し易く、そのガスが外装体の内部空間に充満していき外装体内部の内圧が上昇する場合がある。内圧が異常に高くなると、外装体が破裂（バースト）するに至って内部の収容物が飛散することが懸念されることから、このような外装体の破裂を防止する技術が提案されている。   A laminate-type lithium ion secondary battery includes a bag-shaped exterior body in which the outer peripheral edge portions of two superimposed exterior films are sealed, and a battery body as a power generation element is accommodated in the exterior body. ing. In such a battery, gas tends to be generated in the battery body at the time of overcharging or overheating, and the gas may fill the internal space of the exterior body and the internal pressure inside the exterior body may increase. When the internal pressure becomes abnormally high, there is a concern that the outer package will burst (burst) and the internal contents may be scattered. Therefore, a technique for preventing such burst of the outer package has been proposed.

例えば特許文献１に示すリチウムイオン電池においては、外装体の周縁部の一部に、外装体内部で発生するガスを外部に逃がすための安全弁が設けられている。   For example, in the lithium ion battery shown in Patent Document 1, a safety valve for releasing gas generated inside the exterior body to the outside is provided at a part of the peripheral edge of the exterior body.

しかしながら、同文献の安全弁は構造が複雑であるため、電池自体の構造の複雑化を来すとともに、生産性の低下を来すおそれがある。   However, since the structure of the safety valve of the same document is complicated, the structure of the battery itself may be complicated and the productivity may be lowered.

一方、近年になって、特許文献２，３に示すように、ラミネート型と異なる箱封止型や缶封止型の電池において、多孔質金属シートを安全弁として利用する技術が提案されている。   On the other hand, in recent years, as shown in Patent Documents 2 and 3, a technique for using a porous metal sheet as a safety valve in a box-sealed or can-sealed battery different from a laminate-type has been proposed.

この電池は、外装容器の一部を、多孔質金属シートによって構成し、その多孔質金属シートを安全弁として機能させるものであり、電池内部に充満するガスを多孔質金属シートを介して外部に放出させて、内圧が異常に上昇するのを防止するようにしている。   In this battery, a part of the outer container is composed of a porous metal sheet, and the porous metal sheet functions as a safety valve, and the gas filling the battery is released to the outside through the porous metal sheet. In this way, the internal pressure is prevented from rising abnormally.

この電池に採用される安全弁としての多孔質金属シートは構造がシンプルであるため、この構成の安全弁を、上記特許文献１に示すラミネート型の電池に採用できれば、高性能かつ小型コンパクトな安全弁付きのラミネート型電池を提供することができる。   Since the porous metal sheet as a safety valve employed in this battery has a simple structure, if the safety valve having this configuration can be employed in the laminated battery shown in Patent Document 1, a high-performance, small and compact safety valve is provided. A laminated battery can be provided.

特開２００７−２６５７２５号公報JP 2007-265725 A 特開２００４−２２１１２９号公報JP 2004-221129 A 特開２００３−２１７５４６号公報JP 2003-217546 A

しかしながら、ラミネート型電池の外装体を構成する外装フィルムには、高分子化合物によって構成される難接着性のシーラント層が設けられているため、そのシーラント層に例えばヒートシールによって、安全弁としての多孔質金属シートを接着しただけでは、十分な接着強度を得ることができない。仮にそのシーラント層に多孔質金属シートをヒートシールによって接着した外装体の内部に、電池本体としての電解液を封入して電池を作製した場合には、長期間保管したり使用したりすると、多孔質金属シートおよびシーラント層間で層間剥離が発生するおそれがあり、これらの課題が実用化の妨げとなっている。   However, since the exterior film constituting the exterior body of the laminated battery is provided with a hardly adhesive sealant layer composed of a polymer compound, the sealant layer is porous as a safety valve by, for example, heat sealing. A sufficient adhesive strength cannot be obtained only by bonding the metal sheet. If a battery is produced by encapsulating an electrolyte as a battery body inside an exterior body in which a porous metal sheet is bonded to the sealant layer by heat sealing, There is a possibility that delamination may occur between the porous metal sheet and the sealant, and these problems hinder the practical application.

この発明は、上記の課題に鑑みてなされたものであり、安全弁としての多孔質金属シートを十分な強度で取り付けることができるラミネート型の電池等の電気化学素子用外装体およびその関連技術を提供することを目的とする。   The present invention has been made in view of the above problems, and provides an exterior body for an electrochemical element such as a laminate type battery and the like and a related technology to which a porous metal sheet as a safety valve can be attached with sufficient strength. The purpose is to do.

上記課題を解決するため、本発明は、以下の手段を備えるものである。   In order to solve the above problems, the present invention comprises the following means.

［１］片面側のシーラント層が高分子化合物によって構成された２枚の外装フィルムが互いのシーラント層を対向させた状態で積層されるとともに、その積層状の外装フィルムの外周縁部が封止されるようにしたラミネート型の電気化学素子用外装体であって、
多孔質金属シートによって構成される内圧上昇防止用の安全弁の一端側が内部に配置されるとともに、他端側が外部に配置されるようにして、前記安全弁が積層状の２枚の前記外装フィルムにおける対応する外側縁部間に介在された状態で、前記安全弁が前記外装フィルムのシーラント層に、高分子化合物を含む接着層を介して固定されていることを特徴とする電気化学素子用外装体。 [1] Two exterior films in which the sealant layer on one side is made of a polymer compound are laminated with the sealant layers facing each other, and the outer peripheral edge of the laminated exterior film is sealed A laminate-type outer package for an electrochemical element,
One end side of the safety valve for preventing an increase in internal pressure composed of a porous metal sheet is arranged inside, and the other end side is arranged outside, so that the safety valve is compatible with the two laminated outer films. An exterior body for an electrochemical element, wherein the safety valve is fixed to the sealant layer of the exterior film via an adhesive layer containing a polymer compound while being interposed between outer edges.

［２］前記接着層がポリオレフィン系高分子化合物を含んでいる前項１に記載の電気化学素子用外装体。   [2] The outer package for an electrochemical element as described in [1], wherein the adhesive layer contains a polyolefin polymer compound.

［３］前記安全弁としての多孔質金属シートが、多孔質ニッケルシートである前項１または２に記載の電気化学素子用外装体。   [3] The outer package for an electrochemical element according to the above item 1 or 2, wherein the porous metal sheet as the safety valve is a porous nickel sheet.

［４］前記安全弁は、表面が化成処理された多孔質金属シートである前項１〜３のいずれか１項に記載の電気化学素子用外装体。   [4] The exterior body for an electrochemical element according to any one of [1] to [3], wherein the safety valve is a porous metal sheet having a surface subjected to chemical conversion treatment.

［５］前項１〜４のいずれか１項に記載された外装体を備え、
前記外装体に電気化学素子本体が収容されていることを特徴とする電気化学素子。 [5] The exterior body described in any one of items 1 to 4 is provided,
An electrochemical element having an electrochemical element body accommodated in the outer package.

［６］前項１〜４のいずれか１項に記載された外装体を備え、
前記外装体の内部に電池本体である発電要素が収容されていることを特徴とする電池。 [6] The exterior body described in any one of items 1 to 4 is provided,
A battery characterized in that a power generation element as a battery main body is accommodated in the exterior body.

［７］前記安全弁が、リード端子を兼用している前項６に記載の電池。   [7] The battery according to [6], wherein the safety valve also serves as a lead terminal.

