TWI758446B - 電池用積層體 - Google Patents
電池用積層體 Download PDFInfo
- Publication number
- TWI758446B TWI758446B TW107110304A TW107110304A TWI758446B TW I758446 B TWI758446 B TW I758446B TW 107110304 A TW107110304 A TW 107110304A TW 107110304 A TW107110304 A TW 107110304A TW I758446 B TWI758446 B TW I758446B
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- Taiwan
- Prior art keywords
- copolymer
- ethylene
- mol
- mentioned
- propylene
- Prior art date
Links
- 229920001577 copolymer Polymers 0.000 claims abstract description 135
- 239000000853 adhesive Substances 0.000 claims abstract description 71
- 230000001070 adhesive effect Effects 0.000 claims abstract description 67
- 239000004711 α-olefin Substances 0.000 claims abstract description 66
- 239000010410 layer Substances 0.000 claims abstract description 64
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims abstract description 51
- 239000005977 Ethylene Substances 0.000 claims abstract description 51
- -1 polypropylene Polymers 0.000 claims abstract description 46
- 239000004743 Polypropylene Substances 0.000 claims abstract description 44
- 239000012790 adhesive layer Substances 0.000 claims abstract description 43
- 229910052751 metal Inorganic materials 0.000 claims abstract description 38
- 239000002184 metal Substances 0.000 claims abstract description 38
- 229920001155 polypropylene Polymers 0.000 claims abstract description 38
- 239000000463 material Substances 0.000 claims abstract description 37
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 claims abstract description 32
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 claims abstract description 32
- 229920000089 Cyclic olefin copolymer Polymers 0.000 claims abstract description 26
- 229920000642 polymer Polymers 0.000 claims abstract description 23
- 238000002844 melting Methods 0.000 claims abstract description 21
- 230000008018 melting Effects 0.000 claims abstract description 21
- VXNZUUAINFGPBY-UHFFFAOYSA-N 1-Butene Chemical compound CCC=C VXNZUUAINFGPBY-UHFFFAOYSA-N 0.000 claims abstract description 17
- IAQRGUVFOMOMEM-UHFFFAOYSA-N butene Natural products CC=CC IAQRGUVFOMOMEM-UHFFFAOYSA-N 0.000 claims abstract description 15
- 229920000098 polyolefin Polymers 0.000 claims description 23
- 150000001732 carboxylic acid derivatives Chemical class 0.000 claims description 19
- 229910052782 aluminium Inorganic materials 0.000 claims description 10
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 10
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 8
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical group [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 5
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 5
- 239000000446 fuel Substances 0.000 claims description 5
- 229910001416 lithium ion Inorganic materials 0.000 claims description 5
- 239000010936 titanium Substances 0.000 claims description 5
- 229910052742 iron Inorganic materials 0.000 claims description 4
- 239000000155 melt Substances 0.000 claims description 4
- 229910052719 titanium Inorganic materials 0.000 claims description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 3
