JP2020021727A - Exterior material for power storage device and manufacturing method thereof - Google Patents

Exterior material for power storage device and manufacturing method thereof Download PDF

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JP2020021727A
JP2020021727A JP2019116241A JP2019116241A JP2020021727A JP 2020021727 A JP2020021727 A JP 2020021727A JP 2019116241 A JP2019116241 A JP 2019116241A JP 2019116241 A JP2019116241 A JP 2019116241A JP 2020021727 A JP2020021727 A JP 2020021727A
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exterior material
outermost layer
storage device
layer
adhesive
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JP7234047B2 (en
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大介 中嶋
Daisuke Nakajima
大介 中嶋
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Resonac Packaging Corp
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Showa Denko Packaging Co Ltd
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    • B32B27/00—Layered products comprising a layer of synthetic resin
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    • H—ELECTRICITY
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    • 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
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    • B32B3/00—Layered products comprising a layer with external or internal discontinuities or unevennesses, or a layer of non-planar shape; Layered products comprising a layer having particular features of form
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    • B32B37/10—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the pressing technique, e.g. using action of vacuum or fluid pressure
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    • B32B37/12—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by using adhesives
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    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/117—Inorganic material
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    • H01M50/10—Primary casings; Jackets or wrappings
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    • H01M50/121—Organic material
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    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
    • H01M50/1245—Primary casings; Jackets or wrappings characterised by the material having a layered structure characterised by the external coating on the casing
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    • 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
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Abstract

To provide an exterior material for a power storage device, having a surface high in slipperiness and also high in adhesion with a pressure-sensitive adhesive tape, a manufacturing method thereof, and a power storage device.SOLUTION: An exterior material 1 includes an outermost layer 2, a sealant layer 4, and a barrier layer 3 placed between both layers 2, 4, in a laminated form. The outermost layer 2 is made from at least one selected from the group consisting of a polyamide film, a polyester film, and a polyolefin film. In the surface properties of a surface 2a of the outermost layer 2, the arithmetic average height Sa is in the range of 0.03-0.20 μm. When a projection having a cross section in a position at +0.1 μm height from a reference plane of Sa of 7,500 μmor more is defined as a mountain, the number of mountains is in the range of 5-30 per 1 mm.SELECTED DRAWING: Figure 1

Description

本発明は、リチウムイオン電池等の蓄電デバイス用外装材、その製造方法及び蓄電デバイスに関する。   The present invention relates to an exterior material for a power storage device such as a lithium ion battery, a method for manufacturing the same, and a power storage device.

例えばリチウムイオン電池用の外装材として、最外層とバリア層とシーラント層とを積層状に備えたラミネートフィルムから形成されたものがある。この外装材を用いてリチウムイオン電池を製造する場合、外装材は袋状に形成されたり成形金型を用いた成形加工により容器状に形成され、その内部にリチウムイオン電池内容物（電池セル、電解液等）が収容されて熱封止される。   For example, as an exterior material for a lithium ion battery, there is an exterior material formed from a laminate film including an outermost layer, a barrier layer, and a sealant layer in a laminated state. When a lithium ion battery is manufactured using this exterior material, the exterior material is formed in a bag shape or a container shape by molding using a molding die, and the lithium ion battery contents (battery cells, (Electrolyte solution etc.) is accommodated and heat sealed.

この外装材が用いられたリチウムイオン電池は、これを使用する際には所定の回路に組み込まれたり所定の取付け場所に取り付けられる。その際に、リチウムイオン電池の位置がずれないようにするため、一般的にリチウムイオン電池は絶縁性粘着テープで固定される。   When using the lithium ion battery using this exterior material, the lithium ion battery is incorporated into a predetermined circuit or mounted at a predetermined mounting location when the lithium ion battery is used. At that time, in order to prevent the position of the lithium ion battery from shifting, the lithium ion battery is generally fixed with an insulating adhesive tape.

ところで、外装材の成形性及び滑り性を良くするためやブロッキング対策のため、従来の外装材の表面には滑剤やアンチブロッキング剤が存在していることがある（例えば特許文献１参照）。   Incidentally, a lubricant or an anti-blocking agent may be present on the surface of a conventional exterior material in order to improve the moldability and slipperiness of the exterior material and to prevent blocking (for example, see Patent Document 1).

特許第５６５２１７８号公報Japanese Patent No. 5652178

上述のように外装材の表面に滑剤やアンチブロッキング剤が存在している場合、外装体の表面の粘着テープとの密着性が低下し粘着テープでリチウムイオン電池を位置固定する際に粘着テープが外装材の表面から剥がれることがあった。   As described above, when a lubricant or an anti-blocking agent is present on the surface of the exterior material, the adhesiveness of the surface of the exterior body with the adhesive tape is reduced, and the adhesive tape is used to fix the position of the lithium ion battery with the adhesive tape. In some cases, it was peeled off from the surface of the exterior material.

本発明は、上述した技術背景に鑑みてなされたもので、その目的は、滑り性が高く且つ粘着テープとの密着性も高い表面を有する蓄電デバイス用外装材を提供することにある。   The present invention has been made in view of the above technical background, and an object of the present invention is to provide an exterior material for a power storage device having a surface having high slipperiness and high adhesion to an adhesive tape.

本発明者は、蓄電デバイス用外装材について鋭意研究調査したところ、外装材の最外層が所定のフィルムからなり、更に、最外層の表面の表面性状において、算出平均高さＳａが所定の範囲であり且つ当該表面に存在する多数の凸部のうち所定の大きさの凸部の１ｍｍ２当たりの数が所定の範囲であるものであれば、上記目的を達成しうることが判明し、本発明を完成させた。 The present inventor has conducted intensive research and investigation on the exterior material for an electric storage device, and found that the outermost layer of the exterior material is formed of a predetermined film, and further, in the surface properties of the surface of the outermost layer, the calculated average height Sa is within a predetermined range. It has been found that the above object can be achieved if the number of projections having a predetermined size per 1 mm 2 among a large number of projections present on the surface is within a predetermined range. Was completed.