［８］片面側のシーラント層が高分子化合物によって構成された２枚の外装フィルムを互いのシーラント層を対向させた状態で積層するとともに、その積層状の外装フィルムの外周縁部を封止するようにしたラミネート型の電気化学素子用外装体の製造方法であって、
多孔質金属シートによって構成される内圧上昇防止用の安全弁を準備する準備工程と、
前記安全弁の一端側が前記外装体の内部に配置されるとともに、他端側が前記外装体の外部に配置されるようにして、前記安全弁を積層状の２枚の前記外装フィルムにおける対応する外側縁部間に介在した状態で、前記安全弁を前記外装フィルムのシーラント層に、高分子化合物を含む接着層を介して固定する接着工程とを含むことを特徴とする電気化学素子用外装体の製造方法。 [8] Two exterior films each having a sealant layer on one side made of a polymer compound are laminated with the sealant layers facing each other, and the outer peripheral edge of the laminated exterior film is sealed. A method for producing a laminate-type outer package for an electrochemical element,
A preparation step of preparing a safety valve for preventing an increase in internal pressure constituted by a porous metal sheet;
One end side of the safety valve is disposed inside the exterior body, and the other end side is disposed outside the exterior body, so that the safety valve is disposed on the corresponding outer edge portion of the two laminated exterior films. A method for producing an exterior body for an electrochemical element, comprising: an adhesion step of fixing the safety valve to a sealant layer of the exterior film through an adhesive layer containing a polymer compound in a state of being interposed therebetween.

［９］前記接着工程を行う前に、前記安全弁としての多孔質金属シートの表面に化成処理を行うようにした前項８に記載の電気化学素子用外装体の製造方法。   [9] The method for producing an exterior body for an electrochemical element according to the above item 8, wherein a chemical conversion treatment is performed on the surface of the porous metal sheet as the safety valve before the bonding step.

［１０］前記接着層は、前記安全弁および前記外装フィルム間に塗布され、かつポリオレフィン系高分子化合物を含む接着剤によって構成されている前項８または９に記載の電気化学素子用外装体の製造方法。   [10] The method for producing an exterior body for an electrochemical element according to the item 8 or 9, wherein the adhesive layer is applied between the safety valve and the exterior film and is composed of an adhesive containing a polyolefin polymer compound. .

［１１］前記接着工程は、前記接着剤をエージングするエージング工程を含んでいる前項１０に記載の電気化学素子用外装体の製造方法。   [11] The method for manufacturing an exterior body for an electrochemical element according to [10], wherein the bonding step includes an aging step of aging the adhesive.

［１２］
前記接着層は、前記安全弁および前記外装フィルム間に配置され、かつポリオレフィン系高分子化合物を含む接着用フィルムによって構成されている前項８または９に記載の電気化学素子用外装体の製造方法。 [12]
10. The method for producing an exterior body for an electrochemical element according to 8 or 9 above, wherein the adhesive layer is disposed between the safety valve and the exterior film and is configured by an adhesive film containing a polyolefin polymer compound.

なお本明細書において、「アルミニウム」の語は、アルミニウムおよびその合金を含む意味で用いる。   In this specification, the term “aluminum” is used to include aluminum and its alloys.

発明［１］の電気化学素子用外装体によれば、安全弁としての多孔質金属シートを高分子化合物を含む接着層を介して外装フィルムのシーラント層に固定しているため、安全弁を十分な強度で取り付けることができる。   According to the exterior body for an electrochemical element of the invention [1], since the porous metal sheet as a safety valve is fixed to the sealant layer of the exterior film through the adhesive layer containing the polymer compound, the safety valve has sufficient strength. It can be attached with.

発明［２］の電気化学素子用外装体によれば、より高い強度で多孔質金属シートを固定することができる。   According to the electrochemical element exterior body of the invention [2], the porous metal sheet can be fixed with higher strength.

発明［３］の電気化学素子用外装体によれば、安全弁として多孔質ニッケルシートを使用しているため、内圧上昇時のガス抜きをより確実に行えて、防爆性をより一層高めることができる。   According to the electrochemical element exterior body of the invention [3], since the porous nickel sheet is used as the safety valve, the degassing can be more reliably performed when the internal pressure is increased, and the explosion-proof property can be further enhanced. .

発明［４］の電気化学素子用外装体によれば、より高い強度で多孔質金属シートを外装フィルムに固定することができる。   According to the electrochemical element exterior body of the invention [4], the porous metal sheet can be fixed to the exterior film with higher strength.

発明［５］の電気化学素子によれば、上記と同様に、安全弁としての多孔質金属シートを外装フィルムに十分な強度で取り付けることができる。   According to the electrochemical element of the invention [5], the porous metal sheet as the safety valve can be attached to the exterior film with sufficient strength as described above.

発明［６］の電池によれば、上記と同様に、安全弁としての多孔質金属シートを十分な強度で外装フィルムに取り付けることができる。   According to the battery of the invention [6], the porous metal sheet as a safety valve can be attached to the exterior film with sufficient strength, as described above.

発明［７］の電池によれば、安全弁をリード端子と兼用しているため、部品点数を削減できて、構造の簡素化および生産性の向上を図ることができる。   According to the battery of the invention [7], since the safety valve is also used as the lead terminal, the number of parts can be reduced, and the structure can be simplified and the productivity can be improved.

発明［８］〜［１２］の製造方法によれば、上記と同様に、安全弁としての多孔質金属シートが十分な強度で外装フィルムに取り付けられた電気化学素子用外装体を製造することができる。   According to the production methods of the inventions [8] to [12], it is possible to produce an exterior body for an electrochemical element in which a porous metal sheet as a safety valve is attached to an exterior film with sufficient strength, as described above. .

図１はこの発明の実施形態である電池用外装体の一例を示す概略図である。FIG. 1 is a schematic view showing an example of a battery case according to an embodiment of the present invention. 図２はこの発明の実施形態である電池用外装体の他の例を示す概略図である。FIG. 2 is a schematic view showing another example of the battery outer package according to the embodiment of the present invention. 図３は実施形態の電池用外装体に適用された多孔質金属シートを示す概略図である。FIG. 3 is a schematic view showing a porous metal sheet applied to the battery case of the embodiment. 図４は上記一例の電池用外装体の製造に用いられたＰＰ接着剤付きの多孔質金属シートを示す概略図である。FIG. 4 is a schematic view showing a porous metal sheet with a PP adhesive used in the production of the battery case of the above example. 図５は上記他の例の電池用外装体の製造に用いられたＰＰフィルム付きの多孔質金属シートを示す概略図である。FIG. 5 is a schematic view showing a porous metal sheet with a PP film used in the production of the battery case of another example. 図６はこの発明の電池用外装体が適用された電池の一例を示す概略図である。FIG. 6 is a schematic view showing an example of a battery to which the battery case of the present invention is applied. 図７はこの発明の電池用外装体が適用された電池の他の例を示す概略図である。FIG. 7 is a schematic view showing another example of a battery to which the battery case of the present invention is applied.

図１および図２はこの発明の実施形態である電池用外装体１を示す概略図である。なお図１および図２においては、発明の理解を容易にするため、厚み方向の寸法割合を実際よりも厚く形成している（以下の図３〜図７においても同じ）。   1 and 2 are schematic views showing a battery outer package 1 according to an embodiment of the present invention. In FIG. 1 and FIG. 2, in order to facilitate understanding of the invention, the dimensional ratio in the thickness direction is formed to be thicker than actual (the same applies to FIGS. 3 to 7 below).

図１および図２に示すように、本実施形態の電池用外装体１は、リチウムイオン２次電池用の外装体として用いられるものである。この外装体１は、積層される２枚の外装フィルム（ラミネートフィルム）１１，１１を備えている。   As shown in FIGS. 1 and 2, the battery outer package 1 of the present embodiment is used as an outer package for a lithium ion secondary battery. The exterior body 1 includes two exterior films (laminate films) 11 and 11 to be laminated.

外装フィルム１１は、例えば内面側（片面側）に配置されたシーラント層と、シーラント層上に積層された中間層と、中間層上に積層された外面層とを備えた３層の積層体によって構成されている。   The exterior film 11 is, for example, a three-layer laminate including a sealant layer disposed on the inner surface side (one surface side), an intermediate layer laminated on the sealant layer, and an outer surface layer laminated on the intermediate layer. It is configured.