- 229910052799 carbon Inorganic materials 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 239000010949 copper Substances 0.000 claims description 3
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 2
- 229910052804 chromium Inorganic materials 0.000 claims description 2
- 239000011651 chromium Substances 0.000 claims description 2
- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052737 gold Inorganic materials 0.000 claims description 2
- 239000010931 gold Substances 0.000 claims description 2
- 229910052738 indium Inorganic materials 0.000 claims description 2
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims description 2
- 229910052749 magnesium Inorganic materials 0.000 claims description 2
- 239000011777 magnesium Substances 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 2
- 229910052750 molybdenum Inorganic materials 0.000 claims description 2
- 239000011733 molybdenum Substances 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- 239000010703 silicon Substances 0.000 claims description 2
- 229910052718 tin Inorganic materials 0.000 claims description 2
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- 238000000034 method Methods 0.000 description 24
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- 239000004677 Nylon Substances 0.000 description 3
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- 229920001400 block copolymer Polymers 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 3
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- PUPZLCDOIYMWBV-UHFFFAOYSA-N (+/-)-1,3-Butanediol Chemical compound CC(O)CCO PUPZLCDOIYMWBV-UHFFFAOYSA-N 0.000 description 2
- FJKROLUGYXJWQN-UHFFFAOYSA-N 4-hydroxybenzoic acid Chemical compound OC(=O)C1=CC=C(O)C=C1 FJKROLUGYXJWQN-UHFFFAOYSA-N 0.000 description 2
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- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 2
- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 2
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- UHOVQNZJYSORNB-MZWXYZOWSA-N benzene-d6 Chemical compound [2H]C1=C([2H])C([2H])=C([2H])C([2H])=C1[2H] UHOVQNZJYSORNB-MZWXYZOWSA-N 0.000 description 2
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- 229920001684 low density polyethylene Polymers 0.000 description 2
- 239000004702 low-density polyethylene Substances 0.000 description 2
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 2
- 150000002739 metals Chemical class 0.000 description 2
- 239000005022 packaging material Substances 0.000 description 2
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- 229910052698 phosphorus Inorganic materials 0.000 description 2
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- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 description 2
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 2
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- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 150000003505 terpenes Chemical class 0.000 description 2
- 235000007586 terpenes Nutrition 0.000 description 2
- 239000003643 water by type Substances 0.000 description 2
- 238000001644 13C nuclear magnetic resonance spectroscopy Methods 0.000 description 1