すなわち、本発明は以下の手段を提供する。   That is, the present invention provides the following means.

１） 最外層と、シーラント層と、前記両層間に配置されたバリア層とを積層状に備えた蓄電デバイス用外装材であって、
前記最外層は、ポリアミドフィルム、ポリエステルフィルム及びポリオレフィンフィルムからなる群より選択される少なくとも一つからなり、
前記最外層の表面の表面性状において、
算術平均高さＳａが０．０３〜０．２０μｍの範囲であり、
前記Ｓａの基準面から＋０．１μｍの高さ位置の断面積が７５００μｍ２以上である凸部を山と定義するとき、山の数が１ｍｍ２当たり５〜３０個の範囲である蓄電デバイス用外装材。 1) An exterior material for a power storage device, comprising an outermost layer, a sealant layer, and a barrier layer disposed between the two layers in a laminated state,
The outermost layer is made of at least one selected from the group consisting of a polyamide film, a polyester film, and a polyolefin film,
In the surface properties of the surface of the outermost layer,
Arithmetic mean height Sa is in the range of 0.03 to 0.20 μm,
When a convex portion having a sectional area of 7,500 μm 2 or more at a height position of +0.1 μm from the reference surface of Sa is defined as a mountain, the number of the mountain ranges from 5 to 30 per mm 2. Wood.

２） 前記山における前記基準面から＋０．１μｍの高さ位置の断面の重心位置を前記山の重心位置と定義するとき、１ｍｍ２に存在する互いに近接する前記山の重心位置間の距離が全て１５０〜７００μｍの範囲である前項１記載の蓄電デバイス用外装材。 2) When the position of the center of gravity of the cross section at a height of +0.1 μm from the reference plane in the peak is defined as the position of the center of gravity of the peak, the distance between the positions of the centers of gravity of 1 mm 2 that are close to each other is all Item 2. The exterior material for an electric storage device according to item 1, which has a range of 150 to 700 µm.

３） 前記最外層と前記バリア層が、これら両層間に配置された接着剤層で接着されており、
前記接着剤層の前記最外層側に向いた面が凹凸状に形成されている前項１又は２記載の蓄電デバイス用外装材。 3) the outermost layer and the barrier layer are adhered by an adhesive layer disposed between the two layers;
Item 3. The exterior material for an electric storage device according to Item 1 or 2, wherein a surface of the adhesive layer facing the outermost layer is formed in an uneven shape.

４） 前記接着剤層の前記最外層側の向いた面に形成された凹凸の箇所と、前記最外層の表面に形成された凹凸の箇所とが略一致している前項３記載の蓄電デバイス用外装材。   4) The power storage device according to the above item 3, wherein the irregularities formed on the surface of the adhesive layer facing the outermost layer substantially coincide with the irregularities formed on the surface of the outermost layer. Exterior materials.

５） 前項３又は４記載の蓄電デバイス用外装材の製造方法であって、
外装材における最外層とバリア層の間に配置される接着剤層の接着剤をグラビア塗工法によりバリア層上に塗工する蓄電デバイス用外装材の製造方法。 5) A method for manufacturing an exterior material for an electricity storage device according to the item 3 or 4,
A method for manufacturing an exterior material for an electric storage device, wherein an adhesive of an adhesive layer disposed between an outermost layer and a barrier layer in the exterior material is coated on the barrier layer by a gravure coating method.

６） 前項１〜４のいずれかに記載の蓄電デバイス用外装材で蓄電デバイス内容物が包装された蓄電デバイス。   6) A power storage device in which the power storage device content is packaged with the power storage device exterior material according to any one of the above items 1 to 4.

本発明は以下の効果を奏する。   The present invention has the following effects.

前項１では、外装材の最外層がポリアミドフィルム、ポリエステルフィルム及びポリオレフィンフィルムからなる群から選択される少なくとも一つからなり、最外層の表面の算術平均高さＳａが０．０３〜０．２０μｍの範囲であり、山の数が１ｍｍ２当たり５〜３０個の範囲であることから、最外層の表面である外装材の表面は凹凸部が形成されることで高い滑り性を有するとともに、表面積が拡がることで粘着テープとの接着面積が大きくなり、したがって外装材の表面の粘着テープとの密着性についても高い密着性を有する。 In the preceding item 1, the outermost layer of the exterior material is made of at least one selected from the group consisting of a polyamide film, a polyester film, and a polyolefin film, and the arithmetic average height Sa of the surface of the outermost layer is 0.03 to 0.20 μm. Since the number of peaks is in the range of 5 to 30 per 1 mm 2 , the surface of the exterior material, which is the surface of the outermost layer, has high slipperiness due to the formation of the unevenness, and the surface area is By spreading, the adhesive area with the adhesive tape is increased, and therefore, the adhesiveness of the surface of the exterior material with the adhesive tape is also high.

前項２〜４では、外装材の表面の滑り性を確実に高めることができるし、外装材の表面の粘着テープとの密着性についても確実に高めることができる。   In the above items 2 to 4, the slipperiness of the surface of the exterior material can be surely enhanced, and the adhesion of the surface of the exterior material to the adhesive tape can be surely enhanced.

前項５では、接着剤層の接着剤をグラビア塗工法によりバリア層上に塗工することにより、本発明に係る蓄電デバイス用外装材の最外層の表面について所定の表面性状に確実に実現することができる。   In the above item 5, in which the surface of the outermost layer of the exterior material for an electric storage device according to the present invention is reliably realized to have a predetermined surface property by coating the adhesive of the adhesive layer on the barrier layer by a gravure coating method. Can be.

前項６では、粘着テープで強固に位置固定できる蓄電デバイスを提供し得る。   In the above item 6, it is possible to provide a power storage device that can be firmly fixed in position with an adhesive tape.

