TW201609845A - 金屬箔與樹脂薄膜之疊層用接著劑、使用該組成物之層合體、電池外裝用包裝材料及電池外殼 - Google Patents

金屬箔與樹脂薄膜之疊層用接著劑、使用該組成物之層合體、電池外裝用包裝材料及電池外殼 Download PDF

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TW201609845A
TW201609845A TW104117428A TW104117428A TW201609845A TW 201609845 A TW201609845 A TW 201609845A TW 104117428 A TW104117428 A TW 104117428A TW 104117428 A TW104117428 A TW 104117428A TW 201609845 A TW201609845 A TW 201609845A
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Taiwan
Prior art keywords
resin film
adhesive
metal foil
laminating
polyol
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TW104117428A
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English (en)
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TWI654215B (zh
Inventor
Hiroto Koka
Kazunari Fukase
Naoki Murata
Hui Li
Yasuhiro Nakagawa
Mitsuru Doi
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Showa Denko Kk
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    • B29C51/00—Shaping by thermoforming, i.e. shaping sheets or sheet like preforms after heating, e.g. shaping sheets in matched moulds or by deep-drawing; Apparatus therefor
    • B29C51/002—Shaping by thermoforming, i.e. shaping sheets or sheet like preforms after heating, e.g. shaping sheets in matched moulds or by deep-drawing; Apparatus therefor characterised by the choice of material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C51/00—Shaping by thermoforming, i.e. shaping sheets or sheet like preforms after heating, e.g. shaping sheets in matched moulds or by deep-drawing; Apparatus therefor
    • B29C51/08—Deep drawing or matched-mould forming, i.e. using mechanical means only
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B29C55/00—Shaping by stretching, e.g. drawing through a die; Apparatus therefor
    • B29C55/005—Shaping by stretching, e.g. drawing through a die; Apparatus therefor characterised by the choice of materials
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B29C55/00—Shaping by stretching, e.g. drawing through a die; Apparatus therefor
    • B29C55/02—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets
    • B29C55/023—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets using multilayered plates or sheets
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Abstract

一種金屬箔與樹脂薄膜之疊層用接著劑等，其係具有：使含有鏈狀聚烯烴多元醇(a1)及/或具有來自氫化二聚酸之構成單位與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)、一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)、及聚異氰酸酯(c)之成分加成聚合而得到之聚胺基甲酸酯多元醇(A)；與飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)。