シーラント層は、熱接着性（熱可塑性）を有し、かつ金属塩および有機溶剤（エチレンカーボネートやジメチルカーボネート等）に侵食されないような化合物、例えば高密度ポリエチレン、低密度ポリエチレン、直鎖状低密度ポリエチレン、ポリエチレン系アイオノマー、ポリプロピレンのようなポリオレフィン系樹脂等の高分子化合物からなるものを好適に用いることができる。   The sealant layer has thermal adhesiveness (thermoplasticity) and is not eroded by metal salts and organic solvents (ethylene carbonate, dimethyl carbonate, etc.), such as high density polyethylene, low density polyethylene, linear low density What consists of high molecular compounds, such as polyethylene resin, polyethylene-type ionomer, polyolefin resin like a polypropylene, can be used suitably.

または外面層は、電気絶縁性を有するポリエチレンテレフタレート（ＰＥＴ）等のポリエステルや、ナイロン等のポリアミドによって構成されるものを好適に用いることができる。この外面層は、機械的強度を有し、外面層およびシーラント層間に設けられる中間層を保護する役目を担っている。   Alternatively, the outer surface layer can be preferably made of a polyester such as polyethylene terephthalate (PET) having electrical insulating properties or a polyamide such as nylon. This outer surface layer has mechanical strength and plays a role of protecting an intermediate layer provided between the outer surface layer and the sealant layer.

中間層は、金属箔、例えばアルミニウム箔、ＳＵＳ箔によって構成されるものを好適に用いることができ、中でも特にアルミニウム箔によって構成されるものを用いるのが好ましい。この中間層によって、外部からの水分の浸入や内部からの電解液の蒸発が有効に防止されるようになっている。   As the intermediate layer, a metal foil, for example, an aluminum foil or a SUS foil can be preferably used, and among these, an intermediate layer is particularly preferably used. This intermediate layer effectively prevents moisture from entering from the outside and evaporation of the electrolyte from the inside.

以上の構成の２枚の外装フィルム１１，１１が重ね合わされて（積層されて）、その周縁部がシートヒール（熱溶着）されて、袋状の外装体１を作製するものであるが、本実施形態においては、外周縁部の一部に安全弁２が取り付けられている。   The two exterior films 11, 11 having the above configuration are overlapped (laminated), and the periphery thereof is seat-heeled (heat-welded) to produce a bag-shaped exterior body 1. In the embodiment, the safety valve 2 is attached to a part of the outer peripheral edge.

図３に示すように、本実施形態において、安全弁２としては、多数の微細孔が形成された多孔質金属シート２１が用いられる。このシート２１としては例えば、多孔質ニッケル（Ｎｉ）シート、多孔質ニッケル系合金シート、多孔質銅（Ｃｕ）シート、多孔質銅系合金シート、多孔質パラジウム（Ｐｄ）シートを好適に使用することができる。これらの中でも特に、めっき浴の安全性が高く、かつ加工性も良いという理由から、多孔質ニッケルシート、多孔質ニッケル系合金シートを用いるのが好ましい。   As shown in FIG. 3, in the present embodiment, a porous metal sheet 21 in which a large number of micropores are formed is used as the safety valve 2. For example, a porous nickel (Ni) sheet, a porous nickel-based alloy sheet, a porous copper (Cu) sheet, a porous copper-based alloy sheet, or a porous palladium (Pd) sheet is preferably used as the sheet 21. Can do. Among these, it is preferable to use a porous nickel sheet or a porous nickel-based alloy sheet because the safety of the plating bath is high and the workability is good.

また安全弁２としての多孔質金属シート２１は、例えば電析法を用いて製作することができる。   Moreover, the porous metal sheet 21 as the safety valve 2 can be manufactured using, for example, an electrodeposition method.

安全弁２として用いられる多孔質金属シート２１は、その微細孔の孔径が０．１μｍ〜６μｍのものを用いるのが好ましい。すなわち、孔径が大き過ぎる場合には、外装体１の内部に封入される電解液等の液漏れが発生するおそれがある。逆に孔径が小さ過ぎる場合には、外装体１の内圧上昇時におけるガスリーク性（ガス抜き性）が不十分となり、内圧上昇を確実に防止できないおそれがある。   As the porous metal sheet 21 used as the safety valve 2, it is preferable to use a porous metal sheet having a pore diameter of 0.1 μm to 6 μm. That is, when the hole diameter is too large, there is a risk of leakage of the electrolyte solution or the like enclosed in the exterior body 1. On the other hand, when the hole diameter is too small, the gas leakage property (gas venting property) at the time of increasing the internal pressure of the exterior body 1 becomes insufficient, and there is a possibility that the increase of the internal pressure cannot be reliably prevented.

さらに安全弁２としての多孔質金属シート２１は、厚みが１５μｍ〜１５０μｍのものを使用するのが好ましい。すなわち、厚みが厚過ぎる場合には、多孔質金属シート２１と外装フィルム１１との間を確実にシールすることが困難になるおそれがなる。逆に厚みが薄過ぎる場合には、安全弁２として十分な機械的強度を確保できないおそれがある。   Furthermore, it is preferable to use a porous metal sheet 21 as the safety valve 2 having a thickness of 15 μm to 150 μm. That is, if the thickness is too thick, it may be difficult to reliably seal between the porous metal sheet 21 and the exterior film 11. Conversely, when the thickness is too thin, there is a possibility that sufficient mechanical strength as the safety valve 2 cannot be secured.

本実施形態においては、安全弁２としての多孔質金属シート２１の表面に、クロメート処理等による化成処理を施しておくのが好ましい。すなわちこのクロメート処理によって多孔質金属シート２１の表面の反応性を向上させることができ、多孔質金属シート２１を、後述する接着層３を介して外装体１のシーラント層への接着強度を向上させることができる。   In the present embodiment, it is preferable to subject the surface of the porous metal sheet 21 as the safety valve 2 to chemical conversion treatment such as chromate treatment. That is, the reactivity of the surface of the porous metal sheet 21 can be improved by this chromate treatment, and the adhesion strength of the porous metal sheet 21 to the sealant layer of the exterior body 1 is improved via the adhesive layer 3 described later. be able to.

なお、クロメート処理としては、実施例の欄で詳述するように、塗布型のクロメート処理を行うのが好ましい。   As the chromate treatment, it is preferable to perform a coating type chromate treatment as described in detail in the column of Examples.

本実施形態においては、積層状の外装フィルム１１，１１の外周縁部を熱溶着するのと並行して、安全弁２としての多孔質金属シート２１を、外装フィルム１１，１１間に介在させて接着固定するものである。   In the present embodiment, a porous metal sheet 21 as a safety valve 2 is interposed between the exterior films 11 and 11 and bonded in parallel with the heat-sealing of the outer peripheral edges of the laminated exterior films 11 and 11. It is to be fixed.

本実施形態において、多孔質金属シート２１を外装フィルム１１，１１に接着固定する方法としては、接着剤３１を用いる方法と、接着用（溶着用）フィルム３２を用いる方法との２通りの方法を採用することができる。   In this embodiment, as a method for bonding and fixing the porous metal sheet 21 to the exterior films 11, 11, there are two methods, a method using an adhesive 31 and a method using an adhesive (welding) film 32. Can be adopted.