図１は、本発明の一実施形態に係る蓄電デバイス用外装材の概略断面図である。FIG. 1 is a schematic cross-sectional view of an exterior material for a power storage device according to one embodiment of the present invention. 図２は、外装材の最外層の表面の表面凹凸像におけるＳａの基準面から＋０．１μｍの高さの等高線を示す概略図である。FIG. 2 is a schematic diagram showing contour lines having a height of +0.1 μm from the reference surface of Sa in the surface unevenness image of the surface of the outermost layer of the exterior material. 図３は、図２に示した概略図において互いに近接する山の重心位置間の距離を説明する図である。FIG. 3 is a diagram for explaining the distance between the centers of gravity of the mountains that are close to each other in the schematic diagram shown in FIG.

本発明の一実施形態について図面を参照して以下に説明する。   An embodiment of the present invention will be described below with reference to the drawings.

図１に示すように、本発明の一実施形態に係る蓄電デバイス用外装材１は、蓄電デバイスとして例えばリチウムイオン電池用のものであり、従来の外装材と同じように袋状に形成されたり成形金型を用いた成形加工により容器状に形成され、その内部に蓄電デバイス内容物としてのリチウムイオン電池内容物（電池セル、電解液等）が収容されて熱封止されるものである。   As shown in FIG. 1, an exterior material 1 for an electricity storage device according to an embodiment of the present invention is used for a lithium ion battery, for example, as an electricity storage device, and may be formed in a bag shape like a conventional exterior material. It is formed in a container shape by molding using a molding die, and contains therein lithium ion battery contents (battery cells, electrolyte solution, etc.) as the contents of the electric storage device and is heat-sealed.

図１に示すように、外装材１は、最外層２と、最内層としてのシーラント層４と、両層２、４間に配置されたバリア層３とを積層状に備えたものであって、これらの層２〜４が接着一体化されたラミネートフィルムからなる。   As shown in FIG. 1, the exterior material 1 includes an outermost layer 2, a sealant layer 4 as an innermost layer, and a barrier layer 3 disposed between the two layers 2 and 4 in a stacked state. And a laminated film in which these layers 2 to 4 are bonded and integrated.

外装材１の構成について詳述すると、最外層２とバリア層３は両層２、３間に配置された外側接着剤層５により互いに接着されており、バリア層３とシーラント層４は両層３、４間に配置された内側接着剤層６により互いに接着されている。   The configuration of the exterior material 1 will be described in detail. The outermost layer 2 and the barrier layer 3 are adhered to each other by an outer adhesive layer 5 disposed between the two layers 2 and 3, and the barrier layer 3 and the sealant layer 4 are connected to each other. They are adhered to each other by an inner adhesive layer 6 disposed between 3, 4.

最外層２は、外装材１の基材層とも呼ばれており、ポリアミドフィルム、ポリエステルフィルム及びポリオレフィンフォルムからなる群より選択される少なくとも一つからなる。   The outermost layer 2 is also called a base layer of the exterior material 1 and is made of at least one selected from the group consisting of a polyamide film, a polyester film, and a polyolefin form.

ポリアミドフィルムとしては、二軸延伸ナイロンフィルム（例：二軸延伸６ナイロンフィルム）などが好適に用いられる。   As the polyamide film, a biaxially stretched nylon film (eg, a biaxially stretched 6 nylon film) or the like is suitably used.

ポリエステルフィルムとしては、ポリエチレンテレフタレートフィルム（ＰＥＴフィルム）、ポリエチレンナフタレートフィルム（ＰＥＮフィルム）、ポリブチレンテレフタレートフィルム（ＰＢＴフィルム）などが用いられる。   As the polyester film, a polyethylene terephthalate film (PET film), a polyethylene naphthalate film (PEN film), a polybutylene terephthalate film (PBT film), or the like is used.

ポリオレフィンフィルムとしては、二軸延伸ポリプロピレンフィルム（ＯＰＰフィルム）等のポリプロピレンフィルム、ポリエチレンフィルムなどが用いられる。   As the polyolefin film, a polypropylene film such as a biaxially oriented polypropylene film (OPP film), a polyethylene film, or the like is used.

最外層２の厚さは限定されるものではなく、通常、１０〜５０μｍの範囲である。   The thickness of the outermost layer 2 is not limited, and is usually in the range of 10 to 50 μm.

バリア層３は、通常、金属箔からなる。金属箔としては、アルミニウム（その合金を含む）箔、銅（その合金を含む）箔、ニッケル（その合金を含む）箔、チタン（その合金を含む）箔、ステンレス鋼箔などが用いられ、特にアルミニウム箔が好適に用いられる。また、金属箔はその片面又は両面に化成皮膜などの腐食防止処理層（図示せず）が形成されたものであっても良い。   The barrier layer 3 is usually made of a metal foil. As the metal foil, aluminum (including its alloy) foil, copper (including its alloy) foil, nickel (including its alloy) foil, titanium (including its alloy) foil, stainless steel foil, and the like are used. Aluminum foil is preferably used. Further, the metal foil may have a corrosion prevention treatment layer (not shown) such as a chemical conversion film formed on one or both surfaces thereof.

バリア層３の厚さは限定されるものではなく、通常、５〜５０μｍの範囲であり、特に１０〜４０μｍの範囲であることが望ましい。   The thickness of the barrier layer 3 is not limited, and is usually in the range of 5 to 50 μm, and particularly preferably in the range of 10 to 40 μm.

シーラント層４は、ポリプロピレンフィルム、ポリエチレンフィルムなどからなる。ポリプロピレンフィルムとしては無延伸ポリプロピレンフィルム（ＣＰＰフィルム）などが用いられる。ポリエチレンフィルムとしては直鎖状低密度ポリエチレンフィルム（ＬＬＤＰＥフィルム）などが用いられる。   The sealant layer 4 is made of a polypropylene film, a polyethylene film, or the like. As the polypropylene film, a non-oriented polypropylene film (CPP film) or the like is used. As the polyethylene film, a linear low density polyethylene film (LLDPE film) or the like is used.