Description

金屬箔與樹脂薄膜之疊層用接著劑、使用該組成物之層合體、電池外裝用包裝材料及電池外殼
本發明係關於適於鋰離子電池等之蓄電池的外裝材用接著劑之金屬箔與樹脂薄膜之疊層用接著劑、使用該金屬箔與樹脂薄膜之疊層用接著劑所製造之層合體、使用該層合體之電池外裝用包裝材料及使該電池外裝用包裝材料成形而得之電池外殼。
近年來，筆記型電腦、行動電話等之電子機器，正進行小型化、輕量化、薄型化。因此，關於電子機器用之二次蓄電池，亦要求高性能化、輕量化、移動性能之提高，開發具有高能量密度之鋰離子電池以取代以往的鉛蓄電池，正積極地進行。進而，亦可使用於電動車或油電混合車之電源的鋰離子電池正在實用化。
鋰離子電池中，係使用含鋰之化合物作為正極材料、使用石墨或煤焦等碳材料作為負極材料。進一步地，於正極及負極之間，具備由於碳酸伸丙酯、碳酸伸乙酯等具有滲透力的非質子性溶劑中溶解有作為電解質之 LiPF6、LiBF4等鋰鹽的電解液、或含浸該電解液而得的聚合物凝膠所構成之電解質層。
自以往起，作為電池外殼用包裝材料，已知有依序層合作為外側層之耐熱性樹脂延伸薄膜層、鋁箔層、與作為內側層之熱可塑性樹脂未延伸薄膜層而得的層合體。使用如此之構造的電池外殼用包裝材料而得之電池外殼的情況時，如電解液般之具有滲透力的溶劑通過作為電池外裝所用之層合體中的密封劑之薄膜層時，鋁箔層與樹脂薄膜層間之疊層強度降低，可能成為電解液漏出的原因。因此，正在開發於鋁箔層與內側層之間透過接著劑層接著的電池外殼用包材，該接著劑層含有：含有酸酐基或羧基、羥基等之具備與異氰酸酯之反應性的官能基之樹脂、與多官能異氰酸酯化合物。
例如，專利文獻1中，記載使用溶劑型接著劑形成接著劑層的方法，該溶劑型接著劑係將使乙烯性不飽和羧酸或其酸酐接枝聚合於丙烯之均聚物或丙烯與乙烯之共聚物而得的改質聚烯烴樹脂與多官能異氰酸酯化合物溶解或分散於有機溶劑而得。
另一方面，專利文獻2中，記載了以聚烯烴多元醇與多官能異氰酸酯硬化劑為必須成分，且進一步添加熱可塑性彈性體及/或增黏劑之接著劑組成物；專利文獻3中，記載一種接著劑組成物，其含有選自由具有來自二聚物脂肪酸或其氫化物之疏水性單位的聚酯多元醇、及該聚酯多元醇之異氰酸酯伸長物所成群組的1種以上之主 劑；與由選自由粗甲伸苯基二異氰酸酯、粗二苯基甲烷二異氰酸酯及聚合物型二苯基甲烷二異氰酸酯所成群組之1種以上的聚異氰酸酯化合物所構成之硬化劑。
[先前技術文獻] [專利文獻]
[專利文獻1]日本特開2010-92703號公報
[專利文獻2]日本特開2005-63685號公報
[專利文獻3]日本特開2011-187385號公報
但是，專利文獻1之改質聚烯烴樹脂，於長期保存中或溶劑溶解後係有經時變化，常有塗佈時之操作性變得不安定者，又，係有所形成之接著劑層的接著力產生偏差之虞。又，亦有於假定於車載用途等之高溫下的接著力不佳之虞。
又，專利文獻2及專利文獻3的情況時，塗佈時之操作性或接著力雖比較安定，但接著劑層接觸於通過作為層合體中之密封劑的薄膜層而來的電解液時，會有接著力降低，電池之品質降低的問題。
本發明係於該背景技術下完成者，其目的為提供具有優良接著力，適合作為鋁箔與熱熔合性樹脂薄膜之接合用的疊層用金屬箔與樹脂薄膜之疊層用接著劑。 又，本發明之其他目的，為提供耐熱性、耐電解液性優良，適於電池外裝用包裝材料之金屬箔與樹脂薄膜之層合體。進一步地，本發明之又一其他目的，為提供使用由該層合體所構成之電池外裝用包裝材料所形成之耐熱性、耐電解液性優良的電池外殼。
亦即本發明係關於以下之〔1〕~〔15〕。
〔1〕一種聚胺基甲酸酯多元醇，其係使用於聚胺基甲酸酯系接著劑之多元醇，且該多元醇為使含有：鏈狀聚烯烴多元醇(a1)及/或具有來自氫化二聚酸之構成單位與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)、一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)、及聚異氰酸酯(c)之成分加成聚合而得到。
〔2〕一種金屬箔與樹脂薄膜之疊層用接著劑，其係具有：使含有：鏈狀聚烯烴多元醇(a1)及/或具有來自氫化二聚酸之構成單位與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)、一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)、及聚異氰酸酯(c)之成分加成聚合而得到之聚胺基甲酸酯多元醇(A)；與飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)。
〔3〕如〔2〕之金屬箔與樹脂薄膜之疊層用接著 劑，其中前述含有羥基之烴化合物(b)，為含有具有交聯構造之飽和脂環構造的多元醇。
〔4〕如〔2〕或〔3〕之金屬箔與樹脂薄膜之疊層用接著劑，其中前述含有羥基之烴化合物(b)，為雙酚化合物。
〔5〕如〔2〕~〔4〕中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中前述聚異氰酸酯(c)，為飽和脂環式二異氰酸酯。
〔6〕如〔2〕~〔5〕中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中前述鏈狀聚烯烴多元醇(a1)，為實質上不含有不飽和烴構造之聚烯烴多元醇。