図４に示すように、接着剤３１を用いる方法は、安全弁２としての多孔質金属シート２１の両面における外装フィルム１１，１１との接着面に、予めペースト状態の接着剤３１を塗布しておく。そして図１に示すように、その多孔質金属シート２１をその両側から外装フィルム１１，１１の外周縁部の一部によって挟み込まれるようにして、外装フィルム１１，１１を重ね合わせて配置する。その状態で、重ね合わされた外装フィルム１１，１１の外周縁部のシーラント層同士をヒートシールによって溶着する一方、多孔質金属シート２１に対し外装フィルム１１，１１を両側から挟圧して、多孔質金属シート２１を接着剤３１による接着層３を介して外装フィルム１１，１１のシーラント層にそれぞれ接着固定する。これにより図１に示すように、安全弁２としての多孔質金属シート２１の一部分（一端側）が外部に配置されるとともに、他の部分（他端側）が内部に配置された状態で、外周縁部の全周がシールされた袋状の電池用外装体１が形成される。   As shown in FIG. 4, in the method using the adhesive 31, the adhesive 31 in a paste state is applied in advance to the adhesive surfaces with the exterior films 11 and 11 on both surfaces of the porous metal sheet 21 as the safety valve 2. . Then, as shown in FIG. 1, the exterior films 11 and 11 are overlapped so that the porous metal sheet 21 is sandwiched by a part of the outer peripheral edge of the exterior films 11 and 11 from both sides. In this state, the sealant layers at the outer peripheral edge portions of the overlaid exterior films 11 and 11 are welded together by heat sealing, while the exterior films 11 and 11 are sandwiched from both sides to the porous metal sheet 21 to form a porous metal. The sheet 21 is bonded and fixed to the sealant layers of the exterior films 11 and 11 through the adhesive layer 3 made of the adhesive 31. As a result, as shown in FIG. 1, a part (one end side) of the porous metal sheet 21 as the safety valve 2 is disposed outside, and the other part (the other end side) is disposed inside, A bag-shaped battery case 1 having a sealed peripheral edge is formed.

本実施形態において、接着剤３１の塗布量は、１ｇ／ｍ２〜５ｇ／ｍ２に設定するのが好ましい。すなわち塗布量をこの範囲内に調整することによって、接着剤３１を余分に使用せずに安定状態に確実に接着することができる。 In the present embodiment, the coating amount of the adhesive 31 is preferably set to 1g / m 2 ~5g / m 2 . That is, by adjusting the coating amount within this range, the adhesive 31 can be reliably bonded in a stable state without using an extra amount.

また本実施形態においては、接着剤３１によって、多孔質金属シート２１を外装フィルム１１，１１に接着する際には、接着剤３１をエージング（養生硬化）させることによって、より一層安定状態に接着できて、より一層接着強度を向上させることができる。従って接着剤３１を用いる場合には、エージング処理を行うのが好ましい。   In the present embodiment, when the porous metal sheet 21 is bonded to the exterior films 11 and 11 by the adhesive 31, the adhesive 31 can be bonded in a more stable state by aging (curing and curing). Thus, the adhesive strength can be further improved. Therefore, when the adhesive 31 is used, it is preferable to perform an aging treatment.

エージング条件としては、外装フィルム１１，１１により多孔質金属シート２１を両側から挟持した状態で、挟持圧を０．１ＭＰａ〜１０ＭＰａ、温度を３０℃〜５０℃、期間を２〜９日間に設定するのが好ましい。   As the aging conditions, the sandwiching pressure is set to 0.1 MPa to 10 MPa, the temperature is set to 30 ° C. to 50 ° C., and the period is set to 2 to 9 days in a state where the porous metal sheet 21 is sandwiched from both sides by the exterior films 11 and 11. Is preferred.

一方図５に示すように、接着用フィルム３２を用いる方法は、安全弁２としての多孔質金属シート２１の両面における外装フィルム１１，１１との接着面に、接着用フィルム３２を熱溶着して取り付ける。その後図２に示すように、多孔質金属シート２１をその両側から外装フィルム１１，１１の外周縁部の一部によって挟み込まれるようにして、外装フィルム１１，１１を重ね合わせて配置する。そしてその状態で、重ね合わされた外装フィルム１１，１１の外周縁部のシーラント層同士をヒートシールによって溶着すると同時に、多孔質金属シート２１の接着用フィルム３２とおよび外装フィルム１１，１１のシーラント層とを熱溶着して接着固定する。これにより、安全弁２としての多孔質金属シート２１の一部分（一端側）が外部に配置されるとともに、他の部分（他端側）が内部に配置された状態で、外周縁部の全周がシールされた袋状の電池用外装体１が形成される。   On the other hand, as shown in FIG. 5, in the method using the adhesive film 32, the adhesive film 32 is attached by heat welding to the adhesive surfaces with the exterior films 11 and 11 on both surfaces of the porous metal sheet 21 as the safety valve 2. . Thereafter, as shown in FIG. 2, the exterior films 11, 11 are overlapped so that the porous metal sheet 21 is sandwiched by the outer peripheral edge portions of the exterior films 11, 11 from both sides thereof. And in that state, the sealant layers at the outer peripheral edges of the overlaid exterior films 11 and 11 are welded together by heat sealing, and at the same time, the adhesive film 32 of the porous metal sheet 21 and the sealant layer of the exterior films 11 and 11 Are welded and fixed. Thereby, while the part (one end side) of the porous metal sheet 21 as the safety valve 2 is disposed outside and the other part (the other end side) is disposed inside, the entire circumference of the outer peripheral edge portion is A sealed bag-shaped battery case 1 is formed.

ここで、本実施形態において、接着剤３１および接着用フィルム３２としては、ウレタン系、酸変性ポリオレフィン系、スチレンエラストマー系、アクリル系、シリコーン系、エーテル系、エチレン−酢酸ビニル系、ポリプロプレン系のものを使用でき、中でも、接着性の観点から、アクリル系およびポリプロピレン系のものを使用するのが好ましく、特にポリプロピレン系のものを使用するのが、より一層好ましい。   Here, in this embodiment, as the adhesive 31 and the adhesive film 32, urethane, acid-modified polyolefin, styrene elastomer, acrylic, silicone, ether, ethylene-vinyl acetate, and polypropylene are used. Among them, it is preferable to use acrylic type and polypropylene type, and it is more preferable to use polypropylene type in particular from the viewpoint of adhesiveness.

ところで、本実施形態の外装体１を電池として使用する場合には、内部に、電池本体としての電解液等の発電要素が封入されるとともに、外装体１の外部と内部とを電気的に繋ぐリード端子が設けられる。電解液の封入方法や手順は従来より周知の方法や手順を使用でき、リード端子の取付方法等も、従来より周知の方法を使用することができる。   By the way, when the exterior body 1 of this embodiment is used as a battery, a power generation element such as an electrolytic solution as a battery body is enclosed therein, and the exterior and interior of the exterior body 1 are electrically connected to each other. Lead terminals are provided. Conventionally well-known methods and procedures can be used for the electrolytic solution sealing method and procedures, and conventionally well-known methods can also be used for lead terminal attachment methods and the like.

以上の構成の電池において、内圧が異常に上昇した場合には、内部のガスが、安全弁２を構成する多孔質金属シート２１の微細孔を通って外部に放出されることにより、内圧が過度に上昇するのが防止されて、バーストの発生を確実に防止できて、封入物が飛散するような不具合を確実に防止することができる。   In the battery having the above configuration, when the internal pressure rises abnormally, the internal gas is discharged to the outside through the micropores of the porous metal sheet 21 constituting the safety valve 2, so that the internal pressure is excessively increased. Ascending is prevented, the occurrence of burst can be surely prevented, and the trouble that the inclusions are scattered can be surely prevented.

また本実施形態の電池用外装体１によれば、安全弁２としての多孔質金属シート２１を外装フィルム１１，１１によって挟み込んで接着するだけのものであるため、構造の簡素化を図ることができるとともに、簡単に製造できて、生産効率を向上させることができる。   Moreover, according to the battery exterior body 1 of this embodiment, since the porous metal sheet 21 as the safety valve 2 is merely sandwiched and adhered by the exterior films 11 and 11, the structure can be simplified. At the same time, it can be easily manufactured and the production efficiency can be improved.

