CN115348991B - 树脂组合物、使用了其的薄膜和多层结构体 - Google Patents
树脂组合物、使用了其的薄膜和多层结构体 Download PDFInfo
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- CN115348991B CN115348991B CN202180024925.8A CN202180024925A CN115348991B CN 115348991 B CN115348991 B CN 115348991B CN 202180024925 A CN202180024925 A CN 202180024925A CN 115348991 B CN115348991 B CN 115348991B
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Classifications
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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
-
- 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
- C08L23/06—Polyethene
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
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Abstract
本发明是一种树脂组合物,其含有生物聚乙烯系树脂(A)、乙烯‑乙烯醇系共聚物(B)和碱金属盐(C),上述碱金属盐(C)的含量相对于上述乙烯‑乙烯醇系共聚物(B)的重量以金属换算计为10~1500ppm。根据该树脂组合物,可抑制成型时的凝胶产生、透明性的降低,因此,能够得到外观优异的成型物。
Description
技术领域
本发明涉及树脂组合物,更详细而言,涉及尽管含有生物聚乙烯系树脂,但仍然可抑制凝胶产生、能够形成透明性优异的成型物的树脂组合物,以及使用了其的薄膜和多层结构体。
背景技术
近年来,由塑料垃圾导致的环境负担成为严重问题,因此,为了降低该负担,提出了将源自石油的塑料替换成源自植物等生物质资源的生物质塑料的各种技术。
例如,乙烯-乙烯醇系共聚物(以下有时简写为“EVOH”)因具有优异的阻气性和透明性而常用于食品包装材料,但其中的大多数为了赋予耐水性、强度、其它功能而在制成借助粘接剂层层叠有聚烯烃系树脂等的多层结构体的状态下使用。
因而,提出了如下方案:在这种多层结构体中,由例如源自生物质资源的聚乙烯系树脂(生物聚乙烯系树脂)来形成上述聚烯烃系树脂层的一部分或全部。
另外,为了提高资源的再利用性,还提出了利用回收层来构成这种多层结构体的至少一部分的方案(参照后述专利文献1)。
上述回收层是指:在使用上述多层结构体制造容器等成型物后产生的成型物的碎屑、端部等无用部分、不合格品;或者,回收将成型物用于各种用途后的垃圾等废料,并熔融成型为粒料等后加以利用而形成的层。
现有技术文献
专利文献
专利文献1:日本特开2014-30942号公报
发明内容
发明要解决的问题
然而,上述生物聚乙烯系树脂与源自石油的聚乙烯系树脂相比包含大量低分子量成分,因此,有可能在成型时发生热劣化而产生凝胶,或者树脂原本的透明性降低。因此,对于使用上述回收层得到的成型物、即便不使用回收层也出于兼具阻气性和机械强度的目的而使用生物聚乙烯系树脂和EVOH进行成型的成型物而言,外观的降低有时成为问题,强烈要求对其加以改善。
因而,本发明的课题在于,提供即便含有生物聚乙烯系树脂也能够抑制成型时的凝胶产生、透明性降低的优异树脂组合物。
用于解决问题的方案
本发明人等为了解决上述课题而进行了深入研究,结果发现:通过在将生物聚乙烯系树脂与EVOH加以组合的树脂组合物中进一步相对于上述EVOH以特定的比例含有碱金属盐,从而能够解决上述课题,由此完成了本发明。
即,本发明提供以下的[1]~[9]。
[1]一种树脂组合物,其含有生物聚乙烯系树脂(A)、EVOH(B)和碱金属盐(C),上述碱金属盐(C)的含量相对于上述EVOH(B)的重量以金属换算计为10~1500ppm。
[2]根据[1]所述的树脂组合物,其中,上述生物聚乙烯系树脂(A)与上述乙烯-乙烯醇系共聚物(B)的含有比例(A/B)以重量基准计为100/0.01~100/25。
[3]根据[1]或[2]所述的树脂组合物,其中,上述乙烯-乙烯醇系共聚物(B)中的乙烯含量为20~60摩尔%。
[4]根据[1]~[3]中任一项所述的树脂组合物,其中,上述树脂组合物含有粘接性树脂(D)。
[5]根据[1]~[4]中任一项所述的树脂组合物,其中,上述粘接性树脂(D)为马来酸改性高分子。
[6]根据[1]~[5]中任一项所述的树脂组合物,其中,上述碱金属盐(C)为碱金属的乙酸盐。
[7]根据[1]~[5]中任一项所述的树脂组合物,其中,上述碱金属盐(C)为乙酸钠。
[8]一种薄膜,其由[1]~[7]中任一项所述的树脂组合物形成。
[9]一种多层结构体,其具有阻气层、基材树脂层、以及设置在上述阻气层与基材树脂层之间的中间层,上述中间层为包含[1]~[7]中任一项所述的树脂组合物的层。