〔7〕如〔2〕~〔6〕中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中(b)成分，相對於(a1)及(a2)成分之總量100質量份而言，為5~100質量份，(c)成分中含有的異氰酸基數之比率，相對於(a1)、(a2)及(b)成分中含有的羥基數而言，為0.5~1.3。
〔8〕如〔2〕~〔7〕中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中相對於前述聚胺基甲酸酯多元醇(A)中含有的羥基數而言，聚異氰酸酯(B)中含有的異氰酸基數之比率為1~15。
〔9〕如〔2〕~〔8〕中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其係進一步含有溶劑(C)。
〔10〕一種層合體，其係金屬箔與樹脂薄膜隔著由如〔2〕~〔9〕中任一項之金屬箔與樹脂薄膜之疊層用接 著劑所得到之接著劑層而層合。
〔11〕如〔10〕之層合體，其中前述金屬箔為鋁箔，且前述樹脂薄膜含有熱熔合性樹脂薄膜。
〔12〕如〔10〕或〔11〕之層合體，其中前述金屬箔之厚度為10~100μm，且前述樹脂薄膜之厚度為9~100μm。
〔13〕一種電池外裝用包裝材料，其係使用如〔10〕~〔12〕中任一項之層合體而得到。
〔14〕一種電池外殼，其係使用如〔13〕之電池外裝用包裝材料而得到。
〔15〕一種電池外殼之製造方法，其係將如〔13〕之電池外裝用包裝材料予以深抽拉成形或拉伸膨脹成形。
本發明之金屬箔與樹脂薄膜之疊層用接著劑，接著力優良，使用該金屬箔與樹脂薄膜之疊層用接著劑所形成之金屬箔與樹脂薄膜之層合體，耐熱性、耐電解液性優良，因而適合作為鋰離子電池等之蓄電池的製作所用的電池外裝用包裝材料之素材。又，使用本發明之電池外裝用包裝材料所成形之電池外殼，耐熱性、耐電解液性優良，藉由使用該電池外殼，可提供壽命長之安全的蓄電池。
本發明之金屬箔與樹脂薄膜之疊層用接著劑，係含有：使含有鏈狀聚烯烴多元醇(a1)及/或具有來自氫化二聚酸之構成單位與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)、一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)、及聚異氰酸酯(c)之成分加成聚合而得到之聚胺基甲酸酯多元醇(A)；與飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)。
本發明之金屬箔與樹脂薄膜之疊層用接著劑中，前述聚胺基甲酸酯多元醇(A)相當於主劑、前述飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)相當於硬化劑。
本發明之金屬箔與樹脂薄膜之疊層用接著劑，可適合使用於金屬箔與樹脂薄膜之接著，特別是有用於作為金屬箔與樹脂薄膜疊層用之接著劑，其層合體可適合使用作為電池外裝用包裝材料。
此處，本說明書中之「~」，意指「~」之記載之前的值以上、且「~」之記載之後的值以下。
<聚胺基甲酸酯多元醇(A)>
用於本發明之聚胺基甲酸酯多元醇(A)，如上所述，係使含有(a1)及/或(a2)成分、(b)成分、與(c)成分之成分加成聚合而得到。
〔鏈狀聚烯烴多元醇(a1)〕
本發明之「鏈狀聚烯烴多元醇(a1)」，意指不含有脂 環構造之聚烯烴多元醇(a1)。
使用於本發明之鏈狀聚烯烴多元醇(a1)(以下亦稱為「聚烯烴多元醇(a1)」)，只要係含有使1種或2種以上之烯烴聚合或共聚合而成的聚烯烴骨架、與2個以上之羥基，且不具有脂環構造者，則無特殊限制。具體例子可列舉聚丁二烯多元醇、聚異戊二烯多元醇等之聚二烯多元醇；聚二烯多元醇與聚烯烴之接枝聚合物及此等之聚二烯多元醇或接枝聚合物之氫化物等。此等可單獨或混合2種以上使用。由自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的耐電解液性之觀點而言，較佳為構造中實質上不含有不飽和烴構造的鏈狀聚烯烴多元醇，可列舉例如上述所列舉之各種聚二烯多元醇或接枝聚合物之氫化物。此等之市售品，可列舉例如GI-1000、GI-2000、GI-3000(均為日本曹達股份有限公司製)、EPOL(出光興產股份有限公司製)等。
聚烯烴多元醇(a1)之數平均分子量，較佳為1000~10,000。數平均分子量若為1000以上，自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的接著力，即使接觸電解液亦不易降低，數平均分子量若為10,000以下，則後述之聚胺基甲酸酯多元醇(G)對溶劑之溶解性、及本發明之金屬箔與樹脂薄膜之疊層用接著劑塗佈時之操作性成為良好。
再者，本發明中之數平均分子量，係使用凝膠滲透層析(昭和電工股份有限公司製、Shodex GPC System-11、「Shodex」(註冊商標))，以下述條件於常溫測定，且使用標準聚苯乙烯檢量線所求得之值。
管柱：昭和電工股份有限公司製、KF-806L
管柱溫度：40℃
試樣：試樣聚合物之0.2質量%四氫呋喃溶液
流量：2ml/分
溶離液：四氫呋喃
檢測器：示差折射率計(RI)
〔具有來自氫化二聚酸之構成單位、與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)〕
使用於本發明之具有來自氫化二聚酸之構成單位、與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)(以下亦稱為「聚酯多元醇(a2)」)，由自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的耐電解液性之觀點而言，係具有來自氫化二聚酸之構成單位、與來自氫化二聚物二醇之構成單位。