なお、本実施形態においては、図６および図７に示すように、安全弁２，２である多孔質金属シート２１，２１を、タブリード等のリード端子４，４と兼用して使用することが可能である。この場合、２本のリード端子のうち、一方のみを、安全弁２と兼用させるようにしても良いし、双方共に、安全弁２と兼用させるようにしても良い。   In this embodiment, as shown in FIGS. 6 and 7, the porous metal sheets 21 and 21 that are the safety valves 2 and 2 can be used also as lead terminals 4 and 4 such as tab leads. It is. In this case, only one of the two lead terminals may be used as the safety valve 2, or both may be used as the safety valve 2.

また、上記実施形態等では、外装体１の内部に、電気化学素子本体として電池本体を封入する場合を例に挙げて説明したが、それだけに限られず、本発明の外装体には、電池本体以外の電気化学素子本体を封入することができる。例えば、本発明の外装体に、コンデンサ本体としての蓄電要素を封入することにより、本発明をラミネート型キャパシタ等のコンデンサ素子にも適用することができる。   Moreover, in the said embodiment etc., although the case where a battery main body was enclosed as an electrochemical element main body inside the exterior body 1 was mentioned as an example, it was not restricted only to that, The exterior body of this invention has other than a battery main body. The electrochemical element body can be encapsulated. For example, the present invention can be applied to a capacitor element such as a laminate type capacitor by enclosing a power storage element as a capacitor body in the outer package of the present invention.

次に本発明に関連した実施例、および本発明の要旨を逸脱する比較例について説明する。   Next, examples related to the present invention and comparative examples that depart from the gist of the present invention will be described.

なお表１において、下地処理とは、多孔質金属シート２１に対する下地処理である。接着手段とは、多孔質金属シート２１と外装フィルム１１とを接着するために用いられる手段である。   In Table 1, the base treatment is a base treatment for the porous metal sheet 21. The adhesion means is means used for adhering the porous metal sheet 21 and the exterior film 11.

＜実施例１＞
外装体１を構成する外装フィルム１１として、シーラント層が延伸ポリプロピレンからなり、中間層がアルミニウム箔からなり、外面層が６ナイロンからなる厚さ０．１ｍｍの３層の積層体を準備した。この外装フィルム１１のサイズは、長さ１００ｍｍ、幅１００ｍｍである。 <Example 1>
As the exterior film 11 constituting the exterior body 1, a three-layer laminate having a thickness of 0.1 mm was prepared, in which the sealant layer was made of stretched polypropylene, the intermediate layer was made of aluminum foil, and the outer surface layer was 6 nylon. The exterior film 11 has a length of 100 mm and a width of 100 mm.

安全弁２を構成する多孔質金属シート２１として、電析法を用いて作製した多孔質ニッケル（Ｎｉ）シートを準備した。このシートは、厚さが０．０５ｍｍ、長さが３０ｍｍ、幅が３０ｍｍである。さらにこのシートは、直径１μｍφの細孔が、１００個／ｃｍ２の密度で形成された多孔質のものである。 As the porous metal sheet 21 constituting the safety valve 2, a porous nickel (Ni) sheet prepared using an electrodeposition method was prepared. This sheet has a thickness of 0.05 mm, a length of 30 mm, and a width of 30 mm. Further, this sheet is a porous sheet in which pores having a diameter of 1 μmφ are formed at a density of 100 / cm 2 .

ポリオレフィン系接着剤（ＰＰ接着剤）３１として、東亜合成株式会社製のホットメルト接着剤「アロンメルト（商標）ＰＰＥＴ−１６００」と、ヘキサメチレンジイソシアナートとを１００：１．５の組成で調合したものを準備した。   As a polyolefin-based adhesive (PP adhesive) 31, a hot-melt adhesive “Aronmelt (trademark) PPET-1600” manufactured by Toa Gosei Co., Ltd. and hexamethylene diisocyanate were prepared in a composition of 100: 1.5. I prepared something.

そして、多孔質Ｎｉシート２１の両面（外装フィルム１１，１１との接着面）に、ＰＰ接着剤３１をヘラを用いて塗布した（図４参照）。このときの塗布量は、２．２ｇ／ｍ２とした。 And PP adhesive 31 was apply | coated to both surfaces (adhesion surface with the exterior films 11 and 11) of the porous Ni sheet 21 using the spatula (refer FIG. 4). The coating amount at this time was 2.2 g / m 2 .

続いて図１に示すように、多孔質Ｎｉシート２１をその両側から２枚の外装フィルム１１，１１の外側縁部、つまり外周縁部の一辺部に挟み込まれるように、外装フィルム１１，１１を重ね合わせて配置する。   Subsequently, as shown in FIG. 1, the exterior films 11, 11 are placed so that the porous Ni sheet 21 is sandwiched between the outer edges of the two exterior films 11, 11 from one side, that is, one side of the outer peripheral edge. Overlay and arrange.

さらにその状態で、重ね合わされた外装フィルム１１，１１の外周縁部をヒートシールによって溶着する一方、多孔質Ｎｉシート２１をＰＰ接着剤３１を介して外装フィルム１１，１１のシーラント層に接着固定することにより、安全弁２（多孔質Ｎｉシート２１）付きの外装体１を作製した。ヒートシールの条件は、温度を１５０℃〜２００℃、圧力を０．１ＭＰａ〜０．３ＭＰａ、時間を２秒〜５秒とした。   Further, in this state, the outer peripheral edge portions of the overlaid exterior films 11 and 11 are welded by heat sealing, and the porous Ni sheet 21 is bonded and fixed to the sealant layer of the exterior films 11 and 11 via the PP adhesive 31. Thus, the outer package 1 with the safety valve 2 (porous Ni sheet 21) was produced. The heat sealing conditions were a temperature of 150 ° C. to 200 ° C., a pressure of 0.1 MPa to 0.3 MPa, and a time of 2 seconds to 5 seconds.

＜初期接着性評価＞
こうして得られた実施例１のサンプル（電池用外装体１）に対し、多孔質Ｎｉシート２１と、外装フィルム１１との間の層間接着強度（初期の層間接着強度）について評価した。 <Initial adhesion evaluation>
The interlayer adhesive strength (initial interlayer adhesive strength) between the porous Ni sheet 21 and the exterior film 11 was evaluated for the sample of Example 1 (battery exterior body 1) thus obtained.

すなわち実施例１のサンプルにおいて、多孔質Ｎｉシート２１をＰＰ接着剤３１を介して外装フィルム１１に接着した後、エージングを行わずに、多孔質Ｎｉシート２１と外装フィルム１１との接合部を切り取り、幅３０ｍｍのサンプル切出片を得た。   That is, in the sample of Example 1, after bonding the porous Ni sheet 21 to the exterior film 11 via the PP adhesive 31, the joint between the porous Ni sheet 21 and the exterior film 11 was cut off without aging. A sample cut piece with a width of 30 mm was obtained.

この実施例１のサンプル切出片に対し、ＪＩＳ Ｋ６８５４−２に準拠して、多孔質Ｎｉシート２１と外装フィルム１１との間の層間接着強度を測定した。その結果を表２に示す。なお、得られた結果は、１５ｍｍ幅に換算した値（Ｎ／１５ｍｍ）である。   The interlayer adhesive strength between the porous Ni sheet 21 and the exterior film 11 was measured for the sample cut piece of Example 1 in accordance with JIS K6854-2. The results are shown in Table 2. In addition, the obtained result is a value (N / 15 mm) converted into a 15 mm width.