外側接着剤層５の接着剤は、最外層２とバリア層３を接着可能なものであれば限定されるものではなく、当該接着剤として特に二液硬化型ウレタン系接着剤が用いられることが望ましい。その理由は、二液硬化型ウレタン系接着剤は高い耐水性、高い耐候性などを有するからである。   The adhesive of the outer adhesive layer 5 is not limited as long as the outermost layer 2 and the barrier layer 3 can be bonded, and a two-part curable urethane-based adhesive may be used as the adhesive. desirable. The reason is that the two-part curable urethane-based adhesive has high water resistance, high weather resistance, and the like.

外側接着剤層５は、例えば、最外層２と接着される層であるバリア層３（詳述するとバリア層３の最外層２側に向く面）上に外側接着剤層５の接着剤を所定の塗工方法によって塗工することにより形成される。   The outer adhesive layer 5 is formed, for example, by applying an adhesive of the outer adhesive layer 5 on a barrier layer 3 (specifically, a surface of the barrier layer 3 facing the outermost layer 2) which is a layer bonded to the outermost layer 2. It is formed by coating by the coating method of (1).

外側接着剤層５の接着剤の塗工方法（即ち外側接着剤層５の形成方法）としては、グラビア塗工法、スプレー塗工法、ドクターブレード塗工法などが用いられ、特にグラビア塗工法を用いることが望ましい。その理由は次のとおりである。   As a method of applying the adhesive of the outer adhesive layer 5 (that is, a method of forming the outer adhesive layer 5), a gravure coating method, a spray coating method, a doctor blade coating method, or the like is used, and in particular, a gravure coating method is used. Is desirable. The reason is as follows.

すなわち、グラビア塗工法では、通常、表面に所定のメッシュ数及び深度の彫刻が施されたグラビアロールを用いてパターン塗工が行われる。したがって、グラビア塗工法によって接着剤をバリア層３上に塗工することにより、図１に示すように外側接着剤層５の最外層２側に向く面５ａは規則的に整列した微細な凹凸状に形成される。そして、この面５ａに最外層２が接着されると、この面５ａに形成された微細な凹凸形状が最外層２の表面２ａに反映される。その結果、この面５ａに形成された凹凸の箇所と最外層の表面２ａに形成される凹凸の箇所とが一致する。これにより、最外層２の表面２ａである外装材１の表面について所定の表面性状を確実に実現することができる。   That is, in the gravure coating method, usually, pattern coating is performed using a gravure roll having a surface engraved with a predetermined mesh number and depth. Therefore, by coating the adhesive on the barrier layer 3 by the gravure coating method, the surface 5a of the outer adhesive layer 5 facing the outermost layer 2 side is formed into regularly aligned fine irregularities as shown in FIG. Formed. Then, when the outermost layer 2 is bonded to the surface 5a, the fine irregularities formed on the surface 5a are reflected on the surface 2a of the outermost layer 2. As a result, the irregularities formed on the surface 5a and the irregularities formed on the outermost surface 2a coincide. Thereby, a predetermined surface property can be reliably realized on the surface of the exterior material 1, which is the surface 2a of the outermost layer 2.

内側接着剤層６の接着剤は、バリア層３とシーラント層４を接着可能なものであれば限定されるものではなく、当該接着剤として熱硬化型酸変性ポリプロピレン接着剤などが用いられる。   The adhesive of the inner adhesive layer 6 is not limited as long as it can bond the barrier layer 3 and the sealant layer 4, and a thermosetting acid-modified polypropylene adhesive or the like is used as the adhesive.

内側接着剤層６の接着剤の塗工方法（即ち内側接着剤層６の形成方法）については限定されるものではなく、接着剤の塗工方法として、上述したグラビア塗工法、スプレー塗工法、ドクターブレード塗工法などが用いられる。   The method of applying the adhesive of the inner adhesive layer 6 (that is, the method of forming the inner adhesive layer 6) is not limited, and the gravure coating method, spray coating method, A doctor blade coating method or the like is used.

本実施形態では、外装材１は、最外層２の表面２ａの表面性状において、算術平均高さＳａが０．０３〜０．２０μｍの範囲であるという第１要件と、Ｓａの基準面から＋０．１μｍの高さ位置の断面積が７５００μｍ２以上である凸部を山８（図２参照）と定義するとき、山８の数が１ｍｍ２当たり５〜３０個の範囲であるという第２要件とを満足する必要がある。なお、表面性状はＩＳＯ ２５１７８に準拠して測定される。 In the present embodiment, in the surface properties of the surface 2a of the outermost layer 2, the exterior material 1 has a first requirement that the arithmetic mean height Sa is in a range of 0.03 to 0.20 μm, and +0 from the reference surface of Sa. When a convex portion having a sectional area of 7500 μm 2 or more at a height position of 1 μm is defined as a peak 8 (see FIG. 2), the second requirement that the number of peaks 8 be 5 to 30 per 1 mm 2 And must be satisfied. The surface properties are measured according to ISO 25178.

第１及び第２要件を満足することにより、最外層２の表面２ａは高い滑り性を有するとともに、粘着テープとの接触面積が大きいため最外層２の表面２ａの粘着テープとの密着性についても高い密着性を有する。したがって、リチウムイオン電池を粘着テープで強固に位置固定することができる。   By satisfying the first and second requirements, the surface 2a of the outermost layer 2 has high slipperiness and has a large contact area with the pressure-sensitive adhesive tape. Has high adhesion. Therefore, the position of the lithium ion battery can be firmly fixed by the adhesive tape.

