CN105637058B - 热熔粘合剂 - Google Patents
热熔粘合剂 Download PDFInfo
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- CN105637058B CN105637058B CN201480057409.5A CN201480057409A CN105637058B CN 105637058 B CN105637058 B CN 105637058B CN 201480057409 A CN201480057409 A CN 201480057409A CN 105637058 B CN105637058 B CN 105637058B
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- Prior art keywords
- hotmelt
- component
- polymer
- copolymer
- resin
- Prior art date
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- 239000011347 resin Substances 0.000 claims abstract description 72
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- 239000004743 Polypropylene Substances 0.000 claims abstract description 35
- 125000000524 functional group Chemical group 0.000 claims abstract description 30
- 238000012986 modification Methods 0.000 claims abstract description 19
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- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 4
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Classifications
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- C—CHEMISTRY; METALLURGY
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- C—CHEMISTRY; METALLURGY
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Abstract
本发明提供热熔粘合剂,其具有优异的环境友好性、热稳定性、对聚烯烃基材与聚酯基材的粘合性以及耐热性。本发明涉及热熔粘合剂,其包含:(A)极性官能团改性的共轭二烯类聚合物、(B)脂肪族聚酯类树脂、(C)无定形烯烃类聚合物、(D)结晶聚丙烯树脂、和(E)增粘剂树脂。
Description
技术领域
基于巴黎公约,本申请要求日本专利申请No.2013-221628(2013年10月24日提交)的优先权,并且将所述申请的全部内容通过引用并入本文。
本发明涉及热熔粘合剂,更具体地涉及对诸如聚烯烃与聚酯基材的基材表现出良好的粘合性且特别适合用于汽车内部材料的热熔粘合剂。
背景技术
热熔粘合剂是无溶剂的粘合剂,并且由于粘合剂在被加热熔化后被施加到被粘物,然后通过冷却固化之后显示出粘合性,粘合剂具有能够瞬间粘合与高速粘合的特点。例如,热熔粘合剂目前被广泛用于纸加工、木工、卫生材料、电子领域以及汽车内部材料。
专利文献1公开了用于汽车内部材料的热熔粘合剂,其含有α-烯烃类聚合物作为主要组分(参见,例如[权利要求1]的组分(A))。汽车内部材料的车门装饰板与车顶装饰板常常通过形成诸如丙烯树脂的聚烯烃来得到。因此,在同一文献中公开的热熔粘合剂含有大量的α-烯烃类聚合物,从而提高了对汽车内部材料的粘合性。
此外,具有120℃或更高熔点的结晶聚丙烯被掺合于在同一文献中公开的热熔粘合剂中(见[权利要求1]的组分(B))。作为耐热性改善的结果([0024]),结晶聚丙烯树脂使热熔粘合剂能够更适合诸如汽车内部材料的应用。
然而,有时候聚酯被用在汽车内部材料中,例如在车顶部分的外壳。专利文献1的热熔粘合剂具有优异的聚烯烃基材粘合性,但是对聚酯基材表现出粘合性不足。专利文献1的热熔粘合剂的耐热性也很优异;另一方面,它很可能会经历脆化,从而导致剥离强度不足。