发明的效果
本发明的树脂组合物是在将生物聚乙烯系树脂(A)与EVOH(B)加以组合的树脂组合物中进一步相对于上述EVOH(B)以特定的比例含有碱金属盐(C)而得到的。根据该构成,在将该树脂组合物熔融加热而进行成型时,可抑制凝胶的产生、透明性的降低,因此发挥能够得到外观优异的成型物的效果。并且,尽管使用生物聚乙烯系树脂,但成型物的外观与使用以往的源自石油的聚乙烯系树脂得到的成型物相比也毫不逊色,因此,能够推进在树脂成型物中使用生物聚乙烯系树脂,能够对降低环境负担作出贡献。
并且,本发明的薄膜和多层结构体分别使用了本发明的树脂组合物,因此如上所述,尽管使用生物聚乙烯系树脂,但仍然具有优异的外观,能够对降低环境负担作出贡献。
需要说明的是,在本发明中,“薄膜”是指:包括所谓的“片”、“带”在内的主旨。
此处,可以认为在本发明中能够获得这种效果的原因在于,本发明的树脂组合物在与圆筒、螺杆等高温金属接触的状态下进行熔融加热时,上述碱金属盐(C)会将与上述高温金属接触的树脂组合物的pH控制在适度的范围内,因此,抑制生物聚乙烯系树脂的低分子量成分的热劣化、EVOH的未预期的副反应等,抑制成为凝胶产生、透明性降低的原因的粘度上升。
具体实施方式
以下,针对用于实施本发明的方式进行具体说明,但本发明不限定于这些。
本发明的树脂组合物含有生物聚乙烯系树脂(A)、EVOH(B)和碱金属盐(C)。以下,针对各成分进行说明。
[生物聚乙烯系树脂(A)]
上述“生物聚乙烯系树脂”是指:以可再生的生物质资源作为原料,通过化学合成或生物学合成而得到的聚乙烯系树脂。上述生物聚乙烯系树脂具有如下特征:即便在对其进行焚烧处理的情况下,也会因生物质具备的碳中和性而不使大气中的二氧化碳浓度上升。
上述生物聚乙烯系树脂(A)优选使用由得自植物原料的生物乙醇衍生的源自植物的乙烯。即,上述生物聚乙烯系树脂(A)优选为源自植物的聚乙烯系树脂。
源自植物(生物质资源)的聚乙烯系树脂与源自石油的聚乙烯系树脂在分子量、机械性质/热性质之类的物性方面不产生差异。因而,为了区分它们而通常使用生物质度。上述生物质度是指:由于源自石油的聚乙烯系树脂的碳不含14C(放射性碳14、半衰期为5730年),因此,利用加速器质谱分析来测定该14C的浓度,并作为源自植物的生物聚乙烯系树脂的含有比例的指标。因此,如果是使用源自植物的聚乙烯系树脂得到的薄膜,则测定该薄膜的生物质度时,成为与源自植物的聚乙烯系树脂的含量相符的生物质度。
上述生物质度可利用例如以下的方法进行测定。
[生物质度的测定]
使测定对象试样燃烧而产生二氧化碳,将在真空管线中进行了精制的二氧化碳以铁作为催化剂并利用氢进行还原,使其生成石墨。并且,将该石墨安装于以串联加速器作为基础的14C-AMS专用装置(NEC公司制),进行14C的计数、13C的浓度(13C/12C)、14C的浓度(14C/12C)的测定,由它们的测定值计算试样碳相对于标准现代碳的14C浓度的比例。
作为上述生物聚乙烯系树脂(A),不仅可以使用将这样的由生物乙醇衍生的乙烯聚合而得到的聚乙烯均聚物,还可以使用这样的乙烯与少量共聚单体的共聚物、即聚乙烯共聚物。作为上述聚乙烯共聚物,可列举出例如由乙烯为重量分数小于50%的其它α-烯烃单体或重量分数为3%以下的具有官能团的非烯烃单体形成的共聚物。
作为上述其它α-烯烃单体,可列举出碳原子数为3~20的α-烯烃,例如丙烯、1-丁烯、1-戊烯、1-己烯、1-庚烯、1-辛烯、1-壬烯、1-癸烯、1-十一碳烯、1-十二碳烯、1-十三碳烯、1-十四碳烯、1-十五碳烯、1-十六碳烯、1-十七碳烯、1-十八碳烯、1-十九碳烯、1-二十碳烯、3-甲基-1-丁烯、4-甲基-1-丁烯、3-甲基-1-戊烯、3-乙基-1-戊烯、4-甲基-1-戊烯、4-甲基-1-己烯、4,4-二甲基-1-己烯、4,4-二甲基-1-戊烯、4-乙基-1-己烯、3-乙基-1-己烯、9-甲基-1-癸烯、11-甲基-1-十二碳烯、12-乙基-1-十四碳烯等。它们可以单独使用或组合使用两种以上。
另外,作为上述非烯烃单体,可列举出例如苯乙烯系单体、二烯系单体、环状单体、含有氧原子的单体等。它们可以单独使用或组合使用两种以上。
作为上述苯乙烯系单体,可列举出例如苯乙烯、4-甲基苯乙烯、4-二甲基氨基苯乙烯等。
作为上述二烯系单体,可列举出例如1,3-丁二烯、1,4-戊二烯、1,4-己二烯、1,5-己二烯、1,4-辛二烯、1,5-辛二烯、1,6-辛二烯、1,7-辛二烯、2-甲基-1,5-己二烯、6-甲基-1,5-庚二烯、7-甲基-1,6-辛二烯、4-乙叉基-8-甲基-1,7-壬二烯、4,8-二甲基-1,4,8-癸三烯(DMDT)、二环戊二烯、环己二烯、二环辛二烯等。
作为上述环状单体,可列举出例如亚甲基降冰片烯、5-亚乙基降冰片烯、5-乙叉基-2-降冰片烯、5-亚甲基-2-降冰片烯、5-异丙叉基-2-降冰片烯、6-氯甲基-5-异丙烯基-2-降冰片烯、2,3-二异丙叉基-5-降冰片烯、2-乙叉基-3-异丙叉基-5-降冰片烯、2-丙烯基-2,2-降冰片二烯、环戊烯等。
作为上述含有氧原子的单体,可列举出例如己烯醇、己烯酸、辛烯酸甲酯等。