本說明書中之「二聚酸」，係指使具有乙烯性雙鍵之碳數14~22之脂肪酸(以下亦稱為「不飽和脂肪酸A」)於雙鍵部反應而得之二聚物酸。較佳為使具有2~4個乙烯性雙鍵之不飽和脂肪酸A與具有1~4個乙烯性雙鍵之不飽和脂肪酸A、更佳為使具有2個乙烯性雙鍵之不飽和脂肪酸A與具有1或2個乙烯性雙鍵之不飽和脂肪酸A反應而得之二聚物酸。上述不飽和脂肪酸A，可列舉十 四烯酸(粗租酸(tsuzuic acid)、抹香酸、肉豆蔻油酸)、十六烯酸(棕櫚油酸等)、十八烯酸(油酸、反油酸、反11-十八烯酸等)、二十烯酸(鱈油酸等)、二十二烯酸(芥子酸、鯨蠟烯酸(cetoleic acid)、反芥子酸等)、十四碳二烯酸、十六碳二烯酸、十八碳二烯酸(亞油酸等)、二十碳二烯酸、二十二碳二烯酸、十八碳三烯酸(次亞麻油酸等)、二十碳四烯酸(花生四烯酸等)等，最佳為油酸或亞油酸。所得到之二聚酸，通常係依雙鍵之鍵結部位或異性化，而構造相異的二聚酸混合物，雖可分離來使用，但亦可直接使用。進一步地，所得到之二聚酸，亦可含有少量之單體酸(例如6重量%以下、特別是4重量%以下)或三聚物酸以上之聚合物酸等(例如6重量%以下、特別是4重量%以下)。
本說明書中之「氫化二聚酸」，係指使上述二聚酸之碳-碳雙鍵氫化所得之飽和二羧酸。氫化二聚酸之市售品，可列舉例如EMPOL1008及EMPOL1062(均為BASF公司製)、PRIPOL1009等(Croda公司製)等。
本發明中之「氫化二聚物二醇」，係指使上述二聚酸、上述氫化二聚酸及其低級醇酯之至少1種於觸媒存在下還原，以二聚酸之羧酸或羧酸酯部分為醇，於原料具有碳-碳雙鍵的情況時係以使該雙鍵氫化的二醇為主成分者。氫化二聚物二醇之市售品，可列舉例如Sovermol908(BASF公司製)或PRIPOL2033等(Croda公司製)。
使用於本發明之聚酯多元醇(a2)，可藉由使以 前述氫化二聚酸為必須成分之酸成分、與以前述氫化二聚物二醇為必須成分之醇成分，在酯化觸媒之存在下進行縮合反應來製造。或者，亦可藉由使以前述氫化二聚酸之低級烷基酯為必須成分之酯成分、與以前述氫化二聚物二醇為必須成分之醇成分，在酯交換觸媒之存在下進行酯交換反應來製造。
〔一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)〕
使用於本發明之一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)(以下亦稱為「含有羥基之環式烴(b)」)，由自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的耐電解液性之觀點而言，只要係具有不飽和或飽和脂環式烴構造與2個以上之羥基，且其他部分之構造係由烴所構成之化合物，則無特殊限制。
飽和環式烴構造，可列舉環戊烷骨架、環己烷骨架、環庚烷骨架等之環烷骨架；降莰烷骨架、金剛烷骨架、三環癸烷骨架等之具有交聯構造之飽和脂環構造等，作為具有如此構造之含有羥基之環式烴(b)，可列舉環戊烷二醇、環己烷二醇、環己烷二甲醇、降莰烷二醇、金剛烷二醇、三環癸烷二甲醇等。此等可單獨或混合2種以上使用。較佳為含有具有交聯構造之飽和脂環構造者，較佳例子可列舉降莰烷二醇、金剛烷二醇、三環癸烷二甲醇等。 該等之市售品，可列舉金剛烷三醇(出光興產股份有限公司製、三菱瓦斯化學股份有限公司製)、TCD Alcohol DM(OXEA公司製)等。
不飽和環式烴構造，可列舉環戊烯骨架、環己烯骨架、環庚烯骨架、[4n]輪烯骨架等之環烯骨架；苯骨架、萘骨架、蒽骨架、薁骨架、[4n+2]輪烯骨架等之共軛環構造；二環戊二烯骨架等之具有交聯構造之不飽和脂環構造等，作為具有如此構造之多元醇(b)，可列舉環己烯二醇、聯酚、雙酚、萘二醇、二環戊二烯基二甲醇等。此等可單獨或混合2種以上使用。較佳為雙酚，可列舉雙酚A、雙酚B、雙酚C、雙酚E、雙酚F、雙酚G、雙酚Z等，更佳為雙酚A。
〔聚異氰酸酯(c)〕
本發明所用之聚異氰酸酯(c)，只要係含有2個以上之異氰酸基的化合物、或其多聚物，則無特殊限制。可列舉例如1,4-環己烷二異氰酸酯、異佛酮二異氰酸酯、亞甲基雙(4-環己基異氰酸酯)、1,3-雙(異氰酸基甲基)環己烷、1,4-雙(異氰酸基甲基)環己烷、降莰烷二異氰酸酯等之飽和脂環式二異氰酸酯；2,4-甲伸苯基二異氰酸酯、2,6-甲伸苯基二異氰酸酯、二苯基甲烷-4,4'-二異氰酸酯、1,3-伸苯二甲基二異氰酸酯、1,4-伸苯二甲基二異氰酸酯等之芳香族二異氰酸酯；六亞甲基二異氰酸酯、2,4,4-三甲基六亞甲基二異氰酸酯、2,2,4-三甲基己烷亞甲基二異氰酸酯 等之脂肪族二異氰酸酯；或此等之脲甲酸酯化多聚物、三聚異氰酸酯化物、縮二脲改質物等。此等可單獨或混合2種以上使用。較佳為飽和脂環式二異氰酸酯，可列舉1,4-環己烷二異氰酸酯、異佛酮二異氰酸酯、亞甲基雙(4-環己基異氰酸酯)、1,3-雙(異氰酸基甲基)環己烷、1,4-雙(異氰酸基甲基)環己烷、降莰烷二異氰酸酯等，特佳為異佛酮二異氰酸酯(3-異氰酸酯甲基-3,5,5-三甲基環己基異氰酸酯)、亞甲基雙(4-環己基異氰酸酯)(別名：二環己基甲烷-4,4’-二異氰酸酯)。此等之市售品，可列舉Desmodur I、Desmodur W(各為Bayer公司製)、IPDI、H12MDI(各為Degussa公司製)等。
〔聚胺基甲酸酯多元醇(A)之製造方法〕
