JP4777343B2 - プロピレン系接着剤用重合体組成物およびその積層体 - Google Patents
プロピレン系接着剤用重合体組成物およびその積層体 Download PDFInfo
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- JP4777343B2 JP4777343B2 JP2007510461A JP2007510461A JP4777343B2 JP 4777343 B2 JP4777343 B2 JP 4777343B2 JP 2007510461 A JP2007510461 A JP 2007510461A JP 2007510461 A JP2007510461 A JP 2007510461A JP 4777343 B2 JP4777343 B2 JP 4777343B2
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- ethylene
- olefin
- propylene
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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
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
-
- 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
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F255/00—Macromolecular compounds obtained by polymerising monomers on to polymers of hydrocarbons as defined in group C08F10/00
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F255/00—Macromolecular compounds obtained by polymerising monomers on to polymers of hydrocarbons as defined in group C08F10/00
- C08F255/02—Macromolecular compounds obtained by polymerising monomers on to polymers of hydrocarbons as defined in group C08F10/00 on to polymers of olefins having two or three carbon atoms
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F297/00—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer
- C08F297/06—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the coordination type
- C08F297/08—Macromolecular compounds obtained by successively polymerising different monomer systems using a catalyst of the ionic or coordination type without deactivating the intermediate polymer using a catalyst of the coordination type polymerising mono-olefins
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
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- C08L51/06—Compositions of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers grafted on to homopolymers or copolymers of aliphatic hydrocarbons containing only one carbon-to-carbon double bond
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L53/00—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
-
- 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
- C09J151/00—Adhesives based on graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers
- C09J151/06—Adhesives based on graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers grafted on to homopolymers or copolymers of aliphatic hydrocarbons containing only one carbon-to-carbon double bond
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- 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
- C09J153/00—Adhesives based on block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
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- 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
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- 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
- C08L2666/00—Composition of polymers characterized by a further compound in the blend, being organic macromolecular compounds, natural resins, waxes or and bituminous materials, non-macromolecular organic substances, inorganic substances or characterized by their function in the composition
- C08L2666/02—Organic macromolecular compounds, natural resins, waxes or and bituminous materials
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2666/00—Composition of polymers characterized by a further compound in the blend, being organic macromolecular compounds, natural resins, waxes or and bituminous materials, non-macromolecular organic substances, inorganic substances or characterized by their function in the composition
- C08L2666/02—Organic macromolecular compounds, natural resins, waxes or and bituminous materials
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Description
すなわち、本発明は、(i)グラフト変性ポリプロピレン(A)を40〜92重量%、
(ii)230℃、2.16kg荷重におけるメルトフロ−レ−ト(MFR)が0.01〜10g/10分で、かつ、密度が0.940g/cm3以下のエチレン・α−オレフィ
ン共重合体(B)を5〜30重量%、および
(iii)オレフィン結晶セグメントとエチレン・α−オレフィンセグメントとからなるブロック共重合体(C)を3〜30重量%(但し、(A)、(B)および(C)の合計は100重量%)含み、グラフト変性ポリプロピレン(A)は、不飽和カルボン酸および/またはその誘導体でグラフト変性されたポリプロピレンであり、不飽和カルボン酸またはその誘導体の残基を、グラフト変性ポリプロピレン(A)100重量%に対して、0.01〜5重量%含有し、上記ブロック共重合体(C)がオレフィン結晶−エチレン・ブチレン−オレフィン結晶ブロック共重合体であるプロピレン系接着剤用重合体組成物(D)、並びに、前記のプロピレン系接着剤用重合体組成物を含む層を少なくとも1層有する積層体である。
グラフト変性ポリプロピレン(A)を40〜92重量%、230℃、2.16kg荷重におけるメルトフロ−レ−ト(MFR)が0.01〜10g/10分で、かつ、密度が0.940g/cm3以下のエチレン・α−オレフィン共重合体(B)を5〜30重量%、オレフィン結晶セグメントとエチレン・α−オレフィンセグメントとからなるブロック共重合体(C)を3〜30重量%(但し、(A)、(B)および(C)の合計は100重量%)含むプロピレン系接着剤用重合体組成物(D)の各成分について、以下に説明する。
本発明で用いられるグラフト変性ポリプロピレン(A)は、不飽和カルボン酸および/またはその誘導体でグラフト変性されたポリプロピレンである。
グラフト変性に用いられるポリプロピレンは、プロピレンの単独重合体および/またはプロピレン・α−オレフィン共重合体である。プロピレン・α−オレフィン共重合体のα−オレフィンとしては、エチレンおよび/または炭素数4〜20のα−オレフィンが挙げられ、これらのα−オレフィンは、1種単独でも2種以上使用してもよい。本発明において好ましいα−オレフィンは、炭素数4〜10のα−オレフィンであり、中でも特に炭素数4〜8のα−オレフィンが好適に使用できる。