这些上述其它α-烯烃单体和非烯烃单体可以以可再生的生物质资源作为原料,也可以以石油作为原料。使用以可再生的生物质资源作为原料的单体时,能够进一步提高最终制品的生物质度。另外,使用以石油作为原料的单体时,由于能够获取多种多样的单体,因此,通过将它们组合使用,从而能够根据目的而容易地调整最终得到的生物聚乙烯系树脂的物性等。
本发明中使用的生物聚乙烯系树脂(A)通过乙烯的均聚或者乙烯与上述那样的共聚单体的共聚而得到,上述聚合或共聚可使用茂金属催化剂、齐格勒-诺塔催化剂,并按照常规方法来进行。其中,优选使用茂金属催化剂。
作为上述生物聚乙烯系树脂(A),具体而言,可列举出例如高密度聚乙烯(HDPE、密度为0.940g/cm3以上)、中密度聚乙烯(MDPE、密度为0.925g/cm3以上且小于0.940g/cm3)、低密度聚乙烯(LDPE、密度小于0.925g/cm3)、直链状低密度聚乙烯(LLDPE、密度为0.910~0.925g/cm3)等。它们可以单独使用或组合使用两种以上。其中,优选为高密度聚乙烯、直链状低密度聚乙烯。
上述生物聚乙烯系树脂(A)的熔体流动速率(MFR)(190℃、载荷2160g)通常为0.1~50g/10分钟、优选为0.5~30g/10分钟、特别优选为2~10g/10分钟。该MFR过大时,存在成膜性不稳定的倾向,该MFR过小时,存在粘度变得过高、难以熔融挤出的倾向。
需要说明的是,作为本发明中适合使用的生物聚乙烯系树脂(A)的市售品,可列举出ブラスケム(Braskem)公司制的Green PE等。
[EVOH(B)]
与上述生物聚乙烯系树脂(A)一同使用的EVOH(B)通常是通过使乙烯与乙烯基酯系单体的共聚物、即乙烯-乙烯基酯系共聚物进行皂化而得到的树脂,是非水溶性的热塑性树脂。作为上述乙烯基酯系单体,从经济方面出发,通常使用乙酸乙烯酯。
作为上述乙烯与乙烯基酯系单体的聚合方法,可列举出公知且任意的聚合方法,例如使用溶液聚合、悬浮聚合、乳液聚合进行的方法,通常使用以甲醇作为溶剂的溶液聚合。所得乙烯-乙烯基酯系共聚物的皂化也可以利用公知的方法来进行。
如此操作而制造的EVOH(B)以源自乙烯的结构单元和乙烯醇结构单元为主,通常包含未经皂化而残留的若干量的乙烯基酯结构单元。
作为上述乙烯基酯系单体,从市场获取性、制造时的杂质处理效率良好的观点出发,代表性地使用乙酸乙烯酯。作为其它乙烯基酯系单体,可列举出例如甲酸乙烯酯、丙酸乙烯酯、戊酸乙烯酯、丁酸乙烯酯、异丁酸乙烯酯、特戊酸乙烯酯、癸酸乙烯酯、月桂酸乙烯酯、硬脂酸乙烯酯、叔碳酸乙烯酯等脂肪族乙烯基酯;苯甲酸乙烯酯等芳香族乙烯基酯等,通常可以使用碳原子数为3~20、碳原子数优选为4~10、碳原子数特别优选为4~7的脂肪族乙烯基酯。它们可以单独使用或组合使用两种以上。
上述EVOH(B)中的乙烯含量可利用使乙烯基酯系单体与乙烯进行共聚时的乙烯压力来控制,优选为20~60摩尔%。更优选为25~50摩尔%、特别优选为25~35摩尔%。该含量过低时,存在高湿度下的阻气性、熔融成型性降低的倾向,反之,该含量过高时,存在阻气性降低的倾向。
上述乙烯含量可根据ISO14663进行测定。
另外,上述EVOH(B)中的乙烯基酯成分的皂化度可利用对乙烯-乙烯基酯系共聚物进行皂化时的皂化催化剂(通常使用氢氧化钠等碱性催化剂)的量、温度、时间等来控制,通常为90~100摩尔%、优选为95~100摩尔%、特别优选为99~100摩尔%。若上述皂化度低,则存在阻气性、热稳定性、耐湿性等降低的倾向。
上述EVOH(B)的皂化度可根据JIS K6726(其中,EVOH以均匀溶解于水/甲醇溶剂而得到的溶液的形式使用)来测定。
另外,上述EVOH(B)的MFR(210℃、载荷2160g)通常为0.5~100g/10分钟、优选为1~50g/10分钟、特别优选为3~35g/10分钟。若上述MFR过大,则存在成型性不稳定的倾向,若上述MFR过小,则观察到粘度变得过高、难以熔融挤出的倾向。
上述MFR成为EVOH的聚合度的指标,可利用使乙烯与乙烯基酯系单体进行共聚时的聚合引发剂的量、溶剂的量来调整。
另外,上述EVOH(B)中,在不损害本发明效果的范围(例如EVOH(B)的10摩尔%以下)内,可以进一步包含源自以下所示共聚单体的结构单元。
作为上述共聚单体,可列举出丙烯、1-丁烯、异丁烯等烯烃类;3-丁烯-1-醇、3-丁烯-1,2-二醇、4-戊烯-1-醇、5-己烯-1,2-二醇等含有羟基的α-烯烃类或其酯化物、酰基化物等衍生物;2-亚甲基丙烷-1,3-二醇、3-亚甲基戊烷-1,5-二醇等羟基烷基亚乙烯基类;1,3-二乙酰氧基-2-亚甲基丙烷、1,3-二丙酰氧基-2-亚甲基丙烷、1,3-二丁酰基氧基-2-亚甲基丙烷等羟基烷基亚乙烯基二乙酸酯类;丙烯酸、甲基丙烯酸、巴豆酸、苯二甲酸(酐)、马来酸(酐)、衣康酸(酐)等不饱和酸类或其盐或者烷基的碳原子数为1~18的单烷基酯或二烷基酯类;丙烯酰胺、烷基的碳原子数为1~18的N-烷基丙烯酰胺、N,N-二甲基丙烯酰胺、2-丙烯酰胺丙磺酸或其盐、丙烯酰胺丙基二甲基胺或其酸盐或其季铵盐等丙烯酰胺类;甲基丙烯酰胺、烷基的碳原子数为1~18的N-烷基甲基丙烯酰胺、N,N-二甲基甲基丙烯酰胺、2-甲基丙烯酰胺丙磺酸或其盐、甲基丙烯酰胺丙基二甲基胺或其酸盐或其季铵盐等甲基丙烯酰胺类;N-乙烯基吡咯烷酮、N-乙烯基甲酰胺、N-乙烯基乙酰胺等N-乙烯基酰胺类;丙烯腈、甲基丙烯腈等氰化乙烯基类;烷基的碳原子数为1~18的烷基乙烯基醚、羟基烷基乙烯基醚、烷氧基烷基乙烯基醚等乙烯基醚类;氯乙烯、偏二氯乙烯、氟乙烯、偏二氟乙烯、溴乙烯等乙烯基卤化物类;三甲氧基乙烯基硅烷等乙烯基硅烷类;乙酸烯丙酯、烯丙基氯等烯丙基卤化物类;烯丙醇、二甲氧基烯丙醇等烯丙醇类;(3-丙烯酰胺-3-二甲基丙基)三甲基氯化铵、丙烯酰胺-2-甲基丙磺酸等共聚单体。它们可以单独使用或组合使用两种以上。