- 229940090248 4-hydroxybenzoic acid Drugs 0.000 description 1
- RSWGJHLUYNHPMX-UHFFFAOYSA-N Abietic-Saeure Natural products C12CCC(C(C)C)=CC2=CCC2C1(C)CCCC2(C)C(O)=O RSWGJHLUYNHPMX-UHFFFAOYSA-N 0.000 description 1
- 239000004322 Butylated hydroxytoluene Substances 0.000 description 1
- NLZUEZXRPGMBCV-UHFFFAOYSA-N Butylhydroxytoluene Chemical compound CC1=CC(C(C)(C)C)=C(O)C(C(C)(C)C)=C1 NLZUEZXRPGMBCV-UHFFFAOYSA-N 0.000 description 1
- 229910001200 Ferrotitanium Inorganic materials 0.000 description 1
- JHWNWJKBPDFINM-UHFFFAOYSA-N Laurolactam Chemical compound O=C1CCCCCCCCCCCN1 JHWNWJKBPDFINM-UHFFFAOYSA-N 0.000 description 1
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- 229920000571 Nylon 11 Polymers 0.000 description 1
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- KHPCPRHQVVSZAH-HUOMCSJISA-N Rosin Natural products O(C/C=C/c1ccccc1)[C@H]1[C@H](O)[C@@H](O)[C@@H](O)[C@@H](CO)O1 KHPCPRHQVVSZAH-HUOMCSJISA-N 0.000 description 1
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- 229920002125 Sokalan® Polymers 0.000 description 1
- YIMQCDZDWXUDCA-UHFFFAOYSA-N [4-(hydroxymethyl)cyclohexyl]methanol Chemical compound OCC1CCC(CO)CC1 YIMQCDZDWXUDCA-UHFFFAOYSA-N 0.000 description 1
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- NIDNOXCRFUCAKQ-UHFFFAOYSA-N bicyclo[2.2.1]hept-5-ene-2,3-dicarboxylic acid Chemical compound C1C2C=CC1C(C(=O)O)C2C(O)=O NIDNOXCRFUCAKQ-UHFFFAOYSA-N 0.000 description 1
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- 150000001718 carbodiimides Chemical class 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
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- 125000000753 cycloalkyl group Chemical group 0.000 description 1
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- VZCYOOQTPOCHFL-UPHRSURJSA-N maleic acid Chemical compound OC(=O)\C=C/C(O)=O VZCYOOQTPOCHFL-UPHRSURJSA-N 0.000 description 1
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- RXOHFPCZGPKIRD-UHFFFAOYSA-N naphthalene-2,6-dicarboxylic acid Chemical compound C1=C(C(O)=O)C=CC2=CC(C(=O)O)=CC=C21 RXOHFPCZGPKIRD-UHFFFAOYSA-N 0.000 description 1
- SLCVBVWXLSEKPL-UHFFFAOYSA-N neopentyl glycol Chemical compound OCC(C)(C)CO SLCVBVWXLSEKPL-UHFFFAOYSA-N 0.000 description 1
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- 239000002667 nucleating agent Substances 0.000 description 1
- 239000012766 organic filler Substances 0.000 description 1
- 229910001392 phosphorus oxide Inorganic materials 0.000 description 1
- LFGREXWGYUGZLY-UHFFFAOYSA-N phosphoryl Chemical class [P]=O LFGREXWGYUGZLY-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- 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
- B32B15/01—Layered products comprising a layer of metal all layers being exclusively metallic
-
- 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
-
- 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
- B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
- B32B7/04—Interconnection of layers
- B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/04—Homopolymers or copolymers of ethene
- C08L23/08—Copolymers of ethene
- C08L23/0807—Copolymers of ethene with unsaturated hydrocarbons only containing more than three carbon atoms