さらに、山８におけるＳａの基準面から＋０．１μｍの高さ位置の断面の重心位置（図心位置）を山８の重心位置Ｃ（図３参照）と定義するとき、外装材１は、１ｍｍ２に存在する互いに近接する山８の重心位置Ｃ間の距離が全て１５０〜７００μｍの範囲であるという第３要件を満足していることが望ましい。 Further, when defining the center of gravity (center of gravity) of the cross section of the mountain 8 at a height of +0.1 μm from the reference plane of Sa as the center of gravity C of the mountain 8 (see FIG. 3), the exterior material 1 is 1 mm it is desirable that the distance between the gravity center position C of the mountain 8 close to each other exist in 2 satisfies the third requirement that all ranges 150～700Myuemu.

第３要件を満足することにより、最外層２の表面２ａの滑り性を確実に高めることができるし、粘着テープとの接触面積を確実に大きくすることができるため、最外層２の表面２ａの粘着テープとの密着性についても確実に高めることができる。したがって、リチウムイオン電池を粘着テープで確実に強固に位置固定することができる。   By satisfying the third requirement, the slipperiness of the surface 2a of the outermost layer 2 can be surely increased, and the contact area with the adhesive tape can be surely increased. Adhesion with the adhesive tape can also be reliably increased. Therefore, the position of the lithium ion battery can be securely and firmly fixed with the adhesive tape.

ここで、第２及び第３要件について図２及び３を参照して説明すると、次のとおりである。   Here, the second and third requirements will be described with reference to FIGS. 2 and 3.

図２は、最外層２の表面２ａの表面凹凸像におけるＳａの基準面から＋０．１μｍの高さの等高線を示す概略図である。   FIG. 2 is a schematic diagram showing contour lines having a height of +0.1 μm from the reference surface of Sa in the surface unevenness image of the surface 2 a of the outermost layer 2.

第２要件において、Ｓａの基準面とは最外層２の表面２ａの測定領域の平均高さの面である。基準面から＋０．１μｍの高さの断面積とは基準面から＋０．１μｍの高さの等高線で包囲された面積である。そして、この面積が７５００μｍ２以上である凸部が山８と定義されている。また、山８の数を規定する「１ｍｍ２」とは、測定領域における互いに直交するＸ方向１ｍｍ及びＹ方向１ｍｍの正方形領域Ｓである。図２の場合、山８の数は８個である。 In the second requirement, the reference surface of Sa is a surface having an average height of the measurement region on the surface 2a of the outermost layer 2. The cross-sectional area at a height of +0.1 μm from the reference plane is an area surrounded by contour lines at a height of +0.1 μm from the reference plane. A convex portion having an area of 7500 μm 2 or more is defined as a peak 8. Further, “1 mm 2 ” that defines the number of the peaks 8 is a square area S of 1 mm in the X direction and 1 mm in the Y direction orthogonal to each other in the measurement area. In the case of FIG. 2, the number of the peaks 8 is eight.

なお、１ｍｍ２の正方形領域Ｓの外周境界線１０に跨がって存在する山については、重心位置Ｃが外周境界線１０の内側又は外周境界線１０上に存在している山を１ｍｍ２に存在する山の数にカウントし、重心位置Ｃが外周境界線１０の外側に存在している山は１ｍｍ２に存在する山の数にカウントしない。 In addition, as for the mountain existing over the outer peripheral boundary line 10 of the square area S of 1 mm 2 , the mountain whose center of gravity position C exists inside the outer peripheral boundary line 10 or on the outer peripheral boundary line 10 is set to 1 mm 2 . The number of peaks existing is counted, and the peak whose center of gravity position C exists outside the outer peripheral boundary line 10 is not counted as the number of peaks existing in 1 mm 2 .

図３は、図２に示した概略図において互いに近接する山８の重心位置Ｃ間の距離を説明する図である。   FIG. 3 is a diagram illustrating the distance between the centers of gravity C of the peaks 8 that are close to each other in the schematic diagram illustrated in FIG.

同図に示した山８の分布状態の場合において、第３要件を満足するとは、測定領域における１ｍｍ２の正方形領域Ｓに存在する全ての山８（即ち８個の山８）について互いに近接する山８の重心位置Ｃ間の距離ｄ１〜ｄ１１が全て１５０〜７００μｍの範囲であることを意味する。 In the case of the distribution state of the peaks 8 shown in the figure, satisfying the third requirement means that all the peaks 8 (that is, eight peaks 8) existing in the 1 mm 2 square area S in the measurement area are close to each other. This means that the distances d1 to d11 between the centers of gravity C of the peaks 8 are all in the range of 150 to 700 μm.

以上で本発明の実施形態について説明したが、本発明は上記実施形態に限定されるものではなく、本発明の要旨を逸脱しない範囲で様々に変更可能である。   Although the embodiment of the present invention has been described above, the present invention is not limited to the above embodiment, and can be variously modified without departing from the gist of the present invention.

また、本発明に係る蓄電デバイス用外装材は、リチウムイオン電池用のものであることに限定されるものではなく、その他の蓄電デバイス用のものであっても良く、例えばリチウムイオンキャパシタ用のものであっても良いし電気二重層キャパシタ用のものであっても良い。   Further, the exterior material for a power storage device according to the present invention is not limited to a material for a lithium ion battery, and may be for other power storage devices, for example, a material for a lithium ion capacitor. Or for an electric double layer capacitor.

本発明の具体的な実施例及び比較例を以下に示す。ただし、本発明は下記実施例に限定されるものではない。   Specific examples and comparative examples of the present invention are shown below. However, the present invention is not limited to the following examples.

＜実施例１＞
最外層２を形成するフィルムとしての二軸延伸６ナイロンフィルム（厚さ２５μｍ）、バリア層３を形成する金属箔としてのアルミニウム箔（厚さ３５μｍ）、及び、シーラント層４を形成するフィルムとしての無延伸ポリプロピレンフィルム（厚さ３０μｍ）を準備した。 <Example 1>
A biaxially stretched nylon film (thickness: 25 μm) as a film forming the outermost layer 2, an aluminum foil (thickness: 35 μm) as a metal foil forming the barrier layer 3, and a film forming the sealant layer 4 An unstretched polypropylene film (thickness 30 μm) was prepared.