本發明所用之聚胺基甲酸酯多元醇(A)之製造方法，可藉由於如二月桂酸二丁基錫、二月桂酸二辛基錫、參2-乙基己酸鉍、四乙醯基丙酮酸鋯之公知的胺基甲酸酯化觸媒之存在下或非存在下，使聚烯烴多元醇(a1)及/或聚酯多元醇(a2)、含有羥基之環式烴化合物(b)、與聚異氰酸酯(c)進行加成聚合反應來進行。於觸媒之存在下反應，就縮短反應時間之意義而言較佳。又，該觸媒，較佳為亦用以存在作為當聚胺基甲酸酯多元醇(A)與飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)進行反應而硬化時的硬化促進劑的作用。惟，使用過多時，最終有對作為金屬箔與樹脂薄膜之疊層用接著劑的物性造成不良影響的可能性，因此其使 用量，相對於(a1)、(a2)、(b)及(c)成分之總量100質量份而言，較佳為0.001~1質量份、更佳為0.005~0.5質量份、又更佳為0.01~0.3質量份。又，加成聚合之反應，可使聚烯烴多元醇(a1)及/或聚酯多元醇(a2)、含有羥基之環式烴化合物(b)、與聚異氰酸酯(c)一次全部反應，亦可使聚烯烴多元醇(a1)及/或聚酯多元醇(a2)、與含有羥基之環式烴化合物(b)分別各自地，或適當地組合而與聚異氰酸酯(c)反應後，混合全部的成分進一步進行反應。後者之方法，可列舉例如使含有羥基之環式烴化合物(b)與聚異氰酸酯(c)反應而得到聚胺基甲酸酯聚異氰酸酯後，使聚烯烴多元醇(a1)及/或聚酯多元醇(a2)進行反應而得到聚胺基甲酸酯多元醇(A)等的方法。
又，該加成聚合之反應，亦可於溶劑中進行。所使用之溶劑並無特殊限制，若使用與後述之本發明之金屬箔與樹脂薄膜之疊層用接著劑中可含有的溶劑(C)相同之物，則可省略溶劑餾去等之工程，能夠以更低成本且抑制環境負荷地來製造。
製造聚胺基甲酸酯多元醇(A)時，相對於(a1)、(a2)及(b)成分中所含的羥基數而言，聚異氰酸酯(c)中所含的異氰酸基數之比率(以下亦稱為「NCO/OH比」)，較佳為0.5~1.3、更佳為0.7~1.2、又更佳為0.8~1.1。若為0.5以上，則自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的接著力，即使接觸於電解液亦不易降低，若為1.3以下，則不易引起聚胺基甲 酸酯多元醇(A)製造時之凝膠化，且本發明之金屬箔與樹脂薄膜之疊層用接著劑之塗佈時的操作性成為良好。再者各多元醇成分中所含的羥基數，可由如JIS K 1557-1之滴定法、或如JIS K 1557-6之分光法等公知之方法來求得。後述實施例中，係使用JIS K 1557-1(滴定法)。各異氰酸酯成分中所含的異氰酸基數，可由如JIS K 6806之滴定法等公知之方法求得。
製造聚胺基甲酸酯多元醇(A)時，相對於(a1)及(a2)成分之總量100質量份而言，含有羥基之環式烴化合物(b)之比率，較佳為5~100質量份、更佳為10~50質量份、又更佳為10~45質量份。若為5質量份以上，則自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的接著力，即使接觸於電解液亦不易降低，若為100質量份以下，則聚胺基甲酸酯多元醇(A)對溶劑之溶解性、及本發明之金屬箔與樹脂薄膜之疊層用接著劑之塗佈時的操作性成為良好。
<飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)>
本發明中之飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)(以下亦稱為「聚異氰酸酯(B)」)係於本發明之金屬箔與樹脂薄膜之疊層用接著劑中作為硬化劑而摻合者，與作為前述之聚胺基甲酸酯多元醇(A)製造時的原料所記載的聚異氰酸酯(c)係有區別地記載。
本發明所用之飽和脂肪族及/或飽和脂環式聚 異氰酸酯(B)，只要係由2個以上之異氰酸基所成之化合物、或該等之多聚物，則無特殊限制。可列舉例如六亞甲基二異氰酸酯、2,4,4-三甲基六亞甲基二異氰酸酯、2,2,4-三甲基己烷亞甲基二異氰酸酯等之脂肪族二異氰酸酯；1,4-環己烷二異氰酸酯、異佛酮二異氰酸酯、亞甲基雙(4-環己基異氰酸酯)、1,3-雙(異氰酸基甲基)環己烷、1,4-雙(異氰酸基甲基)環己烷、降莰烷二異氰酸酯等之飽和脂環式二異氰酸酯；或此等之脲甲酸酯化多聚物、三聚異氰酸酯化物、縮二脲改質物等。此等可單獨或混合2種以上使用。由自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的耐電解液性之觀點而言，更佳為飽和脂肪族二異氰酸酯與飽和脂環式二異氰酸酯之組合、及僅飽和脂環式二異氰酸酯。
相對於聚胺基甲酸酯多元醇(A)而言，聚異氰酸酯(B)之NCO/OH比，較佳為1~20、更佳為1~15、又更佳為1~13。NCO/OH比若為1以上，則自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層之特別係對樹脂薄膜之接著力成為良好，NCO/OH比若為20以下，則自本發明之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層的接著力，即使接觸於電解液亦不易降低。
<溶劑(C)>
本發明之金屬箔與樹脂薄膜之疊層用接著劑，亦可含有溶劑(C)。溶劑(C)，只要係可溶解或分散聚胺基甲酸酯 多元醇(A)及聚異氰酸酯(B)者，則無特殊限制。可列舉例如甲苯、二甲苯等之芳香族系有機溶劑；環己烷、甲基環己烷、乙基環己烷等之脂環式系有機溶劑；n-己烷、n-庚烷等之脂肪族系有機溶劑；乙酸乙酯、乙酸丙酯、乙酸丁酯等之酯系有機溶劑；丙酮、甲基乙基酮、甲基丁基酮等之酮系有機溶劑等。此等可單獨或混合2種以上使用。
此等之中，特別由聚胺基甲酸酯多元醇(A)之溶解性的觀點而言，較佳為乙酸乙酯、乙酸丙酯、乙酸丁酯、甲苯、甲基環己烷、甲基乙基酮，更佳為甲苯、甲基乙基酮。
溶劑(C)之含量，相對於由(A)、(B)及(C)成分所構成之金屬箔與樹脂薄膜之疊層用接著劑100質量份而言，較佳為40~95質量份、更佳為50~95質量份、又更佳為80~90質量份。若為40質量份以上，則本發明之金屬箔與樹脂薄膜之疊層用接著劑之塗佈時的操作性成為良好，若為95質量份以下，則將本發明之金屬箔與樹脂薄膜之疊層用接著劑塗佈/硬化所得之層合體的厚度控制性成為良好。