尤其是,作为本发明中使用的EVOH(B),若使用在侧链具有伯羟基的EVOH,则从保持阻气性且二次成型性良好的观点出发是优选的,其中,优选为共聚有含羟基的α-烯烃类的EVOH,特别优选为在侧链具有1,2-二醇结构的EVOH。
并且,在侧链具有伯羟基的EVOH的情况下,源自该具有伯羟基的单体的结构单元的含量通常优选为EVOH的0.1~20摩尔%、进一步优选为0.5~15摩尔%、特别优选为1~10摩尔%。
另外,本发明中使用的EVOH(B)可以进行了氨基甲酸酯化、缩醛化、氰基乙基化、氧亚烷基化等“后改性”。
进而,本发明中使用的EVOH(B)可以是两种以上的EVOH(B),例如乙烯含量不同、皂化度不同、聚合度不同、共聚成分不同等的混合物。
需要说明的是,本发明的树脂组合物中,前述生物聚乙烯系树脂(A)与上述EVOH(B)的含有比率(A/B)以重量基准计优选为100/0.01~100/25、更优选为100/1~100/20、特别优选为100/5~100/15。若上述生物聚乙烯系树脂(A)的配混比例过少,则存在低温下的成型性降低的倾向,另一方面,若生物聚乙烯系树脂(A)过多,则存在阻隔性降低的倾向。
[碱金属盐(C)]
本发明中,作为与上述生物聚乙烯系树脂(A)、EVOH(B)一同使用的碱金属盐(C),可列举出碱金属的有机酸盐和碱金属的无机酸盐,它们可以单独使用,也可以组合使用两种以上。
作为构成上述碱金属盐(C)的碱金属,可列举出锂、钠、钾、铯等,作为与这些碱金属形成盐的有机酸,可列举出乙酸、丙酸、丁酸、月桂酸、硬脂酸、油酸、山嵛酸等羧酸。另外,作为无机酸,可列举出硫酸、亚硫酸、碳酸、磷酸等。适合使用其中的乙酸钠、乙酸钾。
本发明中,上述碱金属盐(C)的含量相对于上述EVOH(B)的重量以金属换算计为10~1500ppm。其中,优选为50~1000ppm,进而,更优选为70~500ppm。即,若上述碱金属盐(C)的含量偏离上述范围,则存在树脂组合物的pH平衡受损、抑制熔融加热时的凝胶产生和透明性降低的效果不充分的倾向。
[其它成分]
另外,本发明的树脂组合物中,除了上述必须成分(A)~(C)之外,在不损害本发明效果的范围内,可以配混除前述(A)~(C)之外的任选成分。例如,为了抑制在使用该树脂组合物进行成型时可能产生的眼眵状物,可以配混以下那样的粘接性树脂(D)。
[粘接性树脂(D)]
作为上述粘接性树脂(D),可列举出例如通过加成反应、接枝反应等使不饱和羧酸或其酸酐化学键合于聚烯烃系树脂而得到的含有羧基的改性聚烯烃系聚合物。作为上述含有羧基的改性聚烯烃系聚合物,可列举出例如马来酸酐接枝改性聚乙烯、马来酸酐接枝改性聚丙烯、马来酸酐接枝改性乙烯-丙烯(嵌段和无规)共聚物、马来酸酐接枝改性乙烯-丙烯酸乙酯共聚物、马来酸酐接枝改性乙烯-乙酸乙烯酯共聚物、马来酸酐改性聚环状烯烃系树脂、马来酸酐接枝改性聚烯烃系树脂等马来酸酐改性高分子。
它们可以单独使用,也可以以两种以上的混合物的形式使用。
作为本发明中可使用的粘接性树脂(D),从不仅有助于抑制在成型时产生眼眵状物的效果、还有助于抑制在熔融加热时产生凝胶的效果和抑制透明性降低的效果的观点出发,特别适合为马来酸酐改性聚乙烯、马来酸酐改性乙烯-α-烯烃共聚物等马来酸酐改性高分子。
上述马来酸酐改性高分子的酸值通常为50mgKOH/g以下、优选为30mgKOH/g以下、特别优选为20mgKOH/g以下。若酸值过高,则存在如下倾向:与EVOH(B)中的羟基的反应位点增加,在熔融混炼过程中生成高聚合度化物,挤出加工时的稳定性降低,难以获得良好的成型物。需要说明的是,酸值的下限通常为1mgKOH/g、优选为2mgKOH/g。另外,上述酸值根据JIS K0070进行测定。
作为上述马来酸酐改性高分子,使用马来酸酐改性聚乙烯时的MFR(190℃、载荷2160g)通常为0.01~150g/10分钟、优选为0.1~50g/10分钟、更优选为1~25g/10分钟、进一步优选为3~10g/10分钟。
另外,作为马来酸酐改性高分子,使用马来酸酐改性乙烯-α-烯烃共聚物时的MFR(230℃、载荷2160g)通常为0.1~150g/10分钟、优选为0.5~100g/10分钟、更优选为1~50g/10分钟、进一步优选为5~35g/10分钟。
若MFR在上述范围外,则存在与生物聚乙烯系树脂(A)和EVOH(B)的相溶性降低、在混合时分散性降低的倾向。
作为上述粘接性树脂(D),在本发明的树脂组合物中含有上述马来酸酐改性高分子的情况下,其含量相对于生物聚乙烯系树脂(A)与EVOH(B)的总计100重量份优选为0.01~25重量份、更优选为1~20重量份、特别优选为5~15重量份。若上述马来酸酐改性高分子的含量在上述范围内,则通过与前述必须成分(A)、(B)的协同效应而能够得到更优异的抑制凝胶产生的效果和抑制透明性降低的效果,故而优选。