- C08L23/0815—Copolymers of ethene with aliphatic 1-olefins
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/18—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms
- C08L23/20—Homopolymers or copolymers of hydrocarbons having four or more carbon atoms having four to nine carbon atoms
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/26—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers modified by chemical after-treatment
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
- C09J123/00—Adhesives based on homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Adhesives based on derivatives of such polymers
- C09J123/02—Adhesives based on homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Adhesives based on derivatives of such polymers not modified by chemical after-treatment
- C09J123/10—Homopolymers or copolymers of propene
- C09J123/14—Copolymers of propene
-
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Abstract
本發明之電池用積層體至少包含滿足下述(1)~(4)之聚丙烯系接著劑層、及金屬製基材層。
(1)上述接著劑包含40~94重量%之丙烯系共聚合體(A)、3~30重量%之含丁烯之共聚合體(B)、3~30重量%之乙烯-α-烯烴共聚合體(C)(其中,將共聚合體(A)、(B)及(C)之合計設為100重量%)
(2)上述共聚合體(A)係藉由示差掃描熱量計測得之熔點為130℃以上之聚合體,且相對於構成上述接著劑所含之所有共聚合體(A)的構造單元之總和100莫耳%,源自乙烯的構造單元之比例之總和為4~25莫耳%
(3)上述共聚合體(B)係源自乙烯的構造單元之含量未滿1莫耳%,且藉由示差掃描熱量計測得之熔點為100℃以下
(4)上述共聚合體(C)係源自乙烯的構造單元之含量為50~99莫耳%。
Description
本發明係關於一種電池用積層體,係關於一種包含新穎之接著劑層及金屬製基材層的積層體。
習知以來,聚丙烯係被廣泛用作剛性、耐熱性、透明性等優異之熱塑性成形材料。該聚丙烯係非極性材料,故而缺乏與例如乙烯-乙烯醇共聚合體等極性材料或金屬之接著性,眾所周知有為了改良接著性而以不飽和羧酸或其衍生物將聚丙烯改質之技術。又,聚丙烯係柔軟性差,故而於用作接著劑時,通常於聚丙烯中調配軟質橡膠成分。
提出有藉由如此般於聚丙烯中調配軟質橡膠成分而接著性經改善之聚丙烯系接著劑(專利文獻1及專利文獻2),進而,提出有藉由添加作為軟質橡膠成分經最適化之丙烯-乙烯共聚合體而熱歷程後之接著性亦優異之聚丙烯系接著劑(專利文獻3)。
專利文獻1:日本專利特開平9-111069號公報
專利文獻2:日本專利特開平4-300933號公報
專利文獻3:國際公開第2007/086425號
然而,使用聚丙烯系接著劑之用途亦向於高溫環境下使用之用途、例如電子資訊材料用途等擴展,對該接著劑要求於高溫環境下亦顯示出與金屬之充分之接著力。
作為具體之用途,可列舉食品包裝材或建築用材料、太陽電池之電極保護構件、鋰離子電池之包裝材或極耳(tab lead)材、燃料電池單元之密封材等。
其中,例如鋰離子電池有於聚乙烯製隔片之熔點即120℃左右斷路之機制,為了進一步提高安全性,要求於接近120℃之溫度亦維持較高之接著力。
於習知技術中,雖已達成丙烯系接著劑層之柔軟性提昇及由此所得之於常溫之接著力提昇,但未發現與其相反之高溫環境下之接著力優異之構成,必須追加使電池之溫度不會上升至樹脂之耐熱溫度以上之系統。
本發明之一實施形態在於提供一種接著性優異、尤其於高溫下接著性亦優異之電池用積層體。
本發明者為了解決上述課題而反覆進行了努力研究,結果發現藉由對丙烯系接著劑層之組成進行改進,可達成上述目的,從而完成了本發明。
即,本發明之一實施形態係關於一種電池用積層體,其至少包含滿足下述必要條件(1)~(4)之聚丙烯系接著劑層(I)、及金屬製基材層(II): (1)上述接著劑包含:40~94重量%之丙烯系共聚合體(A)、3~30重量%之含丁烯之共聚合體(B)、3~30重量%之乙烯-α-烯烴共聚合體(C)(其中,將共聚合體(A)、(B)及(C)之合計設為100重量%);(2)上述共聚合體(A)係藉由示差掃描熱量計(DSC)測得之熔點(TmA)為130℃以上之聚合體,且相對於構成上述接著劑所含之所有共聚合體(A)的構造單元之總和100莫耳%,源自乙烯的構造單元之比例之總和為4~25莫耳%;(3)上述共聚合體(B)係源自乙烯的構造單元之含量未滿1莫耳%,且藉由DSC測得之熔點(TmB)為100℃以下;(4)上述共聚合體(C)係源自乙烯的構造單元之含量為50~99莫耳%。
本發明之一實施形態之電池用積層體與金屬製基材層之常溫下之接著性優異,並且高溫環境下之接著性亦優異。因此,藉由使用該積層體,能夠安全地擴大電池之使用上限溫度,可簡化電池整體之構成。
本發明之一實施形態之電池用積層體(以下亦稱為「本積層體」)係至少包含滿足下述必要條件(1)~(4)之聚丙烯系接著劑層(I)、及金屬製基材層(II)的電池用積層體。
(1)上述接著劑包含:40~94重量%之丙烯系共聚合體(A)、3~30重量%之含丁烯之共聚合體(B)、3~30重量%之乙烯-α-烯烴共聚合體(C)(其中,將共聚合體(A)、(B)及(C)之合計設為100重量%);(2)上述共聚合體(A)係藉由示差掃描熱量計(DSC)測得之熔點(TmA)為130℃以上之聚合體,且相對於構成上述接著劑所含之所有共聚合體(A)的構造單元之總和100莫耳%,源自乙烯的構造單元之比例之總和為4~25莫耳%;(3)上述共聚合體(B)係源自乙烯的構造單元之含量未滿1莫耳%,且藉由DSC測得之熔點(TmB)為100℃以下;(4)上述共聚合體(C)係源自乙烯的構造單元之含量為50~99莫耳%。
接著劑所含之共聚合體(A)可為1種亦可為2種以上,接著劑所含之共聚合體(B)亦係可為1種亦可為2種以上,接著劑所含之共聚合體(C)亦係可為1種亦可為2種以上。
上述聚丙烯系接著劑包含40~94重量%之丙烯系共聚合體(A)、3~30重量%之含丁烯之共聚合體(B)、3~30重量%之乙烯-α-烯烴共聚合體(C)(其中,將共聚合體(A)、(B)及(C)之合計設為100重量%)。
上述聚丙烯系接著劑係以特定量包含該等共聚合體,故而由該接著劑所得之接著劑層與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異。