<其他成分>
本發明之金屬箔與樹脂薄膜之疊層用接著劑，亦可依需要，含有反應促進劑、增黏劑、可塑劑等之添加劑。反應促進劑係用以促進聚胺基甲酸酯多元醇(A)及聚異氰酸酯(B)之反應者，可列舉例如有機錫化合物之二月桂酸二 辛基錫、二乙酸二辛基錫，或3級胺之2,4,6-參(二甲基胺基甲基)酚、二甲基苯胺、二甲基對甲苯胺、N,N-二(β-羥基乙基)-p-甲苯胺等。此等之反應促進劑，可單獨或合併使用2種以上。
前述增黏劑，並無特殊限定。例如，天然系可列舉聚萜烯系樹脂、松香系樹脂等，石油系可列舉由輕石油腦之分解油餾分所得之脂肪族(C5)系樹脂、芳香族(C9)系樹脂、共聚合(C5/C9)系樹脂、脂環族系樹脂等。又，可列舉將此等樹脂之雙鍵部分氫化而得的氫化樹脂。該增黏劑可僅使用1種、亦可合併使用2種以上。前述可塑劑並無特殊限定，可列舉例如聚異戊二烯、聚丁烯等之液狀橡膠、加工油等。
又，只要係不阻礙本發明之效果的範囲，則亦可含有酸改質聚烯烴樹脂等之熱可塑性樹脂或熱可塑性彈性體。可摻合之熱可塑性樹脂及熱可塑性彈性體，可列舉例如乙烯-乙酸乙烯酯共聚合樹脂、乙烯-丙烯酸乙酯共聚合樹脂、SEBS(苯乙烯-乙烯-丁烯-苯乙烯)、SEPS(苯乙烯-乙烯-丙烯-苯乙烯)等。
(層合體)
本發明之層合體，係將金屬箔與樹脂薄膜隔著由本發明之金屬箔與樹脂薄膜之疊層用接著劑(以下亦有單稱為「本發明之疊層用接著劑」者)所得到之接著劑層而接合者。又，本發明之層合體中，只要包含將金屬箔與樹脂薄 膜隔著由本發明之疊層用接著劑所得到之接著劑層而接合之層，則其他亦可包含金屬箔彼此及/或樹脂薄膜彼此隔著由本發明之疊層用接著劑所得到之接著劑層而接合之層。該接合方法，可使用熱疊層方式或乾疊層方式等之公知之方法。熱疊層方式，係指將不含溶劑(C)之本發明之疊層用接著劑，於接觸於接著劑層之層表面加熱熔融、或與接觸於接著劑層之層一起加熱擠出，藉此介於層合體之層間而存在，而形成接著劑層的方式。又，乾疊層方式，係指將含有溶劑(C)之本發明之疊層用接著劑，於接觸於接著劑層之層表面塗佈、乾燥後，與另一方之層疊合而壓接，藉此介於層合體之層間而存在，而形成接著劑層之方式。
本發明之層合體之用途並無特殊限定，作為有用的用途，可列舉包裝用途。包裝於該層合體中之內容物，可列舉含酸、鹼、有機溶劑等之液狀物，例如油灰(厚油灰、薄油灰等)、塗料(油性塗料等)、基漆(lacquer)(清基漆等)、自動車用粗蠟等之溶劑系者等。又，該層合體，亦適合於包裝鋰離子電池之電解液，故可使用作為電池外裝用包裝材料，且係較佳。使用作為電池外裝用包裝材料時，較佳為金屬箔為鋁箔、且樹脂薄膜含有熱熔合性樹脂薄膜，再者於鋁箔之外側設有由耐熱性樹脂薄膜所構成之外層。
(電池外裝用包裝材料)
本發明之電池外裝用包裝材料，係本發明之層合體之於金屬箔外側設有由耐熱性樹脂薄膜所構成之外層者。又，依需要，為了提高機械強度或耐電解液性等之特性，可為追加第1中間樹脂層或/及第2中間樹脂層等之構成。作為較佳形態，具體而言可為如下之構成。再者，接著劑層意指「自本發明之疊層用接著劑所得之接著劑層」，金屬箔層係以鋁箔層來例示。
(1)外層/鋁箔層/接著劑層/樹脂薄膜層
(2)外層/第1中間樹脂層/鋁箔層/接著劑層/樹脂薄膜層
(3)外層/鋁箔層/第2中間樹脂層/接著劑層/樹脂薄膜層
(4)外層/第1中間樹脂層/鋁箔層/第2中間樹脂層/接著劑層/樹脂薄膜層
(5)塗層/外層/鋁箔層/接著劑層/樹脂薄膜層
(6)塗層/外層/第1中間樹脂層/鋁箔層/接著劑層/樹脂薄膜層
(7)塗層/外層/鋁箔層/第2中間樹脂層/接著劑層/樹脂薄膜層
(8)塗層/外層/第1中間樹脂層/鋁箔層/第2中間樹脂層/接著劑層/樹脂薄膜層
上述之中，就第1中間樹脂層而言，聚醯胺樹脂、聚酯樹脂或聚乙烯樹脂等係以提高電池外裝用包裝材料之機械強度為目的來使用。就第2中間樹脂層而言，與第1中間樹脂層同樣地，聚醯胺樹脂、聚酯樹脂或聚乙烯樹脂或聚丙烯等之熱接著性擠出樹脂，係主要以提高耐 電解液性為目的來使用。樹脂薄膜層可使用單層樹脂薄膜、複層樹脂薄膜(藉由2層之共擠出或3層之共擠出等來製造)。又，第2中間樹脂層亦可使用單層樹脂薄膜或複層之共擠出樹脂薄膜。第1中間樹脂層及第2中間樹脂層之厚度，並無特殊限定，設置該等的情況時，通常係0.1~30μm左右。
(外層之耐熱性樹脂薄膜)
使用於外層之樹脂薄膜，係耐熱性、成形性、絕緣性等優良者，一般係使用聚醯胺(耐綸)樹脂或聚酯樹脂之延伸薄膜。該外層薄膜之厚度，係9~50μm左右，未達9μm時，進行包裝材料之成形時，延伸薄膜之延伸不足，容易於鋁箔產生頸縮，引起成形不良。另一方面，超過50μm之厚度的情況時，成形性之效果亦不會特別增加，反而僅會降低體積能量密度，而且造成成本增加。外層薄膜之厚度更佳為10~40μm左右、又更佳為20~30μm。
該使用於外層之薄膜，以延伸薄膜之延伸方向為0°時，以0°、45°、90°之3個方向各自成為拉伸方向的方式，將薄膜切出特定的大小，並進行拉伸試驗時，由得到更銳利的形狀的觀點而言，較佳為使用其拉伸強度為150N/mm2以上、較佳為200N/mm2以上、更佳為250N/mm2以上，且3個方向之拉伸所致之延伸為80%以上、較佳為100%以上、更佳為120%以上者。藉由使拉伸強度為150N/mm2以上、或拉伸所致之延伸為80%以上， 會充分發揮上述效果。再者，拉伸強度及拉伸所致之延伸之值，係於薄膜之拉伸試驗(試驗片長度150mm×寬15mm×厚度9~50μm、拉伸速度100mm/min)中至斷裂為止的值。試驗片係對於3個方向分別切出。
(金屬箔)