另外,本发明的树脂组合物可以进一步含有其它热塑性树脂、通常向热塑性树脂中添加的添加剂。
作为上述添加剂,可列举出例如增塑剂(例如乙二醇、甘油、己二醇等脂肪族多元醇等)、吸氧剂、热稳定剂、光稳定剂、紫外线吸收剂、着色剂、抗静电剂、表面活性剂(其中不包括用作润滑剂的物质)、抗菌剂、抗粘连剂、填充材料(例如无机填料等)等。这些添加剂可以单独使用或组合使用两种以上。
[树脂组合物的制造]
本发明的树脂组合物可以以上述(A)~(C)作为必须成分,并根据需要适当使用上述其它成分(D)、任选添加剂等来制造。并且,作为必须成分的生物聚乙烯系树脂(A)和EVOH(B)也可以使用一次都未用于成型的原料(未再生品),可以使用具备含有生物聚乙烯系树脂(A)和EVOH(B)的层的多层结构体的使用过的回收物、在使用这种多层结构体得到的制品的制造过程中被去除的无用部分、不合格品等。
需要说明的是,上述多层结构体的回收物通常呈现至少一部分使用了生物聚乙烯系树脂(A)的增强层与使用了EVOH(B)的阻气层借助粘接性树脂(D)进行接合的结构,因此,在使用该回收物来制成本发明的树脂组合物的情况下,必然形成包含粘接性树脂(D)的树脂组合物。
以下,关于本发明的树脂组合物的制造方法,针对使用含有包含生物聚乙烯系树脂(A)和EVOH(B)的层的多层结构体的回收物的情况进行说明。
多层结构体的回收物通常以在粉碎后根据需要用筛子等调节了粒度的状态而用作本发明的树脂组合物的原料。
在上述回收物的粉碎时,可通过使用公知的粉碎机来进行。该粉碎品的表观密度通常为0.25~0.85g/mL、进一步优选为0.3~0.7g/mL、特别优选为0.35~0.6g/mL。在表观密度过小的情况下,存在树脂组合物中的生物聚乙烯系树脂(A)的分散不良、在获得成型物的过程中熔融成型性、机械特性降低的倾向,在表观密度过大的情况下,存在因在挤出机中发生供给不良而使所得成型品的再研磨层的熔融成型性降低的倾向。需要说明的是,上述粉碎品的表观密度是按照JIS K6891的“5.3表观密度”试验方法而测得的值。
关于上述表观密度,可通过任意调整粉碎机的粉碎刀具的形状、粉碎刀具的转速、粉碎的处理速度、用作筛子的网状物的网眼大小等来控制。另外,关于粉碎品的形状、粒径,可利用公知的方法进行调整。
为了使用将上述多层结构体回收得到的粉碎品(以下称为“粉碎品”)来获得本发明的树脂组合物,向上述粉碎品中配混前述碱金属盐(C),并均匀混合。需要说明的是,从生产率的观点出发,可以向上述粉碎品中配混作为未再生品的生物聚乙烯系树脂(A)、作为未再生品的EVOH(B)。
作为上述两者的混合方法,可列举出例如干式共混法、熔融混炼法、溶液混合法、浸渗法等公知方法。
作为上述干式共混法,可列举出例如(i)使用转鼓等对上述粉碎品和上述碱金属盐(C)进行干式共混的方法等。并且,在上述干式共混时,可以对碱金属盐(C)直接进行干式共混,也可以预先制备包含碱金属盐(C)的热塑性树脂的粒料,并将该热塑性树脂的粒料与粉碎品进行干式共混。
另外,作为上述熔融混炼法,可列举出例如(ii)对上述干式共混物进行熔融混炼的方法;(iii)向熔融状态的上述粉碎品中添加碱金属盐(C)并进行熔融混炼的方法等。
进而,作为上述溶液混合法,可列举出例如(iv)使用上述粉碎品来制备溶液,向其中配混碱金属盐(C)并凝固成型后,进行固液分离并干燥的方法等。
这些方法之中,从生产率的观点出发,优选为熔融混炼法,特别优选为(ii)的方法。另外,可以将这些方法之中的多个方法加以组合。
本发明的树脂组合物未必需要如上所述地将回收多层结构体而制成的粉碎品用作原料,也可以使用未再生品,即最初制造的生物聚乙烯系树脂(A)、EVOH(B)。使用上述未再生品时,只要以具有本发明的配混组成的方式使用公知的一般方法、例如干式共混法、熔融混炼法、溶液混合法等来制备树脂组合物即可。
需要说明的是,本发明的树脂组合物中,作为必须成分的碱金属盐(C)可以在制备EVOH(B)时按照在EVOH(B)中以规定比例含有碱金属盐(C)的方式进行制备。当然,通过以不含碱金属盐(C)的形式制备EVOH(B),并在混合树脂组合物时利用与前述相同的方法,将碱金属盐(C)配混至树脂成分(A)、(B)并进行混合,从而也可以得到本发明的树脂组合物。
本发明的树脂组合物在均匀混合各成分后,以粒料、粉末状之类的各种形态的树脂组合物的形式进行制备,并以各种成型物的成型用材料的形式来提供。尤其在本发明中,以熔融成型用材料的形式提供时,尽管该树脂组合物含有生物聚乙烯系树脂(A),但在熔融加热时仍然可抑制凝胶的产生、透明性的降低,能够得到外观优异的成型物,因此,尤其适合以熔融成型用材料的形式提供。
并且,作为使用本发明的树脂组合物而得到的成型物,以充分利用本发明的树脂组合物的特性的单层薄膜为首,可以作为具有使用本发明的树脂组合物而成型的层的多层结构体、或者呈现单层或多层且赋予了立体形状的各种成型物而供于实用。
作为用于获得上述成型物的成型方法,适合为熔融成型法。
作为上述熔融成型法,主要采用挤出成型法(T模挤出、吹胀挤出、吹塑成型、熔融纺丝、不规则模具挤出等)、注射成型法。熔融成型温度通常为150~300℃的范围、优选为160~250℃、特别优选为170~230℃。在上述熔融成型温度的范围内,能够将本发明的树脂组合物良好地成型,不会发生以往在含有生物聚乙烯系树脂的树脂组合物中成为问题的凝胶产生、透明性降低,能够得到外观优异的成型物。