上述丙烯系共聚合體(A)之藉由示差掃描熱量計(DSC)測得之熔點(TmA)只要為130℃以上,則並無特別限定。
TmA較佳為130~160℃。
藉由TmA處於上述範圍,可容易地獲得高溫環境下之接著性優異之積層體。
TmA具體而言,可藉由下述實施例中記載之方法進行測定。
作為共聚合體(A),只要為具有源自丙烯的構造單元之共聚合體且TmA為130℃以上,則並無特別限制,可列舉丙烯-α-烯烴共聚合體等。再者,上述共聚合體(A)為與下述共聚合體(C)及改質聚烯烴(D)不同之聚合體。
又,亦可為於該等共聚合體之合成時,使用可與丙烯或α-烯烴共聚合之化合物而獲得之共聚合體。
作為該α-烯烴,較佳為碳數2、4~20之α-烯烴,更佳為碳數2、4~10之α-烯烴。該α-烯烴可為單獨1種,亦可為2種以上。
上述丙烯-α-烯烴共聚合體中之源自α-烯烴的構造單元之含量較佳為1~55莫耳%,更佳為2~50莫耳%,尤佳為2~45莫耳%。
就可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著劑層等方面而言,共聚合體(A)較佳為包含丙烯-乙烯-α-烯烴共聚合體。
該α-烯烴為碳數4以上之α-烯烴,更佳為碳數4~20之α-烯烴,就可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著劑層等方面而言,進而較佳為碳數4~10之α-烯烴,尤佳為1-丁烯。該α-烯烴可為單獨1種,亦可為2種以上。
上述丙烯-乙烯-α-烯烴共聚合體中之源自丙烯的構造單元之含量較佳為45~90莫耳%,更佳為50~85莫耳%,尤佳為55~80莫耳%。
上述丙烯-乙烯-α-烯烴共聚合體中之源自乙烯的構造單元之含量較佳為5~25莫耳%,更佳為10~22莫耳%,尤佳為10~20莫耳%。
上述丙烯-乙烯-α-烯烴共聚合體中之源自α-烯烴的構造單元之含量較佳為1~30莫耳%,更佳為5~28莫耳%,尤佳為10~28莫耳%。
相對於構成上述接著劑所含之所有共聚合體(A)的構造單元之總和100莫耳%,源自乙烯的構造單元之比例之總和(以下亦稱為「乙烯含量Z」)為4~25莫耳%,較佳為5~20莫耳%,更佳為5~15莫耳%。
藉由乙烯含量Z處於上述範圍,可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著劑層。
再者,於接著劑所含之共聚合體(A)為1種之情形時,上述乙烯含量Z係指該共聚合體中之源自乙烯的構造單元之比例。
即,於使用1種共聚合體(A)作為上述接著劑之原料之情形時,作為該共聚合體,使用該共聚合體中之源自乙烯的構造單元之含量為4~25莫耳%之共聚合體。該共聚合體之源自乙烯的構造單元之含量之較佳範圍為與上述乙烯含量Z相同之範圍。
又,例如於上述接著劑所含之共聚合體(A)為2種之情形時(於接著劑包含a重量%之共聚合體A-1[該共聚合體A-1中之源自乙烯的構造單元之比例:m莫耳%]、及b重量%之共聚合體A-2[該共聚合體A-2中之源自乙烯的構造單元之比例:n莫耳%]之情形時),乙烯含量Z(莫耳%)係由下述式算出之值。
乙烯含量Z=m×a/(a+b)+n×b/(a+b)
於使用2種共聚合體(A)作為上述接著劑之原料之情形時,作為各共聚合體,可使用該共聚合體中之源自乙烯的構造單元之含量為4~25莫耳%之共聚合體,亦可使用該共聚合體中之源自乙烯的構造單元之含量為4~25莫耳%以外之共聚合體。
於使用共聚合體中之源自乙烯的構造單元之含量為4~25莫耳%以外之共聚合體之情形時,只要以由上述式算出之乙烯含量Z成為4~25莫耳%之方式,調節所使用之共聚合體(A)之使用比例,或使用源自乙烯的構造單元之含量為既定值之共聚合體(A)作為所使用之共聚合體(A)即可。
再者,於上述接著劑所含之共聚合體(A)為3種以上 之情形時,乙烯含量Z亦係以與上述使用2種共聚合體(A)之情形相同之方式算出。
共聚合體(A)之熔融流動速率(MFR)[ASTM D 1238(溫度:230℃、負重:2.16kg)]較佳為0.1~50g/10分鐘,更佳為0.5~10g/10分鐘。
若MFR處於上述範圍,則可獲得柔軟性與機械強度之平衡優異、接著力更高之接著劑層。
共聚合體(A)之基於JIS K7112測得之密度較佳為0.86~0.91g/cm3,更佳為0.87~0.91g/cm3。
共聚合體(A)之分子量分佈(Mw/Mn)較佳為1.5~5.0,更佳為1.8~4.0。
分子量分佈具體而言,可藉由下述實施例中記載之方法進行測定。
作為共聚合體(A)之製造方法,並無特別限定,可藉由使用齊格勒-納塔觸媒、二茂金屬系觸媒等周知之觸媒的周知之方法進行製造。又,較佳為如滿足成形性且所獲得之積層體具有可耐使用之強度般的共聚合體,於無損本發明之效果之範圍內,立體規則性或分子量無特別限制。
亦可直接利用市售之樹脂。
相對於共聚合體(A)、(B)及(C)之合計100重量%,上述聚丙烯系接著劑中之共聚合體(A)之含量為40~94重量%,較佳為50~85重量%,更佳為55~80重量%。
藉由共聚合體(A)之含量處於上述範圍,可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著 劑層。
又,相對於上述接著劑所含之共聚合體(A)100重量%,上述丙烯-乙烯-α-烯烴共聚合體之含量較佳為10重量%以上,更佳為10~80重量%,尤佳為20~70重量%。
藉由丙烯-乙烯-α-烯烴共聚合體之含量處於上述範圍,可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著劑層。
上述含丁烯之共聚合體(B)為含有源自丁烯的構造單元,且源自乙烯的構造單元之含量未滿1莫耳%之共聚合體,較佳為丙烯-丁烯共聚合體。再者,上述共聚合體(B)為與下述改質聚烯烴(D)不同之聚合體。
共聚合體(B)之源自丁烯的構造單元之含量較佳為10~30莫耳%,更佳為12~28莫耳%。
共聚合體(B)之源自丙烯的構造單元之含量較佳為70~90莫耳%,更佳為72~88莫耳%。
共聚合體(B)之藉由DSC測得之熔點(TmB)為100℃以下,更佳為60~100℃。
藉由TmB處於上述範圍,可容易地獲得常溫下及高溫環境下之接著性平衡良好且優異之積層體。
TmB具體而言,可藉由下述實施例中記載之方法進行測定。
共聚合體(B)之MFR[ASTM D 1238(溫度:230℃、負重:2.16kg)]較佳為0.1~50g/10分鐘,更佳為0.5~10g/10分鐘。
若MFR處於上述範圍,則可獲得柔軟性與機械強度之平衡優異、接著力更高之接著劑層。
共聚合體(B)之基於JIS K7112測得之密度較佳為0.86~0.90g/cm3,更佳為0.87~0.90g/cm3。
共聚合體(B)之分子量分佈(Mw/Mn)較佳為1.5~5.0,更佳為1.8~4.0。
作為共聚合體(B)之製造方法,並無特別限定,可藉由使用齊格勒-納塔觸媒、二茂金屬系觸媒等周知之觸媒的周知之方法進行製造。又,較佳為如滿足成形性且所獲得之積層體具有可耐使用之強度般的共聚合體,於無損本發明之效果之範圍內,立體規則性或分子量無特別限制。
亦可直接利用市售之樹脂。
相對於共聚合體(A)、(B)及(C)之合計100重量%,上述聚丙烯系接著劑中之共聚合體(B)之含量為3~30重量%,較佳為5~30重量%,更佳為5~25重量%。