アルミニウム箔（バリア層３）の両面にそれぞれ化成皮膜を形成した。その形成方法は次のとおりである。すなわち、リン酸、ポリアクリル酸（アクリル系樹脂）、クロム（III）塩化合物、水及びアルコールを含む化成処理液をアルミニウム箔の両面にそれぞれ塗布し１８０℃で乾燥し、これにより化成皮膜を形成した。化成皮膜のクロムの付着量は１０ｍｇ／ｍ２であった。 Chemical conversion coatings were formed on both surfaces of the aluminum foil (barrier layer 3). The forming method is as follows. That is, a chemical conversion treatment solution containing phosphoric acid, polyacrylic acid (acrylic resin), a chromium (III) salt compound, water and alcohol is applied to both sides of an aluminum foil and dried at 180 ° C., thereby forming a chemical conversion film. did. The amount of chromium deposited on the chemical conversion film was 10 mg / m 2 .

次いで、アルミニウム箔の一方の片面に外側接着剤層５の接着剤としての二液硬化型ウレタン系接着剤をグラビア塗工法により塗工し乾燥した。これにより、アルミニウム箔の一方の片面に外側接着剤層５を形成した。接着剤の乾燥後の塗工量は３．５ｇ／ｍ２であった。 Next, a two-component curable urethane-based adhesive as an adhesive for the outer adhesive layer 5 was applied to one side of the aluminum foil by a gravure coating method and dried. Thus, the outer adhesive layer 5 was formed on one side of the aluminum foil. The coating amount after drying of the adhesive was 3.5 g / m 2 .

上述のグラビア塗工法では、表面にメッシュ数８５及び深度１２０μｍの格子型の彫刻が施されたグラビアロールを用いた。   In the gravure coating method described above, a gravure roll having a lattice type engraving with a mesh number of 85 and a depth of 120 μm on the surface was used.

そして、アルミニウム箔と二軸延伸６ナイロンフィルム（最外層２）を外側接着剤層５で仮接着した。   Then, the aluminum foil and the biaxially stretched 6 nylon film (outermost layer 2) were temporarily bonded with the outer adhesive layer 5.

次いで、アルミニウム箔の他方の片面に内側接着剤層６の接着剤としての熱硬化型酸変性ポリプロピレン接着剤を塗布し乾燥した。これにより、アルミニウム箔の他方の片面に内側接着剤層６を形成した。接着剤の乾燥後の塗布量は２．５ｇ／ｍ２であった。 Next, a thermosetting acid-modified polypropylene adhesive as an adhesive for the inner adhesive layer 6 was applied to the other surface of the aluminum foil and dried. Thereby, the inner adhesive layer 6 was formed on the other surface of the aluminum foil. The coated amount of the adhesive after drying was 2.5 g / m 2 .

そして、アルミニウム箔と無延伸ポリプロピレンフィルム（シーラント層４）を内側接着剤層６で仮接着した。これにより、二軸延伸６ナイロンフィルムからなる最外層２とアルミニウム箔からなるバリア層３と無延伸ポリプロピレンフィルムからなるシーラント層４とを積層状に備えた外装材素材を得た。   Then, the aluminum foil and the unstretched polypropylene film (sealant layer 4) were temporarily bonded with the inner adhesive layer 6. As a result, a packaging material was obtained in which the outermost layer 2 composed of a biaxially oriented 6 nylon film, the barrier layer 3 composed of an aluminum foil, and the sealant layer 4 composed of a non-oriented polypropylene film were laminated.

次いで、外装材素材を４０℃の環境下に９日間静置するという条件で加熱エージング処理することにより、外側接着剤層５と内側接着剤層６を同時に硬化させた。これにより、最外層２とバリア層３を外側接着剤層５で本接着するとともに、バリア層３とシーラント層４を内側接着剤層６で本接着した。   Next, the outer adhesive layer 5 and the inner adhesive layer 6 were simultaneously cured by subjecting the exterior material to heat aging under the condition that the external material was allowed to stand at 40 ° C. for 9 days. As a result, the outermost layer 2 and the barrier layer 3 were fully bonded with the outer adhesive layer 5, and the barrier layer 3 and the sealant layer 4 were fully bonded with the inner adhesive layer 6.

以上の方法によりリチウムイオン電池用外装材１を得た。   By the above method, the exterior material 1 for a lithium ion battery was obtained.

＜実施例２〜７、比較例１〜４＞
最外層（二軸延伸６ナイロンフィルム）２の厚さ、グラビアロールの表面に施されるメッシュ数及び深度を様々に変更して上記実施例１と同様に外装材１を得た。 <Examples 2 to 7, Comparative Examples 1 to 4>
The packaging material 1 was obtained in the same manner as in Example 1 except that the thickness of the outermost layer (biaxially stretched 6 nylon film) 2, the number of meshes applied to the surface of the gravure roll, and the depth were variously changed.

上記の実施例１〜７及び比較例１〜４のそれぞれの外装材１について、最外層２の表面２ａの表面性状を測定し、また最外層２の表面２ａの粘着テープとの密着性を調べ、また最外層２の表面２ａの滑り性を評価するために最外層２の表面２ａの動摩擦係数を測定した。その結果を表１にまとめて示す。   For each of the packaging materials 1 of Examples 1 to 7 and Comparative Examples 1 to 4, the surface properties of the surface 2a of the outermost layer 2 were measured, and the adhesion of the surface 2a of the outermost layer 2 to the adhesive tape was examined. The dynamic friction coefficient of the surface 2a of the outermost layer 2 was measured to evaluate the slipperiness of the surface 2a of the outermost layer 2. The results are summarized in Table 1.