[多层结构体]
需要说明的是,作为使用本发明的树脂组合物得到的成型物的一例,针对多层结构体进行说明。包含本发明的树脂组合物的层(包括仅由本发明的树脂组合物形成的层以及由其与其它树脂组合物的混合树脂组合物形成的层这两者)通过与由以除了本发明的树脂组合物之外的热塑性树脂作为主成分的其它基材(以下称为“基材树脂”)形成的基材树脂层、阻气层进行层叠,从而能够进一步赋予强度或者赋予其它功能。并且,在这种多层结构体之中,特别适合为具有阻气层、基材树脂层、以及设置在这些层之间的中间层的多层结构体,且上述中间层为包含本发明的树脂组合物的层。
需要说明的是,上述中间层具有两层以上时,其中的至少一个中间层适合为包含本发明的树脂组合物的层。
作为上述基材树脂,可列举出例如直链状低密度聚乙烯、低密度聚乙烯、超低密度聚乙烯、中密度聚乙烯、高密度聚乙烯、乙烯-丙烯(嵌段和无规)共聚物、乙烯-α-烯烃(碳原子数4~20的α-烯烃)共聚物等聚乙烯系树脂;聚丙烯、丙烯-α-烯烃(碳原子数4~20的α-烯烃)共聚物等聚丙烯系树脂;聚丁烯、聚戊烯、聚环状烯烃系树脂(主链和侧链中的至少一者具有环状烯烃结构的聚合物)等(未改性)聚烯烃系树脂;包括将这些聚烯烃类用不饱和羧酸或其酯进行接枝改性而得到的不饱和羧酸改性聚烯烃系树脂等改性烯烃系树脂在内的广义上的聚烯烃系树脂;离聚物、乙烯-乙酸乙烯酯共聚物、乙烯-丙烯酸共聚物、乙烯-丙烯酸酯共聚物、聚酯系树脂、聚酰胺系树脂(还包括共聚聚酰胺)、聚氯乙烯、聚偏二氯乙烯、丙烯酸系树脂、聚苯乙烯系树脂、乙烯基酯系树脂、聚酯系弹性体、聚氨酯系弹性体、聚苯乙烯系弹性体、氯化聚乙烯、氯化聚丙烯等卤代聚烯烃;芳香族或脂肪族聚酮类等。
这些之中,从经济性和生产率的观点出发,优选为聚酰胺系树脂、聚烯烃系树脂、聚酯系树脂、聚苯乙烯系树脂,更优选为聚乙烯系树脂、聚丙烯系树脂、聚环状烯烃系树脂和这些不饱和羧酸改性聚烯烃系树脂等聚烯烃系树脂。
另外,作为上述阻气层,没有特别限定,可列举出由无机物形成的阻气层、由有机物形成的阻气层。作为上述由无机物形成的阻气层,可列举出铝箔、铝蒸镀层等金属层;或者氧化硅蒸镀层、氧化铝蒸镀层等金属化合物层。作为上述由有机物形成的阻气层,可列举出由聚偏二氯乙烯系聚合物形成的层;由聚乙烯醇、EVOH等乙烯醇系聚合物形成的层。
将包含本发明的树脂组合物的层设为a(a1、a2、…),将基材树脂层设为b(b1、b2、…)时,上述多层结构体的层构成可以为a/b、b/a/b、a/b/a、a1/a2/b、a/b1/b2、b2/b1/a/b1/b2、b2/b1/a/b1/a/b1/b2等任意组合。另外,可以设置将在制造该多层结构体的过程中产生的端部、不合格品等进行再熔融成型而得到的包含本发明的树脂组合物与基材树脂的混合物的再利用层。多层结构体的层数以总数计通常为2~15、优选为3~10。在上述层构成中,可以在各自的层间根据需要夹设含有粘接性树脂的粘接性树脂层。
另外,将包含本发明的树脂组合物的层设为a(a1、a2、…),将阻气层设为c(c1、c2、…)时,上述多层结构体的层构成可以为a/c、c/a/c、a/c/a、a1/a2/c、a/c1/c2、c2/c1/a/c1/c2、c2/c1/a/c1/a/c1/c2等任意组合。另外,可以设置将在制造该多层结构体的过程中产生的端部、不合格品等进行再熔融成型而得到的、包含本发明的树脂组合物与阻气层形成材料的混合物的再利用层。多层结构体的层数以总数计通常为2~15、优选为3~10。在上述层构成中,可以在各自的层间根据需要夹设含有粘接性树脂的粘接性树脂层。
进而,将包含本发明的树脂组合物的层设为a(a1、a2、…),将基材树脂层设为b(b1、b2、…),将阻气层设为c(c1、c2、…)时,上述多层结构体的层构成可以为c/a/b、b/a/c/b、c/a/b/a、c/a1/a2/b、a/c/b1/b2、b2/b1/a/c/b1/b2、b2/b1/c/a/b1/a/c/b1/b2等任意组合。另外,可以设置将在制造上述多层结构体的过程中产生的端部、不合格品等进行再熔融成型而得到的包含本发明的树脂组合物、基材树脂和阻气层形成材料的混合物的再利用层。多层结构体的层数以总数计通常为2~15、优选为3~10。在上述层构成中,可以在各自的层间根据需要夹设含有粘接性树脂的粘接性树脂层。
作为上述粘接性树脂,可以使用公知的树脂,只要根据基材树脂层“b”中使用的热塑性树脂的种类来适当选择即可。代表性地可列举出通过加成反应、接枝反应等使不饱和羧酸或其酸酐化学键合于聚烯烃系树脂而得到的含有羧基的改性聚烯烃系聚合物。作为这种粘接性树脂,可以使用与前述本发明中可使用的粘接性树脂(D)相同的树脂,省略其说明。
需要说明的是,上述基材树脂、粘接性树脂中,在不损害本发明主旨的范围(例如相对于树脂整体为30重量%以下、优选为10重量%以下)内,可以包含以往已知那样的增塑剂、填料、粘土(蒙脱石等)、着色剂、抗氧化剂、抗静电剂、润滑剂、成核材料、抗粘连剂、蜡等。
本发明的树脂组合物与上述基材树脂的层叠(包括夹设粘接性树脂层的情况)可以利用公知的方法来进行。可列举出例如在由本发明的树脂组合物形成的薄膜等上熔融挤出层压基材树脂的方法;在基材树脂层上熔融挤出层压本发明的树脂组合物的方法;将树脂组合物与基材树脂进行共挤出的方法;使用有机钛化合物、异氰酸酯化合物、聚酯系化合物、聚氨酯化合物等公知的粘接剂,将树脂组合物层与基材树脂层进行干式层压的方法;在基材树脂上涂布树脂组合物的溶液后,去除溶剂的方法等。这些之中,从成本、环境的观点出发,优选为将树脂组合物与基材树脂进行共挤出的方法。