藉由共聚合體(B)之含量處於上述範圍,可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著劑層。
上述乙烯-α-烯烴共聚合體(C)只要為源自乙烯的構造單元之含量為50~99莫耳%之共聚合體,則並無特別限定。再者,上述共聚合體(C)為與下述改質聚烯烴(D)不同之聚合體。
共聚合體(C)之源自乙烯的構造單元之含量較佳為60~95莫耳 %,更佳為70~90莫耳%。
作為上述α-烯烴,較佳為碳數3~20之α-烯烴,更佳為碳數3~10之α-烯烴,尤佳為丙烯或丁烯。共聚合體(C)之源自α-烯烴的構造單元之含量較佳為1~50莫耳%,更佳為5~40莫耳%,尤佳為10~30莫耳%。
上述α-烯烴可為單獨1種,亦可為2種以上。
共聚合體(C)之MFR[ASTM D 1238(溫度:230℃、負重:2.16kg)]較佳為0.1~70g/10分鐘,更佳為0.5~20g/10分鐘。
若MFR處於上述範圍,則可獲得柔軟性與機械強度之平衡優異、接著力更高之接著劑層。
共聚合體(C)之基於JIS K7112測得之密度較佳為0.85~0.90g/cm3,更佳為0.86~0.89g/cm3。
共聚合體(C)之分子量分佈(Mw/Mn)較佳為1.5~5.0,更佳為1.8~4.0。
作為共聚合體(C)之製造方法,並無特別限定,可藉由使用齊格勒-納塔觸媒、二茂金屬系觸媒等周知之觸媒的周知之方法進行製造。又,較佳為如滿足成形性且所獲得之積層體具有可耐使用之強度般的共聚合體,於無損本發明之效果之範圍內,立體規則性或分子量無特別限制。
亦可直接利用市售之樹脂。
相對於共聚合體(A)、(B)及(C)之合計100重量%,上述聚丙烯系接著劑中之共聚合體(C)之含量為3~30重量%,較佳為5~28重量%,更佳為10~25重量%。
藉由共聚合體(C)之含量處於上述範圍,可容易地獲得與金屬製基材層之常溫下及高溫環境下之接著性平衡良好且優異之接著劑層。
[改質聚烯烴(D)]
就可容易地獲得所得之接著劑層與金屬製基材層之接著性優異之積層體等方面而言,上述聚丙烯系接著劑較佳為包含經不飽和羧酸及/或其衍生物改質之改質聚烯烴(D)。
該接著劑所含之改質聚烯烴(D)可為1種亦可為2種以上。
改質聚烯烴(D)係以不飽和羧酸及/或其衍生物將聚烯烴(以下亦稱為「主幹聚合體」。該主幹聚合體亦為改質聚烯烴(D)中除源自上述不飽和羧酸及其衍生物的構造單元以外之構造單元)改質而獲得,含有源自該不飽和羧酸及/或其衍生物的構造單元。
於改質聚烯烴(D)中,亦可使用2種以上之主幹聚合體。
作為上述主幹聚合體,例如可列舉聚丙烯(d1)、乙烯-丙烯-α-烯烴共聚合體(d2)及乙烯-α-烯烴共聚合體(d3)。
聚丙烯(d1)例如為丙烯之均聚物及/或丙烯-α-烯烴共聚合體。又,亦可含有若干種不同之同排聚丙烯。
作為該α-烯烴,並無特別限定,可較佳地列舉乙烯及碳數4~20之α-烯烴,該等α-烯烴可為單獨1種亦可為2種以上。較佳之α-烯烴為乙烯及碳數4~10之α-烯烴,其中更佳為乙烯及碳數4~8之α-烯烴。此處,丙烯-α-烯烴共聚合體中之自丙烯衍生的構造單元之含量為至少50莫耳%以上且未滿100莫耳%。
聚丙烯(d1)之製造方法並無特別限定,可列舉使用齊格勒-納塔觸媒、二茂金屬系觸媒等周知之觸媒的周知之方法。
作為聚丙烯(d1),較佳為結晶性之聚合體,於共聚合體之情形時,可為無規共聚合體,亦可為嵌段共聚合體。又,較佳為如滿足成形性且所獲得之積層體具有可耐使用之強度般的共聚合體,於無損本發明之效果之範圍內,立體規則性或分子量無特別限制。
亦可直接利用市售之樹脂。
乙烯-丙烯-α-烯烴共聚合體(d2)例如含有45~89莫耳%之源自丙烯的構造單元、10~25莫耳%之源自乙烯的構造單元、1~30莫耳%之源自碳數4~20之α-烯烴的構造單元。
作為該α-烯烴,較佳為碳數4~10之α-烯烴。該α-烯烴可為單獨1種亦可為2種以上。
於共聚合體(d2)中,源自乙烯的構造單元之含量較佳為10~22莫耳%,更佳為10~20莫耳%,源自丙烯的構造單元之含量較佳為50~85莫耳%,更佳為55~80莫耳%,源自α-烯烴的構造單元之含量較佳為5~28莫耳%,更佳為10~28莫耳%。
共聚合體(d2)之製造方法並無特別限定,可列舉使用齊格勒-納塔觸媒、二茂金屬系觸媒等周知之觸媒的周知之方法。
作為共聚合體(d2),可為無規共聚合體,亦可為嵌段共聚合體。又,較佳為如滿足成形性且所獲得之積層體具有可耐使用之強度般的共聚合體,於無損本發明之效果之範圍內,立體規則性或分子量無特別限制。
亦可直接利用市售之樹脂。
乙烯-α-烯烴共聚合體(d3)較佳為含有50~99莫耳%之源自乙烯的構造單元、1~50莫耳%之源自碳數3~20之α-烯烴 的構造單元。
作為該α-烯烴,更適宜為碳數3~10之α-烯烴。該α-烯烴可為單獨1種亦可為2種以上。
於共聚合體(d3)中,源自乙烯的構造單元之含量更佳為55~98莫耳%,尤佳為60~95莫耳%,源自α-烯烴的構造單元之含量更佳為2~45莫耳%,尤佳為5~40莫耳%。
作為共聚合體(d3)之製造方法,並無特別限定,可列舉使用齊格勒-納塔觸媒、二茂金屬系觸媒等周知之觸媒的周知之方法。
作為共聚合體(d3),較佳為結晶性之聚合體,可為無規共聚合體,亦可為嵌段共聚合體。又,較佳為如成形性優異且所獲得之積層體具有可耐使用之強度般的共聚合體,於無損本發明之效果之範圍內,立體規則性或分子量無特別限制。
亦可直接利用市售之樹脂。
上述主幹聚合體中之源自丙烯的構造單元之含量較佳為90~100莫耳%,更佳為95~100莫耳%。
若上述主幹聚合體中之源自丙烯的構造單元之含量處於上述範圍,則可容易地獲得耐熱性優異之接著劑層。
作為上述不飽和羧酸及/或其衍生物,可列舉:具有1個以上之羧酸基的不飽和化合物、具有羧酸基的不飽和化合物與烷基醇之酯、具有1個以上之羧酸酐基的不飽和化合物等。
作為不飽和基,可列舉乙烯基、伸乙烯基、不飽和環狀烴基等。
作為上述不飽和羧酸及/或其衍生物,較適宜為不飽和二羧酸或其酸酐,尤佳為馬來酸、耐地酸(nadic acid)或該等之酸酐。
不飽和羧酸及/或其衍生物可單獨使用1種,亦可使用2種以上。
相對於上述主幹聚合體100重量份,改質聚烯烴(D)中之源自不飽和羧酸及其衍生物的構造單元之量較佳為0.01~5重量份,更佳為0.05~3.5重量份。
若源自不飽和羧酸及其衍生物的構造單元之量處於上述範圍,則可容易地獲得成形性與接著性之平衡優異之接著劑層。
作為對上述主幹聚合體進行改質之方法,並無特別限制,較佳為使用主幹聚合體及不飽和羧酸及/或其衍生物的接枝聚合。
關於使不飽和羧酸及/或其衍生物接枝之方法,並無特別限定,可採用溶液法、熔融混練法等習知公知之接枝聚合法。例如可列舉:將上述主幹聚合體熔融,並於其中添加不飽和羧酸及/或其衍生物進行接枝反應之方法;或使上述主幹聚合體溶解於溶劑中而製成溶液,並於其中添加不飽和羧酸及/或其衍生物進行接枝反應之方法等。
又,改質聚烯烴(D)亦可於使少量之不飽和羧酸及/或其衍生物接枝後,進而以二胺、碳二醯亞胺等對源自不飽和羧酸及/或其衍生物之構造進行修飾。
相對於共聚合體(A)、(B)及(C)之合計100重量份,上述聚丙烯系接著劑中之改質聚烯烴(D)之含量較佳為0.1~15重量份,更佳為1~13重量份,尤佳為2~12重量份。
藉由改質聚烯烴(D)之含量處於上述範圍,可容易地獲得與金屬製基材層之接著性優異之接著劑層。