Figure 2020021727
Figure 2020021727

表１中の「最外層」の「材質」欄において、「Ｎｙ」は二軸延伸６ナイロンフィルムを意味している。   In the “Material” column of “Outermost layer” in Table 1, “Ny” means a biaxially stretched 6 nylon film.

表面性状の測定、粘着テープとの密着性の評価、及び、動摩擦係数（滑り性）の測定はそれぞれ次のようにして行った。   The measurement of the surface properties, the evaluation of the adhesion to the pressure-sensitive adhesive tape, and the measurement of the dynamic friction coefficient (slipperiness) were performed as follows.

<<表面性状>>
外装材１の最外層２の表面２ａについてＩＳＯ ２５１７８に準拠して表面性状として算術平均高さＳａを測定するとともに、１ｍｍ２当たりの山８の数、及び、１ｍｍ２に存在する互いに近接する山８の重心位置Ｃ間の距離を測定した。このときの測定条件及び測定方法は次のとおりである。 << Surface properties >>
With measuring the arithmetic average height Sa as surface properties in compliance with ISO 25178 for the surface 2a of the outermost layer 2 of the outer package 1, the number of 1 mm 2 per mountain 8, and a mountain close to each other are present in 1 mm 2 The distance between the centroid positions C of No. 8 was measured. The measuring conditions and measuring method at this time are as follows.

外装材１から縦１０ｍｍ×横１０ｍｍの正方形の試料を切り出した。この試料の表面について任意の箇所で表面性状を走査型白色干渉顕微鏡（日立ハイテクノロジーズ社製「ＶＳ１３３０」）を用いて測定した。この測定に用いたレンズは二光束干渉対物レンズ５×、波長フィルターは５２０ｎｍであった。   From the exterior material 1, a square sample of 10 mm long × 10 mm wide was cut out. The surface property of the surface of the sample was measured at an arbitrary position using a scanning white interference microscope (“VS1330” manufactured by Hitachi High-Technologies Corporation). The lens used for this measurement was a two-beam interference objective lens 5 ×, and the wavelength filter was 520 nm.

表１中の「最小距離ｄｍｉｎ」欄及び「最大距離ｄｍａｘ」欄の数値は、それぞれ、１ｍｍ２に存在する互いに近接する山８の重心位置Ｃ間の距離についての最小距離ｄｍｉｎ及び最大距離ｄｍａｘを意味している。 The numerical values in the “minimum distance dmin” column and “maximum distance dmax” column in Table 1 represent the minimum distance dmin and the maximum distance dmax for the distance between the centers of gravity C of the mutually adjacent peaks 8 existing at 1 mm 2 , respectively. Means.

<<粘着テープとの密着性>>
最外層２の表面２ａの粘着テープとの密着性を次の条件及び方法で調べた。 << Adhesiveness with adhesive tape >>
The adhesion of the surface 2a of the outermost layer 2 to the adhesive tape was examined under the following conditions and method.

外装材１から幅１５ｍｍ×長さ１５０ｍｍの試験片を切り出した。この試験片の表面にその長さ方向に沿って粘着力１３Ｎ／ｃｍの粘着テープ（ｔｅｓａ ７０４１５）を貼り付けた。粘着テープの幅は５ｍｍ、その長さは８０ｍｍ以上であった。そして、この粘着テープ上に重さ２ｋｇｆのハンドロールを５往復走行させ、その後、常温で１時間静置した。   A test piece having a width of 15 mm and a length of 150 mm was cut out from the exterior material 1. An adhesive tape (tesa 70415) having an adhesive force of 13 N / cm was attached to the surface of the test piece along its length direction. The width of the adhesive tape was 5 mm, and the length was 80 mm or more. Then, a hand roll having a weight of 2 kgf was reciprocated five times on the adhesive tape, and then allowed to stand at room temperature for 1 hour.

次いで、引張試験機として島津製作所製ストログラフ（ＡＧＳ−５ｋＮＸ）を用い、その一方のチャックで試験片の端部を挟着固定するとともに、他方のチャックで粘着テープの端部を掴んだ。そして、ＪＩＳ Ｋ６８５４−３（１９９９）に準拠して３００ｍｍ／ｍｉｎの剥離速度で１８０°剥離させた時の剥離強度を測定し、この測定値が安定したところの値を最外層２の表面２ａの粘着テープとの密着力（その単位：Ｎ／５ｍｍ）とした。   Next, a stroma (AGS-5kNX) manufactured by Shimadzu Corporation was used as a tensile tester, and one end of the test piece was pinched and fixed, and the other end of the adhesive tape was gripped by the other chuck. Then, the peel strength at the time of 180 ° peeling at a peeling speed of 300 mm / min was measured in accordance with JIS K 6854-3 (1999), and the value at which this measured value was stabilized was taken as the value of the surface 2 a of the outermost layer 2. The adhesive force with the adhesive tape (unit: N / 5 mm) was used.

そして、最外層２の表面２ａの粘着テープとの密着性についての評価基準として、粘着テープとの密着力が６Ｎ／５ｍｍ以上である場合を「◎（非常に高い）」、５Ｎ／５ｍｍ以上６Ｎ／５ｍｍ未満である場合を「○（高い）」、及び、５Ｎ／５ｍｍ未満である場合を「×（低い）」とした。   Then, as an evaluation criterion for the adhesiveness of the surface 2a of the outermost layer 2 to the adhesive tape, a case where the adhesive force with the adhesive tape is 6N / 5mm or more is "◎ (very high)", 5N / 5mm or more and 6N or more. The case where it was less than / 5 mm was rated as “○ (high)”, and the case where it was less than 5 N / 5 mm was rated as “x (low)”.

<<動摩擦係数（滑り性）>>
最外層２の表面２ａの滑り性を評価するため、最外層２の表面２ａの動摩擦係数をＪＩＳ Ｋ７１２５（１９９９）に準拠して測定した。 << Dynamic friction coefficient (slipperiness) >>
In order to evaluate the slipperiness of the surface 2a of the outermost layer 2, the kinetic friction coefficient of the surface 2a of the outermost layer 2 was measured according to JIS K7125 (1999).