金屬箔係扮演對水蒸氣等之障壁性的角色，材質一般使用純鋁系或鋁-鐵系合金之O材(軟質材)，且為較佳。鋁箔之厚度，為了確保加工性及確保防止氧或水分侵入包裝內的障壁性，較佳為10~100μm左右。鋁箔之厚度未達10μm時，成形時會有產生鋁箔斷裂、或產生針孔，而使氧或水分入侵之虞。另一方面，鋁箔之厚度超過100μm時，不會特別提高成形時之斷裂改善效果或針孔發生防止效果，而僅有包裝材料之總厚度厚、質量增加、體積能量密度降低。鋁箔一般而言係使用30~50μm左右之厚度者，較佳為使用40~50μm之厚度者。再者，為了提高與樹脂薄膜之接著性或提高耐蝕性，較佳為預先對鋁箔施以矽烷偶合劑或鈦偶合劑等之底塗處理、鉻酸鹽處理等之化成處理。
(樹脂薄膜)
作為樹脂薄膜，較佳為聚丙烯、聚乙烯、馬來酸改質聚丙烯、乙烯-丙烯酸酯共聚物或離子聚合物樹脂等之熱熔合性樹脂薄膜。此等樹脂具有熱封性，扮演提高對腐蝕 性強之鋰蓄電池之電解液等的耐藥品性的角色。此等之薄膜厚度，較佳為9~100μm、更佳為20~80μm、最佳為40~80μm。樹脂薄膜之厚度若為9μm以上，則可得到充分的熱封強度，對電解液等之耐蝕性成為良好。樹脂薄膜之厚度若為100μm以下，則電池外裝用包裝材料之強度充分、且成形性成為良好。
(塗層)
本發明之電池外裝用包裝材料，亦可於外層之上設置塗層。塗層之形成法，係有塗覆氣體障壁性之聚合物的方法、蒸鍍鋁金屬或氧化矽/氧化鋁等之無機氧化物，而塗覆金屬及無機物之薄膜的方法等。藉由設置塗層，可得到水蒸氣及其他之氣體障壁性更優良的層合體。
(電池外殼)
本發明之電池外殼係藉由使本發明之電池外裝用包裝材料成形而得到。本發明之電池外裝用包裝材料，係耐電解液性或耐熱性、水蒸氣及其他之氣體障壁性優良，適合使用作為蓄電池、特別是鋰離子電池用之電池外殼。又，本發明之電池外裝用包裝材料其成形性非常良好，因此藉由遵照公知之方法成形，可簡便地得到本發明之電池外殼。成形之方法並無特殊限定，若藉由深抽拉成形或拉伸膨脹成形而成形時，可製作複雜形狀或尺寸精度高之電池外殼。
[實施例]
以下藉由實施例及比較例以更具體說明本發明，但本發明不受此等實施例之任何限制。
(合成例1)
於附有攪拌機、水分離器之反應容器中，饋入作為氫化二聚物二醇之「Sovermol908」(BASF公司製)220.00g、作為氫化二聚酸之「EMPOL1008」(BASF公司製)230.00g、作為觸媒之二月桂酸丁基錫之「KS-1260」(堺化學工業製)0.10g，於約240℃，自常壓下開始，一邊使縮合水流出，同時減壓，進行脫水酯化反應，得到聚酯多元醇(以下記載為聚酯多元醇(1))。
(合成例2)
於具備攪拌裝置、溫度計及冷凝器之反應容器中，投入雙酚A(新日鐵化學製、化合物名2,2-雙(4-羥基苯基)丙烷)23.29g、「KS-1260」(堺化學工業製、二月桂酸二丁基錫)0.01g、及「Desmodur I」(Bayer公司製異佛酮二異氰酸酯)34.02g、甲基乙基酮113.13g，一邊攪拌，同時使用油浴昇溫至85~90℃。之後，一邊攪拌2.5小時，同時持續反應，得到聚胺基甲酸酯聚異氰酸酯(以下記載為聚胺基甲酸酯聚異氰酸酯(2))之甲基乙基酮溶液。
(合成例3)
除了使用雙酚F(本州化學工業製)20g以取代雙酚A以外，係與合成例2相同方式，得到聚胺基甲酸酯聚異氰酸酯(以下記載為聚胺基甲酸酯聚異氰酸酯(3))之甲基乙基酮溶液。
(合成例4)
於具備攪拌裝置、溫度計及冷凝器之反應容器中，投入聚酯多元醇(1)112.50g、「TCD醇DM」(OXEA公司製、三環癸烷二甲醇)12.50g、對苯二酚單甲基醚(和光純藥工業製)0.04g、「KS-1260」(堺化學工業製、二月桂酸二丁基錫)0.03g、及「Desmodur W」(Bayer公司製、亞甲基雙(4-環己基異氰酸酯))28.97g、甲苯70g，一邊攪拌，同時使用油浴昇溫至85~90℃。之後，一邊攪拌2.5小時，同時持續反應。之後，測定紅外吸收光譜，確認異氰酸基之吸收消失，結束反應，進一步投入甲苯636.5g，攪拌溶解，得到聚胺基甲酸酯多元醇(以下記載為聚胺基甲酸酯多元醇(4))之甲苯溶液(固體成分濃度18質量%)。
(合成例5~10、比較合成例11~13)
以與合成例3相同之方法，以如表2所示之成分、量進行合成，得到聚胺基甲酸酯多元醇(4)~(13)之甲苯溶液或甲苯與甲基乙基酮之混合溶劑溶液(固體成分濃度18質量%)。
表2中，GI-1000、GI-2000係日本曹達製氫化聚丁二烯多元醇，G-1000係日本曹達製聚丁二烯多元醇，14BG係三菱化學製1,4-丁二醇。
關於合成例1~10及比較合成例11~13，係示於表1、2。
(實施例1)
於合成例4中所得之聚胺基甲酸酯多元醇(4)之甲苯溶液33.33g(固體成分6.00g、甲苯27.33g)中，添加「Duranate TKA-100」(旭化成化學品股份有限公司製、六亞甲基二異氰酸酯三聚異氰酸酯化物)0.34g、甲苯15.08g，配製金屬箔與樹脂薄膜之疊層用接著劑1。接著，使用該疊層用接著劑1，如以下般以乾疊層方式來製造具有外層/外層用接著劑/鋁箔層/疊層用接著劑1/樹脂薄膜之構造的電池外裝用包裝材料。
外層：延伸聚醯胺薄膜(厚度25μm)
外層用接著劑：胺基甲酸酯系乾疊層用接著劑(東洋Morton股份有限公司製：AD502/CAT10、塗佈量3g/m2(塗佈時))
鋁箔層：鋁-鐵系合金之鋁箔(AA規格8079-O材、厚度40μm)
疊層用接著劑1：上述金屬箔與樹脂薄膜之疊層用接著劑1(塗佈量：乾燥後之厚度為2μm)
樹脂薄膜：未延伸聚丙烯薄膜(厚度30μm)
(實施例2~7、比較例1~5)
以與實施例1相同之方法，以如表3所示之成分、量來進行金屬箔與樹脂薄膜之疊層用接著劑2~12之配製，使用各自之金屬箔與樹脂薄膜之疊層用接著劑來製造電池外裝用包裝材料。
表3中，酸改質聚丙烯，係經馬來酸酐及丙烯酸辛酯改質之酸改質聚丙烯(酸價20mg/KOH)，Millionate MR-200，係日本聚胺基甲酸酯製聚合物型二苯基甲烷二異氰酸酯。