本発明で用いられるグラフト変性ポリプロピレン(A)のASTM D1238に準じ、230℃、2.16kg荷重の下に測定されたメルトフロ−レ−ト(MFR)は、通常0.01〜400g/10分、好ましくは0.1〜90g/10分である。MFR値がこの範囲にあるグラフト変性ポリプロピレン(A)は、流動性に優れるため、大型品も成形でき、かつ高速成形もできるようなプロピレン系接着剤用重合体組成物(D)を得ることが可能となる。
エチレン・α−オレフィン共重合体(B)
本発明で用いられるエチレン・α−オレフィン共重合体(B)は、メルトフロ−レ−ト(ASTM D1238に準じて230℃、2.16kg荷重で測定した値)が0.01〜10g/10分であり、そして密度が0.940g/cm3以下のエチレン・α−オレフィン共重合体である。エチレン・α−オレフィン共重合体(B)は、好ましくはエチレンと炭素数3〜20のα−オレフィンとのランダム共重合体である。これらのうち、炭素数3または4のα−オレフィンが好ましい。すなわち、エチレン・α−オレフィン共重合体(B)としては、エチレン・プロピレンランダム共重合体が好ましい。
上記エチレン・α−オレフィン共重合体(B)のメルトフロ−レ−トは、好ましくは0.01〜10g/10分であり、密度は、好ましくは0.85〜0.90g/cm3である。
さらに、本発明で使用されるエチレン・α−オレフィン共重合体(B)は、上記条件を満足する限り、少量の無水マレイン酸などをグラフトしたものであってもよい。また、上記条件を満足する限り、少量の無水マレイン酸などをグラフトした後、グラフトモノマ−をさらにジアミンなどで修飾したものであってもよい。なお、グラフトされた重合体、ジアミンなどで修飾された重合体が上記の条件を外れたものであっても、エチレン・α−オレフィン共重合体(B)の全体として上記条件を満足していればよい。
本発明で用いられるオレフィン結晶セグメントとエチレン・α−オレフィンセグメントとからなるブロック共重合体(C)は、グラフト変性ポリプロピレン(A)相とエチレン・α−オレフィン共重合体(B)相との相溶性を向上し、マトリックスレベルでの相間剥離を低減させる効果を奏するものが選択される。基本的には、オレフィン結晶セグメントは、グラフト変性ポリプロピレン(A)相との相溶性に、エチレン・α−オレフィンセグメントは、エチレン・α−オレフィン共重合体(B)相との相溶性に寄与している。その結果、接着剤層の白化防止に優れた効果を得ることができる。
プロピレン系接着剤用重合体組成物(D)
本発明のプロピレン系接着剤用重合体組成物(D)は、上述のグラフト変性ポリプロピレン(A)、エチレン・α−オレフィン共重合体(B)、およびオレフィン結晶−エチレン・α−オレフィンブロック共重合体(C)を含有していることを特徴とするプロピレン系接着剤用重合体組成物(D)である。
また、本発明のプロピレン系接着剤用重合体組成物(D)には、本発明の目的を損なわない範囲で、公知のプロセス安定剤、耐熱安定剤、耐熱老化剤、フィラ−などを添加することも可能である。本発明においては、特に、粘着性を付与する目的でいわゆる粘着付与剤を配合することが好ましい。粘着性を付与する物質としては、例えば、ロジン誘導体、テルペン樹脂、石油樹脂、およびそれらの水素化物を挙げることができ、これらの中では、水素化テルペン樹脂、水素化石油樹脂が好ましい。粘着付与剤は、プロピレン系接着剤用重合体組成物(D)70〜95重量%に対して、粘着付与剤5〜30重量%の割合で配合することが好ましい。
本発明のプロピレン系接着剤用重合体組成物(D)は、積層体の接着層として好適に使用される。積層体を構成する他の熱可塑性樹脂層の樹脂としては、種々の熱可塑性樹脂、例えば、ポリオレフィン、ポリアミド、エチレン・ビニルアルコ−ル共重合体、ウレタン系接着剤を塗布した基材または金属が使用できる。
本発明の積層体は、公知の種々の方法により製造することができる。例えば、インフレ−ション成形、キャスト成形、チュ−ブ成形、押出コ−ティング成形などの公知の共押出法により製造することができ、また、単層あるいは複層のフィルムなどを成形した後に、加熱によりドライラミする方法などを例示することができる。
実施例および比較例において使用した樹脂を以下に示す。なお、特に断らない限り、いずれも常法にしたがい重合を行って調製した。
PP-1 :無水マレイン酸グラフト変性エチレン・プロピレンランダム共重合体(A)
(無水マレイン酸グラフト量=0.22重量%、
230℃、2.16kg荷重でのMFR 11g/10分、
密度 0.90g/cm3)、
PE-1 :エチレン・プロピレン共重合体(B)
(190℃、2.16kg荷重でのMFR 0.4g/10分、
密度 0.87g/cm3)、
PE-2 :エチレン・ヘキセン共重合体(B)
(190℃、2.16kg荷重でのMFR 4.0g/10分、
密度 0.92g/cm3)、
PE-3 :エチレン・ブテン共重合体(B)
(190℃、2.16kg荷重でのMFR 2.0g/10分、
密度 0.95g/cm3)、
CEBC-1:オレフィン結晶−エチレン・ブチレン−オレフィン結晶ブロック共重合体(C)
(商品名ダイナロン6200P、JSR(株)製、
230℃、2.16kg荷重でのMFR 2.5g/10分、
密度 0.88g/cm3)
EVOH :エチレン・ビニルアルコール共重合体
(商品名エバール F101A、クラレ(株)製、