需要说明的是,将本发明的树脂组合物与其它树脂组合物的混合树脂组合物与上述基材树脂进行层叠的情况下,也可以使用与上述相同的方法。
上述多层结构体根据需要可以实施(加热)拉伸处理。拉伸处理可以为单轴拉伸、双轴拉伸中的任一者,在双轴拉伸的情况下,可以为同时拉伸,也可以为逐次拉伸。另外,作为拉伸方法,也可以采用辊拉伸法、拉幅机拉伸法、筒管拉伸法、拉伸吹塑法、真空压空成型等之中的拉伸倍率高的方法。拉伸温度在多层结构体的熔点附近的温度下从通常为40~170℃、优选为60~160℃左右的范围中进行选择。拉伸温度过低时,拉伸性变得不良,拉伸温度过高时,难以维持稳定的拉伸状态。
另外,在上述拉伸处理后,出于赋予尺寸稳定性的目的,可以进行热固定。热固定可以利用公知的手段来实施,例如,对于上述拉伸处理后的多层结构体,边保持张紧状态边通常以80~180℃、优选以100~165℃进行通常为2~600秒左右的热处理。另外,将由使用本发明的树脂组合物得到的多层结构体形成的拉伸薄膜用作收缩用薄膜时,为了赋予热收缩性,不进行上述热固定,只要进行例如对拉伸后的薄膜吹冷风而将其冷却固定等处理即可。
另外,根据情况,也可以使用本发明的多层结构体来获得杯、托盘状的多层容器。该情况下,通常采用深拉成型法,具体而言,可列举出真空成型法、压空成型法、真空压空成型法、助压模塞式真空压空成型法等。进而,由多层型坯(吹塑前的中空管状的预成型物)获得管、瓶状的多层容器(层叠体结构)时,采用吹塑成型法。具体而言,可列举出挤出吹塑成型法(双头式、模具移动式、型坯移动式、旋转式、储压器式、水平型坯式等)、冷却型坯式吹塑成型法、注射吹塑成型法、双轴拉伸吹塑成型法(挤出式冷却型坯双轴拉伸吹塑成型法、注射式冷却型坯双轴拉伸吹塑成型法、注射成型在线式双轴拉伸吹塑成型法等)等。所得层叠体根据需要可以进行热处理、冷却处理、压延处理、印刷处理、干式层压处理、溶液或熔融涂覆处理、制袋加工、深拉加工、箱加工、管加工、分裂加工等。
上述多层结构体(包括拉伸后的结构体)的厚度、以及构成多层结构体的树脂组合物层、基材树脂层和粘接性树脂层的厚度因层构成、基材树脂的种类、粘接性树脂的种类、用途、包装形态、要求物性等而无法一概而论,多层结构体(包括拉伸后的结构体)的厚度通常为10~5000μm、优选为30~3000μm、特别优选为50~2000μm。树脂组合物层通常为1~500μm、优选为3~300μm、特别优选为5~200μm,基材树脂层通常为5~3000μm、优选为10~2000μm、特别优选为20~1000μm,粘接性树脂层通常为0.5~250μm、优选为1~150μm、特别优选为3~100μm。
进而,关于上述多层结构体中的树脂组合物层相对于基材树脂层的厚度比(树脂组合物层/基材树脂层),在各层存在多个的情况下,以厚度最大的层彼此的比值计,通常为1/99~50/50、优选为5/95~45/55、特别优选为10/90~40/60。另外,关于上述多层结构体中的树脂组合物层相对于粘接性树脂层的厚度比(树脂组合物层/粘接性树脂层),在各层存在多个的情况下,以厚度最大的层彼此的比值计,通常为10/90~99/1、优选为20/80~95/5、特别优选为50/50~90/10。
由利用上述多层结构体而得到的薄膜、拉伸薄膜形成的包括袋和杯、托盘、管、瓶等在内的容器使用生物聚乙烯系树脂,因此,与以往的100%使用源自石油的聚乙烯的容器相比,环境负担小,能够满足社会上的要求。并且,尽管使用生物聚乙烯系树脂,在该树脂组合物层中仍然可抑制凝胶的产生,透明性也优异,因此,具有优异的外观,可广泛地用作一般食品、以及蛋黄酱、调味汁等调味料、味噌等发酵食品、色拉油等油脂食品、饮料、化妆品、药品等的各种包装材料容器。
实施例
以下,列举出实施例,更具体地说明本发明,但本发明只要不超过其主旨,就不限定于以下的实施例。需要说明的是,只要没有特别记载,则以下的“份”、“%”是指:重量基准。
在实施例之前,准备以下的成分。
[生物聚乙烯系树脂(A)]
A-1:源自植物的直链状低密度聚乙烯[SLH118(Braskem公司制、Green PE)、MFR为1.0g/10分钟(190℃、载荷2160g)]
A-2:源自植物的直链状低密度聚乙烯[SEB853(Braskem公司制、Green PE)、MFR为2.7g/10分钟(190℃、载荷2160g)]
[石油聚乙烯系树脂(A’)]
A’:低密度聚乙烯[LF448K1(Japan polyethylene Corporation制、NOVATEC LD)、MFR为2.0g/10分钟(190℃、载荷2160g)]
[EVOH(B)]
B-1:乙烯-乙烯醇共聚物[乙烯含量为29mol%、皂化度为99.7摩尔%、MFR为8g/10分钟(210℃、载荷2160g)]
B-2:乙烯-乙烯醇共聚物[乙烯含量为29mol%、皂化度为99.7摩尔%、MFR为8g/10分钟(210℃、载荷2160g)]
B-3:乙烯-乙烯醇共聚物[乙烯含量为44mol%、皂化度为99.6摩尔%、MFR为12g/10分钟(210℃、载荷2160g)]