＜封止性評価＞
上記実施例１と同様に電池用外装体１を作製した。この場合、外装体１の内部に、電池本体（発電要素）である電解液が封入されるように、外装フィルム１１，１１の全周をヒートシールした。なお、外装体１の内部には、電解液として、１ＭのＬｉＰＦ６溶液（ＥＣ：ＤＥＣ＝１：１）を５ｍｌ注入した。 <Sealability evaluation>
A battery outer package 1 was produced in the same manner as in Example 1. In this case, the entire periphery of the exterior films 11 and 11 was heat-sealed so that the electrolyte solution which is the battery body (power generation element) was sealed inside the exterior body 1. In addition, 5 ml of 1M LiPF6 solution (EC: DEC = 1: 1) was injected into the exterior body 1 as an electrolytic solution.

こうして得られた実施例１のサンプルに対し、６０℃、湿度９０％Ｒｈの下で１週間保管した。この保管条件は、アレニウス加速に基づいて予測すると、２０℃で４ヶ月間保管した場合に相当する。そして保管後に、液漏れが発生したか否かを観察した。その結果を表２に示す。   The sample of Example 1 thus obtained was stored for 1 week at 60 ° C. and a humidity of 90% Rh. Predicting this storage condition based on Arrhenius acceleration corresponds to the case of storage at 20 ° C. for 4 months. Then, after storage, it was observed whether liquid leakage occurred. The results are shown in Table 2.

＜保管後接着性評価＞
上記封止性評価の試験を行った後（上記と同様の条件で保管した後）、実施例１のサンプルに対し、上記の初期接着性評価と同様に、サンプル切出片を切り出して、上記と同様に、多孔質Ｎｉシート２１と外装フィルム１１との間の層間接着強度を測定した。その結果を表２に示す。 <Evaluation of adhesion after storage>
After performing the test for evaluation of the sealing property (after storing under the same conditions as above), the sample cut piece was cut out for the sample of Example 1 in the same manner as in the initial adhesive evaluation. Similarly, the interlayer adhesive strength between the porous Ni sheet 21 and the exterior film 11 was measured. The results are shown in Table 2.

＜実施例２＞
実施例１と同様に、外装フィルム１１および多孔質Ｎｉシート２１とを接着した後、表１に示すように、ＰＰ接着剤３１のエージングを行って、外装体１を作製し、実施例２のサンプルとした。エージングの条件は、圧力０．１ＭＰａ〜０．３ＭＰａ、温度３０℃〜５０℃、期間２日〜９日である。 <Example 2>
As in Example 1, after the exterior film 11 and the porous Ni sheet 21 were bonded, as shown in Table 1, the PP adhesive 31 was aged to produce the exterior body 1, and A sample was used. The aging conditions are a pressure of 0.1 MPa to 0.3 MPa, a temperature of 30 ° C. to 50 ° C., and a period of 2 days to 9 days.

こうして得られた実施例２のサンプル（外装体１）に対し、上記実施例１と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表２に示す。   For the sample of Example 2 (exterior body 1) thus obtained, each evaluation of initial adhesiveness, sealing property and adhesiveness after storage was performed in the same manner as in Example 1. The results are shown in Table 2.

＜実施例３＞
変性ポリオレフィン系フィルム３２として、東亜合成株式会社製のホットメルト接着剤「アロンメルト（商標）ＰＰＥＴ２１０２」のブロックを２１ｃｍ×２９ｃｍの２枚のテフロン（登録商標）製の板（厚さ２ｍｍ）で挟み、１９０℃のホットプレスで１分間加熱溶融し、その後脱気し、３Ｍｐａで加圧、冷却して得られた厚さ１０５μｍの接着用フィルムを準備した。 <Example 3>
As a modified polyolefin film 32, a block of hot melt adhesive “Aronmelt (trademark) PPET2102” manufactured by Toa Gosei Co., Ltd. is sandwiched between two Teflon (registered trademark) plates (thickness 2 mm) of 21 cm × 29 cm, An adhesive film having a thickness of 105 μm obtained by heating and melting with a hot press at 190 ° C. for 1 minute, then degassing, pressurizing and cooling at 3 Mpa was prepared.

そして、安全弁２としての多孔質Ｎｉシート２１の両面（外装フィルム１１，１１との接着面）に、変性ポリオレフィン系フィルム３２を熱接着により溶着した（図５参照）。この熱溶着の条件は、温度を１５０℃〜２００℃、圧力を０．１ＭＰａ〜０．３ＭＰａ、時間を２〜５秒とした。   And the modified polyolefin-type film 32 was welded to both surfaces (adhesion surface with the exterior films 11 and 11) of the porous Ni sheet | seat 21 as a safety valve 2 by heat bonding (refer FIG. 5). The heat welding conditions were a temperature of 150 ° C. to 200 ° C., a pressure of 0.1 MPa to 0.3 MPa, and a time of 2 to 5 seconds.

こうして変性ポリオレフィン系フィルム３２を溶着した多孔質Ｎｉシート２１をその両側から２枚の外装フィルム１１，１１の周縁部（一辺）に挟み込まれるように、外装フィルム１１，１１を重ね合わせて配置する（図２参照）。   Thus, the exterior films 11 and 11 are arranged so as to overlap each other so that the porous Ni sheet 21 to which the modified polyolefin film 32 is welded is sandwiched between the peripheral edges (one side) of the two exterior films 11 and 11 from both sides ( (See FIG. 2).

さらにその状態で、重ね合わされた外装フィルム１１，１１の全周をヒートシールによって溶着して、外装体１を作製し、実施例３のサンプルとした。ヒートシールの条件は上記実施例１と同様である。   Further, in this state, the entire periphery of the overlaid exterior films 11, 11 was welded by heat sealing to produce the exterior body 1, which was used as a sample of Example 3. The heat sealing conditions are the same as in Example 1 above.

こうして得られた実施例３のサンプル（外装体１）に対し、上記実施例１と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表２に示す。   For the sample of Example 3 (exterior body 1) thus obtained, each evaluation of initial adhesiveness, sealing property and adhesiveness after storage was performed in the same manner as in Example 1. The results are shown in Table 2.

＜実施例４＞
表１に示すように、上記実施例１と同様の多孔質Ｎｉシート２１に対し、下地処理として、塗布型クロメート処理を行った。塗布型クロメート処理は、リン酸クロム（III ）２％とキトサン系樹脂２％を分散した原液と、純水と、ＩＰＡ（イソプロピルアルコール）とを１：２：０．５の組成で調合した液に、多孔質Ｎｉシート２１を浸漬した後、引き上げて、１５０℃〜２５０℃、１０秒〜１０分の条件で乾燥を行うものである。 <Example 4>
As shown in Table 1, coating-type chromate treatment was performed as a base treatment on the porous Ni sheet 21 similar to that in Example 1 described above. The coating type chromate treatment is a liquid prepared by mixing a stock solution in which 2% chromium (III) phosphate and 2% chitosan resin are dispersed, pure water, and IPA (isopropyl alcohol) in a composition of 1: 2: 0.5. Then, after the porous Ni sheet 21 is immersed, it is pulled up and dried under conditions of 150 ° C. to 250 ° C. for 10 seconds to 10 minutes.

この塗布型クロメート処理を行った多孔質Ｎｉシート２１を用いて、上記実施例２と同様にして、外装体１を作製し、実施例４のサンプルとした。   Using the porous Ni sheet 21 subjected to the coating-type chromate treatment, the exterior body 1 was produced in the same manner as in Example 2 above, and a sample of Example 4 was obtained.

こうして得られた実施例４のサンプルに対し、上記実施例１と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表２に示す。   For the sample of Example 4 obtained in this way, each evaluation of initial adhesiveness, sealing property and post-storage adhesiveness was performed in the same manner as in Example 1. The results are shown in Table 2.