於上述接著劑中,亦可於無損本發明之效果之範圍內,以調整剛性等目的而適當含有丙烯均聚物、上述聚合體(A)~(D)以外之共聚合體、或苯乙烯系彈性體等。又,亦可以調整成形性等目的而適當含有低密度聚乙烯(LDPE)或線性低密度聚乙烯(LLDPE)等。
此外,亦可視需要含有黏著賦予劑、抗氧化劑、紫外線吸收劑、中和劑、成核劑、光穩定劑、抗靜電劑、抗黏連劑、潤滑劑、臭氣吸附劑、抗菌劑、顏料、無機質及有機質之填充劑、各種合成樹脂等公知之添加劑。
較佳為於上述接著劑中,尤其以賦予黏著性之目的而調配所謂黏著賦予劑。作為該黏著賦予劑,例如可列舉松香衍生物、萜烯樹脂、石油樹脂及該等之氫化物,該等之中,較佳為氫化萜烯樹脂、氫化石油樹脂。
相對於接著劑100重量%,黏著賦予劑之調配量較佳為2~30重量%。
關於上述接著劑,可列舉:對於上述共聚合體(A)~(C)、以及視需要之上述改質聚烯烴(D)及上述其他成分,藉由各種公知之方法例如亨舍爾混合機、V型混合器、帶式混合器、滾筒混合器等進行混合之方法,利用單軸擠出機、雙軸擠出機、捏合機、班布里混合機等進行熔融混練之方法。再者,亦可視需要將藉由上述混合所得之混合物或藉由熔融混練所得之熔融混練物造粒或粉碎。
上述接著劑之基於ASTM D 1238(溫度:230℃、負 重:2.16kg)之MFR並無特別限定,就成為接著劑層(I)之成形性優異之接著劑等方面而言,較佳為0.1~100g/10分鐘,更佳為0.1~30g/10分鐘。
上述接著劑之基於JIS K7112測得之密度較佳為0.85~0.91g/cm3,更佳為0.86~0.90g/cm3。
本積層體只要具有聚丙烯系接著劑層(I)及金屬製基材層(II),則並無特別限制,亦可根據所需之用途具有其他層。
本積層體就可進一步發揮本發明之效果等方面而言,較佳為上述接著劑層(I)與金屬製基材層(II)接觸。
再者,聚丙烯系接著劑層(I)係使用上述聚丙烯系接著劑而獲得之層,較佳為包含聚丙烯系接著劑之層。
本積層體係用於電池,作為該電池,較佳為太陽電池、鋰離子電池及燃料電池。
作為本積層體之具體用途,可列舉:太陽電池之密封材(玻璃與電池單元間之密封材)或鋁框架之固定材、將色素增感太陽電池之活性物質彼此固定之黏合劑或將透明電極與活性物質固定之接著層、鋰離子電池之包裝材(鋁與密封劑PP之間之接著層)、極耳材(鋁或銅與密封劑PP之間之接著層)、燃料電池單元之隔片(鈦或不鏽鋼等)彼此之接著層、燃料電池單元之隔片與各種襯墊之間之接著層等。
本積層體之厚度並無特別限制,只要根據所需之用途適當選擇即可,較佳為5μm~100mm,更佳為10μm~50mm。
本積層體中之接著劑層(I)與金屬製基材層(II)之接著力(180°剝離法,拉伸試驗機,23℃,十字頭速度:200mm/min)較佳為50~500N/20mm,更佳為100~300N/20mm。
該接著力處於上述範圍之積層體可謂常溫下之接著性優異之積層體。
本積層體中之接著劑層(I)與金屬製基材層(II)之接著力(180°剝離法,拉伸試驗機,110℃,十字頭速度:200mm/min)較佳為50~500N/20mm,更佳為60~300N/20mm。
該接著力處於上述範圍之積層體可謂高溫環境下之接著性優異之積層體。
本積層體可藉由將上述聚丙烯系接著劑熔融,於熔融狀態下與金屬製基材層(II)進行積層而製造。又,亦可藉由以下方式而製造積層體:將熔融狀態之上述聚丙烯系接著劑塗佈於金屬薄膜、金屬板、金屬管等金屬製基材層(II)之表面上之方法;或由上述聚丙烯系接著劑預先形成經成形為薄膜或片材狀等之接著劑層,於使該接著劑層與金屬製基材層(II)接觸之狀態下使該接著劑層熔融。作為此時供給使接著劑層熔融所需之熱能的手段,可列舉公知之手段,例如可列舉熱壓、燃燒、高頻加熱、雷射加熱。
上述聚丙烯系接著劑層(I)之厚度並無特別限制,只要根據所需之用途適當選擇即可,就可容易地獲得具有充分之接著性的電池用積層體等方面而言,較佳為3~500μm,更佳為10~400μm。
上述金屬製基材層(II)包含選自金、銅、鐵、鉻、鋅、鈷、鋁、鈦、錫、銦、鎂、鉬、錳及矽所構成群組中之至少1種元素。
上述金屬製基材層(II)可列舉:包含該等中之1種元素的金屬板或金屬箔、包含含有該等中之2種以上之元素之合金的板或箔等。
作為上述元素,較佳為鋁、鐵、不鏽鋼、鈦等。
上述金屬製基材層(II)之厚度並無特別限制,只要根據所需之用途適當選擇即可,較佳為2μm~100mm,更佳為5μm~50mm。
作為上述其他層,可列舉無機物層、熱塑性樹脂層、阻氣層等。
作為上述無機物層,較佳為將金屬製基材層(II)之表面被覆之層。
作為該無機物層,只要無損本發明之效果,則並無特別限制,例如可列舉:包含含有1種以上之作為構成上述金屬製基材層(II)之元素而列舉的金屬元素的氧化物、氮化物、氮氧化物、硫化物、磷化物、磷氧化物、磷氮化物及磷氮氧化物等無機化合物的層。
作為該金屬元素,較佳為鋁、鐵、不鏽鋼、鈦等。
作為上述熱塑性樹脂層,可列舉下述阻隔層以外之各種包含熱塑性樹脂的層,例如包含聚烯烴、聚酯、聚碳酸酯、聚丙烯酸、聚胺基甲酸酯的層,具體而言,可列舉包含未經接枝改質之聚丙烯的層、包含熱塑性丙烯系彈性體的層、包含聚酯系樹脂的層等。
上述包含聚酯系樹脂的層亦可為調整形成該層的原 料之組成而賦予有印刷性或易接著性、蒸鍍性的層。
作為上述聚酯系樹脂,具體而言可列舉:使間苯二甲酸、鄰苯二甲酸、對苯二甲酸、2,6-萘二羧酸、己二酸、癸二酸等二羧酸或羥基羧酸(例如對羥基苯甲酸)與乙二醇、丙二醇、丁二醇、二乙二醇、1,4-環己烷二甲醇、新戊二醇等脂肪族二醇進行聚縮合而獲得之樹脂等。
上述二羧酸、羥基羧酸及脂肪族二醇分別可使用1種或2種以上。
作為上述聚酯系樹脂之代表例,可列舉PET、聚2,6-萘二甲酸乙二酯(PEN)、聚對苯二甲酸丁二酯(PBT)。又,該樹脂除均聚物以外,亦可為含有30莫耳%以下之第三成分之共聚物。
作為上述阻氣層,並無特別限制,可列舉具有阻氣性的各種公知之樹脂,例如使用乙烯-乙酸乙烯酯共聚合體皂化物(EVOH)、聚醯胺樹脂(PA)、聚偏二氯乙烯系樹脂、聚丙烯腈等阻隔性優異之樹脂的阻隔樹脂層。
作為上述EVOH,較佳可列舉將乙烯含有率15~70莫耳%之乙烯-乙酸乙烯酯共聚合體皂化而獲得之皂化度90~100%之聚合體。
作為上述PA,例如可列舉尼龍6、尼龍66、尼龍610、尼龍12、尼龍11、MXD尼龍、非晶形尼龍、共聚合尼龍。
本積層體作為具有上述其他層之情形時之構成例,並無特別限制,可列舉:基材層(II)/接著劑層(I)/阻隔層;基材層(II)/接著劑層(I)/阻隔層/接著劑層(I)/基材層(II);基材層(II)/接著劑層(I)/阻隔層/接著劑層(I)/熱塑性樹脂層等積層體。
以下,列舉實施例及比較例更具體地對本發明進行說明,但本發明只要不超出其宗旨,則並不受該等實施例之任何限制。
按照ASTM D 1238,於230℃、2.16kg負重之下測定MFR。
依據JIS K7112測定密度。
藉由下述方法進行示差掃描熱測定,藉此測定使用作為下述接著劑之原料的共聚合體之Tm。
將5mg左右之試樣裝入至專用鋁鍋中,使用PerkinElmer(股)製造之DSCPyris1或DSC7,以320℃/min自30℃升溫至200℃,於200℃保持5分鐘後,以10℃/min自200℃降溫至30℃,於30℃進而保持5分鐘,繼而以10℃/min進行升溫,根據此時之吸熱曲線求出熔點。
於在測定時檢測出數個峰之情形時,將於最高溫側檢測出之峰溫度定義為熔點(Tm)。
使用作為下述接著劑之原料的共聚合體中之源自丙烯的構造單元、源自乙烯的構造單元及源自α-烯烴的構造單元之含量係藉由 13C-NMR利用以下之裝置及條件測得。