B-4:乙烯-乙烯醇共聚物[乙烯含量为44mol%、皂化度为98.5摩尔%、MFR为4g/10分钟(210℃、载荷2160g)]
B-5:乙烯-乙烯醇共聚物[乙烯含量为44mol%、皂化度为99.6摩尔%、MFR为13g/10分钟(210℃、载荷2160g)]
[碱金属盐(C)]
·乙酸钠(乙酸Na)
·乙酸钾(乙酸K)
[其它金属盐(C')]
·硬脂酸钙(StCa)
·硬脂酸镁(StMg)
·硬脂酸锌(StZn)
·乙酸钙(乙酸Ca)
[粘接性树脂(D)]
·马来酸酐改性高分子:马来酸酐改性聚乙烯[三菱化学公司制、Modic M533、MFR为2.5g/10分钟(190℃、载荷2160g)]
<评价项目(评价方法、评价基准)的说明>
接着,以下示出针对实施例品、比较例品、参考例品的评价项目的详情。
(1)凝胶量
使用由实施例、比较例、参考例中使用的树脂组合物形成的粒料,利用下述成膜条件进行成膜,由此得到厚度30μm的单层薄膜。
<成膜条件>
挤出机:直径(H)40mm、L/H=28
螺杆:全螺纹类型压缩比=2.5
并且,针对该单层薄膜,通过目视来测量凝胶量。具体而言,从单层薄膜的下表面照射光,将不透光的部分(直径为0.4mm以上)作为1个凝胶,数出每单位面积(4cm×4cm)的凝胶数,如下所示地进行评价。
×(poor):凝胶数为40个以上或无法成膜
△(good):凝胶数为15个以上且小于40个
○(very good):凝胶数为4个以上且小于15个
◎(excellent):凝胶数为3个以下或无法测量凝胶
(2)透明性(内部雾度)
使用由实施例、比较例、参考例中使用的树脂组合物形成的粒料,与上述同样操作,制作厚度30μm的单层薄膜。并且,关于该单层薄膜的透明性,使用雾度计(日本电色公司制、NDH2000),按照JIS K7105,测定总雾度(%)。上述总雾度是以百分数的形式表示试验片的扩散光线透射率除以总光线透射率而得到的值,总雾度的值越是低值,则表示薄膜透明性越良好。其中,为了评价薄膜内部的雾度,在测定时使用在薄膜两面涂布液体石蜡而得到的试样,在去除由薄膜表面的凹凸导致的影响的状态下,测定内部雾度(%)。并且,根据其值,如下所述地进行评价。
×(poor):20%以上
△(good):15%以上且小于20%
○(very good):10%以上且小于15%
◎(excellent):小于10%
[实施例1~9、比较例1~8、参考例1~3]
将各成分以呈现后述表1~表3所示组成的方式进行配混,并从双轴混炼挤出机(日本制钢所制、TEX32)的原料供给口导入至料筒内,并运送至温度设定为240℃的混炼区中进行熔融共混,将熔融共混物从安装于喷出口的模具挤出成股线状。利用树脂用造粒机将所得股线状挤出物进行粒料化,得到粒料状的树脂组合物。
并且,对于所得的实施例1~9品和比较例1~8品、参考例1~3品,针对前述评价项目(凝胶量、透明性[内部雾度])进行测定和评价。将它们的结果一并示于下述表1~表3。
[表1]
[表2]
[表3]
根据上述结果可知:实施例1~9品在两个评价项目中的评价均大致良好,外观优异。
另一方面可知:比较例1~8品在两个评价项目中的至少一者的评价比实施例品差,外观存在问题。
另外可知:根据参考例1~3品,在使用源自石油的聚乙烯的情况下,无论有无碱金属盐,在两个评价项目中的评价均与实施例品相当,无论是否添加碱金属盐,均不会对两个评价造成影响。
由这些结果可知:比较例1~8品的外观问题是仅在使用生物聚乙烯系树脂时产生的的特有课题,该课题可通过添加碱金属盐来解决。
需要说明的是,在上述实施例中,针对本发明中的具体方式进行了示例,但上述实施例只不过是单纯的示例,不做限定性解释。应该认为对于本领域技术人员而言显而易见的各种变形全部落入本发明的范围内。
产业上的可利用性
本发明是含有生物聚乙烯系树脂(A)、EVOH(B)和碱金属盐(C)的树脂组合物,尽管含有上述生物聚乙烯系树脂(A),但仍然可抑制成型时的凝胶产生、透明度的降低,可广泛地用作能够得到外观优异的成型物的树脂组合物。
Claims (6)
1.一种树脂组合物,其特征在于,含有生物聚乙烯系树脂(A)、乙烯-乙烯醇系共聚物(B)和碱金属盐(C),所述碱金属盐(C)的含量相对于所述乙烯-乙烯醇系共聚物(B)的重量以金属换算计为10~1500ppm,
所述碱金属盐(C)为乙酸钠和/或乙酸钾,
所述生物聚乙烯系树脂(A)与所述乙烯-乙烯醇系共聚物(B)的含有比例(A/B)以重量基准计为100/0.01~100/15。
2.根据权利要求1所述的树脂组合物,其特征在于,所述乙烯-乙烯醇系共聚物(B)中的乙烯含量为20~60摩尔%。
3.根据权利要求1或2所述的树脂组合物,其特征在于,所述树脂组合物含有粘接性树脂(D)。
4.根据权利要求3所述的树脂组合物,其特征在于,所述粘接性树脂(D)为马来酸改性高分子。
5.一种薄膜,其特征在于,由权利要求1~4中任一项所述的树脂组合物形成。
6.一种多层结构体,其特征在于,具有阻气层、基材树脂层、以及设置在所述阻气层与基材树脂层之间的中间层,所述中间层为包含权利要求1~4中任一项所述的树脂组合物的层。
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