＜実施例５＞
表１に示すように、上記と同様の多孔質Ｎｉシート２１に対し、下地処理として塗布型クロメート処理を行った。その後、そのシート２１に実施例３と同様に、変性ポリオレフィン系フィルム３２を溶着した後、外装フィルム１１，１１を溶着して、外装体１を作製し、実施例５のサンプルとした。 <Example 5>
As shown in Table 1, a coating type chromate treatment was performed as a base treatment on the porous Ni sheet 21 similar to the above. Then, after the modified polyolefin film 32 was welded to the sheet 21 in the same manner as in Example 3, the exterior films 11 and 11 were welded to produce the exterior body 1, which was used as the sample of Example 5.

こうして得られた実施例５のサンプルに対し、上記と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表２に示す。   The samples of Example 5 obtained in this way were each evaluated for initial adhesion, sealing properties and adhesion after storage in the same manner as described above. The results are shown in Table 2.

＜実施例６＞
安全弁２を構成する多孔質金属シート２１として、電析法を用いて作製した多孔質銅系合金（Ｃｕ系合金）シートを準備した。このシートは、厚さが０．０５ｍｍ、長さが３０ ｍｍ、幅が３０ｍｍである。さらにこのシートは、直径１μｍφの細孔が、１００個／ｃｍ２の密度で形成された多孔質のものである。 <Example 6>
As the porous metal sheet 21 constituting the safety valve 2, a porous copper-based alloy (Cu-based alloy) sheet prepared using an electrodeposition method was prepared. This sheet has a thickness of 0.05 mm and a length of 30. mm and a width of 30 mm. Further, this sheet is a porous sheet in which pores having a diameter of 1 μmφ are formed at a density of 100 / cm 2 .

この多孔質Ｃｕ系合金シートを使用した以外は、上記実施例５と同様にして、外装体１を作製し、実施例８のサンプルとした。   Except that this porous Cu-based alloy sheet was used, an exterior body 1 was produced in the same manner as in Example 5 above, and a sample of Example 8 was obtained.

こうして得られた実施例８のサンプルに対し、上記と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表２に示す。   The samples of Example 8 obtained in this manner were each evaluated for initial adhesiveness, sealing property, and post-storage adhesiveness in the same manner as described above. The results are shown in Table 2.

＜実施例７＞
安全弁２を構成する多孔質金属シート２１として、電析法を用いて作製した多孔質パラジウム系合金（Ｐｄ系合金）シートを準備した。このシートは、厚さが０．０５ｍｍ、長さが３０ｍｍ、幅が３０ｍｍである。さらにこのシートは、直径１μｍφの細孔が、１００個／ｃｍ２の密度で形成された多孔質のものである。 <Example 7>
As the porous metal sheet 21 constituting the safety valve 2, a porous palladium alloy (Pd alloy) sheet produced using an electrodeposition method was prepared. This sheet has a thickness of 0.05 mm, a length of 30 mm, and a width of 30 mm. Further, this sheet is a porous sheet in which pores having a diameter of 1 μmφ are formed at a density of 100 / cm 2 .

この多孔質Ｐｄ系合金シートを使用した以外は、上記実施例５と同様にして、外装体１を作製し、実施例９のサンプルとした。   Except that this porous Pd-based alloy sheet was used, the exterior body 1 was produced in the same manner as in Example 5 above, and used as a sample of Example 9.

こうして得られた実施例９のサンプルに対し、上記と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表２に示す。   The sample of Example 9 obtained in this manner was evaluated for initial adhesiveness, sealing property and post-storage adhesiveness in the same manner as described above. The results are shown in Table 2.

＜比較例１＞   <Comparative Example 1>

表３に示すように、多孔質Ｎｉシート２１に対し下地処理を行わず、さらにＰＰ接着剤や変性ポリオレフィン系フィルム等も用いずに、多孔質Ｎｉシート２１と外装フィルム１１とをヒートシールによって溶着して、比較例１のサンプル（外装体１）を作製した。換言すると、ＰＰ接着剤を使用しなかったこと以外は、実施例１と同様にして、比較例１のサンプルを得た。なおヒートシールの条件や、多孔質Ｎｉシート２１および外装フィルム１１の構成は、上記実施例１と同様である。   As shown in Table 3, the porous Ni sheet 21 and the exterior film 11 are welded by heat sealing without performing the base treatment on the porous Ni sheet 21 and without using a PP adhesive or a modified polyolefin film. Thus, a sample of Comparative Example 1 (exterior body 1) was produced. In other words, a sample of Comparative Example 1 was obtained in the same manner as Example 1 except that no PP adhesive was used. The conditions for heat sealing and the configurations of the porous Ni sheet 21 and the exterior film 11 are the same as those in Example 1.

こうして得られた比較例１のサンプルに対し、上記と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表４に示す。   The samples of Comparative Example 1 thus obtained were evaluated for initial adhesion, sealing properties and post-storage adhesive properties in the same manner as described above. The results are shown in Table 4.

＜比較例２＞
表３に示すように、多孔質Ｎｉシート２１に対し下地処理として塗布型クロメート処理を行った以外は、上記比較例１と同様にして、外装体１を作製し、比較例２のサンプルとした。 <Comparative example 2>
As shown in Table 3, the exterior body 1 was produced in the same manner as in the comparative example 1 except that the coating-type chromate treatment was performed as the base treatment for the porous Ni sheet 21 to obtain a sample of the comparative example 2. .

こうして得られた比較例２のサンプルに対し、上記と同様に、初期接着性、封止性および保管後接着性の各評価を行った。その結果を表４に示す。   For the sample of Comparative Example 2 obtained in this way, each evaluation of initial adhesiveness, sealing property and adhesiveness after storage was performed in the same manner as described above. The results are shown in Table 4.

＜評価結果＞
表２および表４から明らかなように、比較例１，２のサンプルに対し、実施例１〜７のサンプルは、良好な結果が得られた。 <Evaluation results>
As is clear from Tables 2 and 4, the samples of Examples 1 to 7 obtained good results with respect to the samples of Comparative Examples 1 and 2.

特に実施例４に示すように多孔質金属シート２１を、下地処理後に、エージングを伴うＰＰ接着剤によって外装フィルム１１に接着したサンプルや、実施例３，５，６，７に示すように多孔質金属シート２１を外装フィルム１１に変性ポリオレフィン系フィルムによって接着したサンプルは、多孔質金属シート２１を外装フィルム１１に接着した直後から十分な接着性（初期の層間強度）が得られ、さらに漏れの発生が一切なく封止性も良好であった。さらに保管後においても十分な接着性（保管後の層間強度）を得ることができ、長期間の使用によっても良好な接着性を維持できることを確認できた。   In particular, a porous metal sheet 21 as shown in Example 4 was bonded to the exterior film 11 with a PP adhesive with aging after the base treatment, or porous as shown in Examples 3, 5, 6, and 7. The sample in which the metal sheet 21 is adhered to the exterior film 11 with a modified polyolefin film can provide sufficient adhesion (initial interlayer strength) immediately after the porous metal sheet 21 is adhered to the exterior film 11, and further leakage occurs. No sealing at all. Furthermore, sufficient adhesiveness (interlaminar strength after storage) could be obtained even after storage, and it was confirmed that good adhesiveness could be maintained even after long-term use.

また実施例２に示すように下地処理を行わずに、エージングを伴うＰＰ接着剤によって接着したサンプルは、下地処理を行ったサンプル（実施例４，６等）よりも接着性や封止性が少し劣るものの、まずまずの評価を得ることができた。   In addition, as shown in Example 2, the sample bonded with the PP adhesive with aging without performing the ground treatment has more adhesiveness and sealability than the sample subjected to the ground treatment (Examples 4 and 6). Although it was a little inferior, we were able to get a reasonable evaluation.