源自丙烯、乙烯及α-烯烴的構造單元之含量之定量化係使用日本電子(股)製造之JECX400P型核磁共振裝置,使用氘代鄰二氯苯/氘苯(80/20容量%)混合溶劑作為溶劑,於將試樣濃度設為60mg/0.6mL、將測定溫度設為120℃、將觀察核設為13C(100MHz)、將序列設為單脈衝質子解耦、將脈衝寬度設為4.62μ秒(45°脈衝)、將重複時間設為5.5秒、將累計次數設為8000次、將29.73ppm設為化學位移之基準值的條件下測得。
根據下述接著劑所使用之共聚合體(A)之使用量、及上述聚合物之組成中測得之該共聚合體(A)中之源自乙烯的構造單元之含量,基於上述式,算出相對於構成接著劑所含之共聚合體(A)的構造單元之總和100莫耳%之源自乙烯的構造單元之比例之總和(乙烯含量Z)。
源自不飽和羧酸及其衍生物的構造單元之量(接枝量)係藉由紅外線吸收分析裝置測定源自該構造單元之峰(於使用馬來酸酐之情形時為1790cm-1)之強度,使用預先製成之校準曲線進行定量。
使用作為下述接著劑之原料的共聚合體之Mw及Mw/Mn係使用將2根東曹(股)製造之TSKgelGMH6-HT及2根 TSKgelGMH6-HTL(管柱尺寸均為直徑7.5mm、長度300mm)串列連接而成之管柱,使用液相層析儀(Waters公司製造,Alliance/GPC2000型)而測得。流動相介質係使用含有0.025重量%之抗氧化劑(丁基羥基甲苯,武田藥品工業(股)製造)之鄰二氯苯,於將試樣濃度設為0.15%(V/W)、將流速設為1.0mL/分鐘、將溫度設為140℃之條件下進行測定。關於標準聚苯乙烯,於分子量為500~20,600,000之情形時係使用東曹(股)製造。
對於所獲得之層析圖,使用Waters公司製造之資料處理軟體Empower2,藉由公知之方法利用使用標準聚苯乙烯樣品的校準曲線進行解析,藉此算出數量平均分子量(Mn)、Mw及Mw/Mn。
將實施例及比較例中使用之聚烯烴示於以下。再者,只要未特別說明,則該等聚烯烴均係按照常規方法進行聚合而製備。
‧PP:無規聚丙烯
(MFR=7.0g/10分鐘、密度=0.90g/cm3、乙烯含量=3mol%、丙烯含量=96mol%、丁烯含量=1mol%、熔點=140℃)
‧PBER:乙烯-丙烯-α-烯烴共聚合體
(MFR=7.0g/10分鐘、密度=0.87g/cm3、乙烯含量=13mol%、丙烯含量=68mol%、丁烯含量=19mol%、熔點=140℃、Mw/Mn=2.1)
‧PBR-1:丙烯-丁烯無規共聚合體(MFR=7.0g/10分鐘、密度=0.88g/cm3、丙烯含量=74mol%、丁烯含量=26mol%、熔點=75℃、Mw/Mn=2.1)
‧PBR-2:丙烯-丁烯無規共聚合體
(MFR=7.0g/10分鐘、密度=0.89g/cm3、丙烯含量=85mol%、丁烯含量=15mol%、熔點=98℃、Mw/Mn=2.2)
‧EPR:乙烯-α-烯烴共聚合體
(MFR=8.0g/10分鐘、密度=0.87g/cm3、乙烯含量=80mol%、丙烯含量=20mol%、Mw/Mn=2.1)
‧EBR:乙烯-α-烯烴共聚合體
(MFR=8.0g/10分鐘、密度=0.87g/cm3、乙烯含量=85mol%、丁烯含量=15mol%、Mw/Mn=2.1)
‧改質PP:改質同排均聚丙烯(MFR=100g/10分鐘、密度0.90g/cm3、馬來酸酐接枝量=3.0wt%)
使用單軸擠出機將PP(45重量%)、PBER(20重量%)、PBR-1(10重量%)、EPR(20重量%)、及改質PP(5重量%)於230℃進行熔融混練,獲得丙烯系接著劑。所獲得之丙烯系接著劑之MFR為8.2g/10 分鐘,密度為0.89g/cm3。
利用附帶T字模之擠出成形機,由實施例1中所獲得之接著劑而成形厚度50μm之薄膜。以厚度300μm之2片鋁箔夾持所獲得之薄膜,利用熱封機於160℃、0.1MPa之條件下進行5秒鐘熱密封。將所獲得之多層薄膜切成20mm寬度,使用拉伸試驗機,藉由180°剝離法於室溫23℃下或110℃下測定鋁箔與接著劑層之接著力(單位:N/20mm)。十字頭速度係設為200mm/min。將結果示於表1。
按照表1所示之調配配方製備丙烯系接著劑,除此以外,藉由與實施例1相同之方法製備接著劑,並使用所獲得之接著劑製造積層體,測定其接著力。將結果示於表1。
Claims (11)
- 一種電池用積層體,其至少包含滿足下述必要條件(1)~(5)之聚丙烯系接著劑層(I)、及金屬製基材層(II):(1)上述接著劑包含丙烯系共聚合體(A)、含丁烯之共聚合體(B)及乙烯-α-烯烴共聚合體(C),且相對於該等之合計100重量%,包含40~94重量%之上述共聚合體(A)、3~30重量%之上述共聚合體(B)、3~30重量%之上述共聚合體(C);(2)上述共聚合體(A)係藉由示差掃描熱量計測得之熔點為130℃以上之聚合體,且相對於構成上述接著劑所含之所有共聚合體(A)的構造單元之總和100莫耳%,源自乙烯的構造單元之比例之總和為4~25莫耳%;(3)上述共聚合體(B)係源自乙烯的構造單元之含量未滿1莫耳%,且藉由示差掃描熱量計測得之熔點為100℃以下;(4)上述共聚合體(C)係源自乙烯的構造單元之含量為50~99莫耳%;(5)相對於上述共聚合體(A)、(B)及(C)之合計100重量份,上述聚丙烯系接著劑包含經選自不飽和羧酸及其衍生物中之至少1種改質之改質聚烯烴(D)0.1~15重量份。
- 如請求項1之電池用積層體,其中,相對於上述接著劑所含之共聚合體(A)100重量%,上述共聚合體(A)包含10重量%以上之丙烯-乙烯-α-烯烴共聚合體,該α-烯烴之碳數為4以上。
- 如請求項2之電池用積層體,其中,上述丙烯-乙烯-α-烯烴共 聚合體為丙烯-乙烯-1-丁烯共聚合體。
- 如請求項1之電池用積層體,其中,相對於除源自上述不飽和羧酸及其衍生物的構造單元以外的構造單元100重量份,上述改質聚烯烴(D)含有0.01~5重量份之源自不飽和羧酸及其衍生物的構造單元,進而,於改質聚烯烴(D)中,除源自上述不飽和羧酸及其衍生物的構造單元以外的構造單元中之源自丙烯的構造單元之含量為90~100莫耳%。
- 如請求項1之電池用積層體,其中,上述共聚合體(A)為丙烯-α-烯烴共聚合體,該α-烯烴之碳數為2、4~20,上述共聚合體(A)係源自該α-烯烴的構造單元之含量為1~55莫耳%,且依據ASTM D 1238以溫度230℃、負重2.16kg測得之熔體流動速率為0.1~50g/10分鐘。
- 如請求項1之電池用積層體,其中,上述共聚合體(B)含有10~30莫耳%之源自丁烯的構造單元、90~70莫耳%之源自丙烯的構造單元,且依據ASTM D 1238以溫度230℃、負重2.16kg測得之熔體流動速率為0.1~50g/10分鐘。
- 如請求項1之電池用積層體,其中,上述共聚合體(C)之依據ASTM D 1238以溫度230℃、負重2.16kg測得之熔體流動速率為0.1~70g/10分鐘。
- 如請求項1之電池用積層體,其中,上述電池為太陽電池。
- 如請求項1之電池用積層體,其中,上述電池為鋰離子電池。
- 如請求項1之電池用積層體,其中,上述電池為燃料電池。
- 如請求項1之電池用積層體,其中,上述金屬製基材層(II)包含選自金、銅、鐵、鉻、鋅、鈷、鋁、鈦、錫、銦、鎂、鉬、錳及矽所構成群組中之至少1種元素。
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