<剝離強度>
對所得之電池外殼用包裝材料，測定常態T字剝離強度、電解液溶劑浸漬後之T字剝離強度及85℃環境下之T字剝離強度。測定之條件、方法係如下述(1)~(3)所述。各試驗係以n=2來進行，取其平均值。又，結果示於表4(單位均為N/15mm)。
(1)常態T字剝離強度
使用長150mm×寬15mm之試驗片及Autograph AG-X(島津製作所股份有限公司製)，於23℃×50%RH環境下以剝離速度100mm/min剝離，測定鋁箔層與未延伸聚丙烯薄膜層間之180°剝離強度。
(2)電解液溶劑浸漬後之T字剝離強度
將長150mm×寬15mm之試驗片浸漬於電解液溶劑(碳 酸伸乙酯/碳酸二乙酯、質量比50/50)，於85℃環境下放置1日後取出，使用該試驗片，與上述(1)相同方式，測定鋁箔層與未延伸聚丙烯薄膜層間之180°剝離強度。
(3)85℃環境下之T字剝離強度
使用長150mm×寬15mm之試驗片及Autograph AG-X(島津製作所股份有限公司製)，放置於85℃環境下，於試驗片溫度成為85℃後，以剝離速度100mm/min剝離，測定鋁箔層與未延伸聚丙烯薄膜層間之180°剝離強度。
由表4之結果，可知本發明之金屬箔與樹脂薄膜之疊層用接著劑(實施例1~7)，常態T字剝離強度、電解液溶劑浸漬後之T字剝離強度及85℃環境下之T字剝離強度均為優良。
相對於此，可知使用不含(b)成分之金屬箔與樹脂薄膜之疊層用接著劑作為聚胺基甲酸酯多元醇之原料時(比較例1~4)，常態T字剝離強度、電解液溶劑浸漬後之T字剝離強度及85℃環境下之T字剝離強度均為不充分，使用以改質聚烯烴為主劑之金屬箔與樹脂薄膜之疊層用接著劑時(比較例5)，於85℃環境下之T字剝離強度不充分。
[產業上之可利用性]
本發明之金屬箔與樹脂薄膜疊層用金屬箔與樹脂薄膜之疊層用接著劑，於電解液浸漬後或高溫下亦具 有優良接著力，特別適合於鋁箔與熱熔合性樹脂薄膜之接合用。又，本發明之層合體，其耐熱性、耐電解液性優良，因而適合使用於鋰離子電池等之蓄電池之製作所用的電池外裝用包裝材料，藉由使該層合體成形，可製造耐熱性、耐電解液性優良的電池外殼。此外，藉由使用該電池外殼，可製造壽命長之安全的蓄電池。

Claims (15)

  1. 一種聚胺基甲酸酯多元醇，其係使用於聚胺基甲酸酯系接著劑之多元醇，且該多元醇為使含有：鏈狀聚烯烴多元醇(a1)及/或具有來自氫化二聚酸之構成單位與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)；一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)；及聚異氰酸酯(c)之成分加成聚合而得到。
  2. 一種金屬箔與樹脂薄膜之疊層用接著劑，其係具有：使含有：鏈狀聚烯烴多元醇(a1)及/或具有來自氫化二聚酸之構成單位與來自氫化二聚物二醇之構成單位之聚酯多元醇(a2)；一併具有飽和或不飽和之環式烴構造與2個以上之羥基的含有羥基之烴化合物(b)；及聚異氰酸酯(c)之成分加成聚合而得到之聚胺基甲酸酯多元醇(A)、與飽和脂肪族及/或飽和脂環式聚異氰酸酯(B)。
  3. 如請求項2之金屬箔與樹脂薄膜之疊層用接著劑，其中前述含有羥基之烴化合物(b)，為含有具有交聯構造之飽和脂環構造的多元醇。
  4. 如請求項2或3之金屬箔與樹脂薄膜之疊層用接著劑，其中前述含有羥基之烴化合物(b)，為雙酚化合物。
  5. 如請求項2~4中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中前述聚異氰酸酯(c)，為飽和脂環式二異 氰酸酯。
  6. 如請求項2~5中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中前述鏈狀聚烯烴多元醇(a1)，為實質上不含有不飽和烴構造之聚烯烴多元醇。
  7. 如請求項2~6中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中(b)成分，相對於(a1)及(a2)成分之總量100質量份而言，為5~100質量份，(c)成分中含有的異氰酸基數之比率，相對於(a1)、(a2)及(b)成分中含有的羥基數而言，為0.5~1.3。
  8. 如請求項2~7中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其中相對於前述聚胺基甲酸酯多元醇(A)中含有的羥基數而言，聚異氰酸酯(B)中含有的異氰酸基數之比率為1~15。
  9. 如請求項2~8中任一項之金屬箔與樹脂薄膜之疊層用接著劑，其係進一步含有溶劑(C)。
  10. 一種層合體，其係金屬箔與樹脂薄膜隔著由如請求項2~9中任一項之金屬箔與樹脂薄膜之疊層用接著劑所得到之接著劑層而層合。
  11. 如請求項10之層合體，其中前述金屬箔為鋁箔，且前述樹脂薄膜含有熱熔合性樹脂薄膜。
  12. 如請求項10或11之層合體，其中前述金屬箔之厚度為10~100μm，且前述樹脂薄膜之厚度為9~100μm。
  13. 一種電池外裝用包裝材料，其係使用如請求項10~12中任一項之層合體而得到。
  14. 一種電池外殼，其係使用如請求項13之電池外裝用包裝材料而得到。
  15. 一種電池外殼之製造方法，其係將如請求項13之電池外裝用包裝材料予以深抽拉成形或拉伸膨脹成形。
TW104117428A 2014-08-05 2015-05-29 金屬箔與樹脂薄膜之疊層用接著劑、使用該組成物之層合體、電池外裝用包裝材料及電池外殼 TWI654215B (zh)

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