さらに実施例１に示すように、下地処理もエージングも行わずに、ＰＰ接着剤によって接着したサンプルは、保管試験において、つまり長期間経過した後に液漏れの発生が認められたものの、初期の段階では、液漏れはなく、短期間であれば使用できるものと考えられる。   Further, as shown in Example 1, the sample adhered with the PP adhesive without performing the ground treatment or aging was observed in the storage test, that is, the occurrence of liquid leakage after a long time passed, but the initial stage. Then, it is thought that there is no liquid leak and it can be used for a short period of time.

また初期と保管後の層間強度を比較した場合、実施例１では１／３程度まで層間強度が低下していた。さらに実施例２，３では層間強度の低下が１／２程度に抑えられていた。また下地処理を行った実施例４〜７では、層間強度の低下が少なかった。   Moreover, when the interlayer strength after initial storage and storage was compared, in Example 1, the interlayer strength was reduced to about 1/3. Further, in Examples 2 and 3, the decrease in interlayer strength was suppressed to about ½. Moreover, in Examples 4-7 which performed the base treatment, there was little fall of interlayer intensity | strength.

これに対し、比較例１，２に示すように、ＰＰ接着剤や変性ポリオレフィン系フィルムを使用しないサンプルでは、下地処理を行っても行わなくとも、多孔質金属シートを外装フィルムに十分に接着することができず、接着性（層間接着強度）の評価や、封止性の評価を行うことができなかった。   On the other hand, as shown in Comparative Examples 1 and 2, in the sample not using the PP adhesive or the modified polyolefin film, the porous metal sheet is sufficiently adhered to the exterior film regardless of whether the base treatment is performed. It was not possible to evaluate adhesiveness (interlayer adhesive strength) or sealability.

この発明の電気化学素子用外装体は、ラミネート型の電池や、ラミネート型のキャパシタに適用可能である。   The outer package for an electrochemical element of the present invention can be applied to a laminate type battery or a laminate type capacitor.

１：外装体
１１：外装フィルム
２：安全弁
２１：多孔質金属シート
３：接着層
３１：接着剤
３２：接着用フィルム
４：リード端子
1: exterior body 11: exterior film 2: safety valve 21: porous metal sheet 3: adhesive layer 31: adhesive 32: adhesive film 4: lead terminal

Claims (12)

片面側のシーラント層が高分子化合物によって構成された２枚の外装フィルムが互いのシーラント層を対向させた状態で積層されるとともに、その積層状の外装フィルムの外周縁部が封止されるようにしたラミネート型の電気化学素子用外装体であって、
多孔質金属シートによって構成される内圧上昇防止用の安全弁の一端側が内部に配置されるとともに、他端側が外部に配置されるようにして、前記安全弁が積層状の２枚の前記外装フィルムにおける対応する外側縁部間に介在された状態で、前記安全弁が前記外装フィルムのシーラント層に、高分子化合物を含む接着層を介して固定されていることを特徴とする電気化学素子用外装体。 Two exterior films in which the sealant layer on one side is made of a polymer compound are laminated with the sealant layers facing each other, and the outer peripheral edge of the laminated exterior film is sealed. A laminate-type outer package for an electrochemical element,
One end side of the safety valve for preventing an increase in internal pressure composed of a porous metal sheet is arranged inside, and the other end side is arranged outside, so that the safety valve is compatible with the two laminated outer films. An exterior body for an electrochemical element, wherein the safety valve is fixed to the sealant layer of the exterior film via an adhesive layer containing a polymer compound while being interposed between outer edges. 前記接着層がポリオレフィン系高分子化合物を含んでいる請求項１に記載の電気化学素子用外装体。   The exterior body for an electrochemical element according to claim 1, wherein the adhesive layer contains a polyolefin polymer compound. 前記安全弁としての多孔質金属シートが、多孔質ニッケルシートである請求項１または２に記載の電気化学素子用外装体。   The exterior body for an electrochemical element according to claim 1 or 2, wherein the porous metal sheet as the safety valve is a porous nickel sheet. 前記安全弁は、表面が化成処理された多孔質金属シートである請求項１〜３のいずれか１項に記載の電気化学素子用外装体。   The exterior body for an electrochemical element according to any one of claims 1 to 3, wherein the safety valve is a porous metal sheet having a surface subjected to chemical conversion treatment. 請求項１〜４のいずれか１項に記載された外装体を備え、
前記外装体に電気化学素子本体が収容されていることを特徴とする電気化学素子。 The exterior body described in any one of claims 1 to 4 is provided,
An electrochemical element having an electrochemical element body accommodated in the outer package. 請求項１〜４のいずれか１項に記載された外装体を備え、
前記外装体の内部に電池本体である発電要素が収容されていることを特徴とする電池。 The exterior body described in any one of claims 1 to 4 is provided,
A battery characterized in that a power generation element as a battery main body is accommodated in the exterior body. 前記安全弁が、リード端子を兼用している請求項６に記載の電池。   The battery according to claim 6, wherein the safety valve also serves as a lead terminal. 片面側のシーラント層が高分子化合物によって構成された２枚の外装フィルムを互いのシーラント層を対向させた状態で積層するとともに、その積層状の外装フィルムの外周縁部を封止するようにしたラミネート型の電気化学素子用外装体の製造方法であって、
多孔質金属シートによって構成される内圧上昇防止用の安全弁を準備する準備工程と、
前記安全弁の一端側が前記外装体の内部に配置されるとともに、他端側が前記外装体の外部に配置されるようにして、前記安全弁を積層状の２枚の前記外装フィルムにおける対応する外側縁部間に介在した状態で、前記安全弁を前記外装フィルムのシーラント層に、高分子化合物を含む接着層を介して固定する接着工程とを含むことを特徴とする電気化学素子用外装体の製造方法。 Two exterior films each having a sealant layer on one side made of a polymer compound are laminated with the sealant layers facing each other, and the outer peripheral edge of the laminated exterior film is sealed. A method for producing a laminate-type outer package for an electrochemical element,
A preparation step of preparing a safety valve for preventing an increase in internal pressure constituted by a porous metal sheet;
One end side of the safety valve is disposed inside the exterior body, and the other end side is disposed outside the exterior body, so that the safety valve is disposed on the corresponding outer edge portion of the two laminated exterior films. A method for producing an exterior body for an electrochemical element, comprising: an adhesion step of fixing the safety valve to a sealant layer of the exterior film through an adhesive layer containing a polymer compound in a state of being interposed therebetween. 前記接着工程を行う前に、前記安全弁としての多孔質金属シートの表面に化成処理を行うようにした請求項８に記載の電気化学素子用外装体の製造方法。   The method for producing an exterior body for an electrochemical element according to claim 8, wherein a chemical conversion treatment is performed on the surface of the porous metal sheet as the safety valve before the adhesion step. 前記接着層は、前記安全弁および前記外装フィルム間に塗布され、かつポリオレフィン系高分子化合物を含む接着剤によって構成されている請求項８または９に記載の電気化学素子用外装体の製造方法。   The method for producing an exterior body for an electrochemical element according to claim 8 or 9, wherein the adhesive layer is applied between the safety valve and the exterior film and is composed of an adhesive containing a polyolefin polymer compound. 前記接着工程は、前記接着剤をエージングするエージング工程を含んでいる請求項１０に記載の電気化学素子用外装体の製造方法。   The method for producing an exterior body for an electrochemical element according to claim 10, wherein the adhesion step includes an aging step of aging the adhesive. 前記接着層は、前記安全弁および前記外装フィルム間に配置され、かつポリオレフィン系高分子化合物を含む接着用フィルムによって構成されている請求項８または９に記載の電気化学素子用外装体の製造方法。
The method for producing an exterior body for an electrochemical element according to claim 8 or 9, wherein the adhesive layer is disposed between the safety valve and the exterior film and is composed of an adhesive film containing a polyolefin polymer compound.
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