190℃、2.16kg荷重でのMFR 1.6g/10分、
密度 1.190g/cm3、エチレン共重合比率 32モル%)
[実施例1]
<プロピレン系接着剤用重合体組成物(D)の製造>
(A)MFRが11g/10分、密度が0.90g/cm3である無水マレイン酸グラフト変性エチレン・プロピレンランダム共重合体(PP−1)75重量%と、(B)MFRが0.4g/10分、密度が0.87g/cm3であるエチレン・プロピレン共重合体(PE−1)20重量%と、(C)MFRが2.5g/10分、密度0.88g/cm3であるオレフィン結晶−エチレン・ブチレン−オレフィン結晶ブロック共重合体(CEBC-1)5重量%とを1軸押出機を用いて230℃にて溶融混練して、プロピレン系接着剤用重合体組成物(D)を得た。得られたプロピレン系接着剤用重合体組成物(D)のMFRは7.5g/10分、密度は0.90g/cm3であった。
下記の成形条件で、共押出成形により3層フィルム(フィルム−1)を成形し、得られた3層フィルムのEVOH層とプロピレン系接着剤用重合体組成物(D)からなる接着層との層間接着強度(剥離強度)を、初期および90℃で24時間熱処理した後に剥離速度300mm/分にてT型剥離することにより求めた。
外層/中間層/内層=40/40/160μm
外層 :EVOH
中間層:プロピレン系接着剤用重合体組成物(D)
内層 :高圧法LDPE
T-ダイ成形機:ダイ径40mmφ押出機(外層)
設定温度・・・220℃
ダイ径40mmφ押出機(中間層)
設定温度・・・220℃
ダイ径40mmφ押出機(内層)
設定温度・・・220℃
成形速度:5m/分
<白化伸び>
下記の成形条件にて、プロピレン系接着剤用重合体組成物(D)をプレス成形し、引っ張り速度200mm/分で引っ張り試験を行った時に、白化を開始する引っ張り伸びを求めた。
プロピレン系接着剤用重合体組成物(D)=100μm
T-ダイ成形機:ダイ径40mmφ押出機
設定温度・・・220℃
成形速度:10m/分
[実施例2〜3、比較例1〜3]
中間層を構成するポリプロピレン系接着剤用重合体組成物(D)の組成を表1に示した組成に代えたこと以外は、実施例1と同様にして接着剤用重合体組成物(D)の製造を行い、3層積層体を成形した。得られたプロピレン系接着剤用重合体組成物(D)の物性および成形された積層体の測定・評価結果を表1に示す。
Claims (2)
- (i)グラフト変性ポリプロピレン(A)を40〜92重量%、
(ii)230℃、2.16kg荷重におけるメルトフロ−レ−ト(MFR)が0.01〜10g/10分で、かつ、密度が0.940g/cm3以下のエチレン・α−オレフィ
ン共重合体(B)を5〜30重量%、および
(iii)オレフィン結晶セグメントとエチレン・α−オレフィンセグメントとからなるブロック共重合体(C)を3〜30重量%(但し、(A)、(B)および(C)の合計は100重量%)含み、
グラフト変性ポリプロピレン(A)は、不飽和カルボン酸および/またはその誘導体でグラフト変性されたポリプロピレンであり、不飽和カルボン酸またはその誘導体の残基を、グラフト変性ポリプロピレン(A)100重量%に対して、0.01〜5重量%含有し、
上記ブロック共重合体(C)がオレフィン結晶−エチレン・ブチレン−オレフィン結晶ブロック共重合体である
プロピレン系接着剤用重合体組成物(D)。 - 請求項1に記載のプロピレン系接着剤用重合体組成物を含む層を少なくとも1層有する積層体。
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JPS6162544A (ja) * | 1984-09-03 | 1986-03-31 | Mitsubishi Chem Ind Ltd | 樹脂組成物 |
JPH0841276A (ja) * | 1994-07-29 | 1996-02-13 | Mitsubishi Chem Corp | 塗装用プロピレン系樹脂組成物 |
JPH1060128A (ja) * | 1996-08-13 | 1998-03-03 | Nissha Printing Co Ltd | フィルムおよび絵付用シート |
JP2001294836A (ja) * | 2000-04-14 | 2001-10-23 | Mitsui Chemicals Inc | 接着性樹脂組成物および積層体 |
JP2005068420A (ja) * | 2003-08-07 | 2005-03-17 | Mitsui Chemicals Inc | 粘着シート |
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US20090275700A1 (en) | 2009-11-05 |
CN101151342B (zh) | 2012-06-27 |
JPWO2006104058A1 (ja) | 2008-09-04 |
EP1867692A1 (en) | 2007-12-19 |
US8106122B2 (en) | 2012-01-31 |
WO2006104058A1 (ja) | 2006-10-05 |
EP1867692A4 (en) | 2008-07-16 |
EP1867692B1 (en) | 2013-01-16 |
CN101151342A (zh) | 2008-03-26 |
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