表１に示すように、実施例１〜７の外装材１の最外層２の表面２ａは動摩擦係数が小さく、滑り性が良好であった。さらに、実施例１〜７の外装材１の最外層２の表面２ａは粘着テープとの密着性が高く、特に実施例１〜６の外装材１の最外層２の表面２ａは粘着テープとの密着性が非常に高かった。   As shown in Table 1, the surface 2a of the outermost layer 2 of the exterior materials 1 of Examples 1 to 7 had a small coefficient of kinetic friction and had good slipperiness. Furthermore, the surface 2a of the outermost layer 2 of the exterior material 1 of Examples 1 to 7 has high adhesion to the adhesive tape, and particularly the surface 2a of the outermost layer 2 of the exterior material 1 of Examples 1 to 6 The adhesion was very high.

本発明は、蓄電デバイス（例：リチウムイオン電池、リチウムイオンキャパシタ、電気二重層キャパシタ）用外装材に利用可能である。   INDUSTRIAL APPLICABILITY The present invention can be used for an exterior material for a power storage device (eg, lithium ion battery, lithium ion capacitor, electric double layer capacitor).

１：外装材
２：最外層
３：バリア層
４：シーラント層
５：外側接着剤層
６：内側接着剤層
８：山
Ｃ：山の重心位置 1: exterior material 2: outermost layer 3: barrier layer 4: sealant layer 5: outer adhesive layer 6: inner adhesive layer 8: mountain C: center of gravity of mountain

本発明者は、蓄電デバイス用外装材について鋭意研究調査したところ、外装材の最外層が所定のフィルムからなり、更に、最外層の表面の表面性状において、算術平均高さＳａが所定の範囲であり且つ当該表面に存在する多数の凸部のうち所定の大きさの凸部の１ｍｍ２当たりの数が所定の範囲であるものであれば、上記目的を達成しうることが判明し、本発明を完成させた。 The present inventors have revealed that extensive research for exterior material for a power storage device becomes the outermost layer of the outer package from given film, further, the surface texture of the surface of the outermost layer, the range arithmetic average height Sa is given It is clear that the above object can be achieved if the number of projections of a predetermined size per 1 mm 2 among a large number of projections existing on the surface is within a predetermined range. Completed the invention.

Claims (6)

最外層と、シーラント層と、前記両層間に配置されたバリア層とを積層状に備えた蓄電デバイス用外装材であって、
前記最外層は、ポリアミドフィルム、ポリエステルフィルム及びポリオレフィンフィルムからなる群より選択される少なくとも一つからなり、
前記最外層の表面の表面性状において、
算術平均高さＳａが０．０３〜０．２０μｍの範囲であり、
前記Ｓａの基準面から＋０．１μｍの高さ位置の断面積が７５００μｍ２以上である凸部を山と定義するとき、山の数が１ｍｍ２当たり５〜３０個の範囲である蓄電デバイス用外装材。 An outermost layer, a sealant layer, and a packaging material for a power storage device including a barrier layer disposed between the two layers in a stacked state,
The outermost layer is made of at least one selected from the group consisting of a polyamide film, a polyester film, and a polyolefin film,
In the surface properties of the surface of the outermost layer,
Arithmetic mean height Sa is in the range of 0.03 to 0.20 μm,
When a convex portion having a sectional area of 7,500 μm 2 or more at a height position of +0.1 μm from the reference surface of Sa is defined as a mountain, the number of the mountain ranges from 5 to 30 per mm 2. Wood. 前記山における前記基準面から＋０．１μｍの高さ位置の断面の重心位置を前記山の重心位置と定義するとき、１ｍｍ２に存在する互いに近接する前記山の重心位置間の距離が全て１５０〜７００μｍの範囲である請求項１記載の蓄電デバイス用外装材。 When the position of the center of gravity of the cross section at a height of +0.1 μm from the reference plane in the peak is defined as the position of the center of gravity of the peak, the distance between the positions of the centers of gravity of 1 mm 2 which are close to each other is all 150 to The exterior material for an electricity storage device according to claim 1, which has a range of 700 µm. 前記最外層と前記バリア層が、これら両層間に配置された接着剤層で接着されており、
前記接着剤層の前記最外層側に向いた面が凹凸状に形成されている請求項１又は２記載の蓄電デバイス用外装材。 The outermost layer and the barrier layer are bonded by an adhesive layer disposed between these two layers,
The exterior material for an electric storage device according to claim 1 or 2, wherein a surface of the adhesive layer facing the outermost layer is formed in an uneven shape. 前記接着剤層の前記最外層側の向いた面に形成された凹凸の箇所と、前記最外層の表面に形成された凹凸の箇所とが略一致している請求項３記載の蓄電デバイス用外装材。   4. The exterior for a power storage device according to claim 3, wherein the uneven portion formed on the surface of the adhesive layer facing the outermost layer substantially matches the uneven portion formed on the surface of the outermost layer. 5. Wood. 請求項３又は４記載の蓄電デバイス用外装材の製造方法であって、
外装材における最外層とバリア層の間に配置される接着剤層の接着剤をグラビア塗工法によりバリア層上に塗工する蓄電デバイス用外装材の製造方法。 It is a manufacturing method of the exterior material for electrical storage devices of Claim 3 or 4, Comprising:
A method for manufacturing an exterior material for an electric storage device, wherein an adhesive of an adhesive layer disposed between an outermost layer and a barrier layer in the exterior material is coated on the barrier layer by a gravure coating method. 請求項１〜４のいずれかに記載の蓄電デバイス用外装材で蓄電デバイス内容物が包装された蓄電デバイス。   An electricity storage device in which the electricity storage device contents are packaged with the electricity storage device exterior material according to claim 1.
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