在汽车领域内,由于对环境问题越来越多的关注,用天然材料、植物材料以及可生物降解材料代替从石油衍生的常规原料已经取得了进展。从诸如全球变暖的环境问题的观点出发,由于二氧化碳气体排放的增加,还对于不使用石油作为原料的聚乳酸类树脂进行了研究,涉及汽车内部材料与粘合剂。
专利文献2中公开了含有聚乳酸类树脂与聚丁二酸丁二醇酯或聚丁二酸乙二醇酯的热熔粘合剂。专利文献3中公开了含有聚乳酸与聚乙烯醇类树脂的热熔粘合剂。专利文献4提及热熔粘合剂组合物,其是含有热塑性树脂与增粘剂作为主要成分的组合物,它们中的一种或两种含有聚乳酸,或者由乳酸和其它羟基羧酸衍生的乳酸共聚物树脂。
与聚烯烃类热熔粘合剂相比,聚乳酸类热熔粘合剂的胶粘性、粘合性、热稳定性、耐热性等往往较差。在专利文献2-4中所公开的聚乳酸类热熔粘合剂不适合汽车内部材料应用,因为与在汽车内部材料中使用的聚烯烃基材等的粘合性特别差。
作为增强对聚烯烃基材的粘合性的方法,提出了在聚乳酸类热熔粘合剂中混合聚烯烃的方法。然而,聚乳酸具有难以与聚烯烃混合的问题,并且与“增粘剂树脂”的相容性较差,“增粘剂树脂”是热熔粘合剂的添加剂且具有较差的热稳定性。
文献列表
专利文献
专利文献1:JP 2009-126991A
专利文献2:JP 2010-155951A
专利文献3:JP 2004-256642A
专利文献4:JP 5-339557A
发明内容
技术问题
本发明的目的是解决上述问题,并提供环境友好性高并且热稳定性高的热熔粘合剂,其对聚烯烃基材与聚酯基材具有优异的粘合性,并且还具有优异的耐热性。
解决方案
本发明的优选实施方案如下。
1、热熔粘合剂,其包含:
(A)极性官能团改性的共轭二烯类聚合物,
(B)脂肪族聚酯类树脂,
(C)无定形烯烃类聚合物,
(D)结晶聚丙烯树脂,和
(E)增粘剂树脂。
2、根据上述1的热熔粘合剂,其中,所述极性官能团是选自酸酐基团、马来酸基团、羧基基团、氨基基团、亚氨基基团、烷氧基甲硅烷基基团、硅烷醇基团、甲硅烷基醚基团、羟基基团和环氧基团中的至少一种官能团。
3、根据上述1或2的热熔粘合剂,其中,所述极性官能团改性的共轭二烯类聚合物(A)包含选自氨基基团改性的氢化型苯乙烯嵌段共聚物和马来酸基团改性的氢化型苯乙烯嵌段共聚物中的至少一种。
4、根据上述1-3中任一项的热熔粘合剂,其中,所述脂肪族聚酯类树脂(B)包含聚乳酸类树脂。
5、根据上述1-4中任一项的热熔粘合剂,其中,所述无定形烯烃类聚合物(C)包括乙烯/丙烯/1-丁烯共聚物。
6、根据上述1-5中任一项的热熔粘合剂,其中,基于100重量份的组分(A)至(E)的总重量,结晶聚丙烯树脂(D)的量是3-30重量份。
7、通过施加根据上述1-6中任一项的热熔粘合剂得到的汽车内部材料。
发明的有益效果
根据本发明,在热熔粘合剂内混合极性官能团改性的聚合物能够改善脂肪族聚酯类树脂如聚乳酸类树脂与其它组分的相容性,从而能够提供热熔粘合剂,其是环境友好的,并且还显示出对聚烯烃基材与聚酯基材改进的粘合性,以及热稳定性,其还具有优异的耐热性,并且特别适合于汽车内部材料的应用。
具体实施方案
本发明的热熔粘合剂至少包含:(A)极性官能团改性的共轭二烯类聚合物、(B)脂肪族聚酯类树脂、(C)无定形烯烃类聚合物、(D)结晶聚丙烯树脂,和(E)增粘剂树脂,其也可以分别被称为“组分A”、“组分B”、“组分C”、“组分D”和“组分E”。
如在本文中所用,“改性的聚合物”是指(i)其中官能团是在获得聚合物之后赋予的那些以及(ii)其中官能团在聚合过程中被引入的那些。
<(A)极性官能团改性的共轭二烯类聚合物>
本发明的热熔粘合剂含有极性官能团改性的共轭二烯类聚合物(A)(组分A),因此,脂肪族聚酯类树脂(B)与其它组分,例如无定形烯烃类聚合物(C)、结晶聚丙烯树脂(D)以及增粘剂树脂(E)的相容性得到提高,从而提高了胶粘性、粘合性以及热稳定性。
在本发明中使用的极性官能团改性的共轭二烯类聚合物(A)是指具有至少一个极性官能团的共轭二烯类聚合物。对于引入极性官能团到其上的位置没有特别限制,并且位置可以是在聚合物的端部,或者除了聚合物的端部的内侧。极性官能团可以被赋予至得到的聚合物,或在聚合单体的过程中被引入。
“极性官能团”的实例包括酸酐基团如马来酸酐基团;羧基基团、马来酸基基团、氨基基团、亚氨基基团、烷氧基甲硅烷基基团、硅烷醇基团、甲硅烷基醚基团、羟基基团以及环氧基团。在这些基团中,马来酸酐基团、马来酸基团、氨基基团、环氧基团以及羧基基团是优选的。
“共轭二烯类聚合物”是指包含基于共轭二烯化合物的结构单元(共轭二烯单元)的聚合物。
在本文中,“共轭二烯化合物”是指具有至少一对共轭双键的二烯烃化合物。“共轭二烯化合物”的具体实例包括:例如1,3-丁二烯、2-甲基-1,3-丁二烯(或异戊二烯)、2,3-二甲基-1,3-丁二烯、1,3-戊二烯以及1,3-己二烯。1,3-丁二烯与2-甲基-1,3-丁二烯是特别优选的。这些共轭二烯化合物可以被单独使用或组合使用。
在本发明中,除了共轭二烯单元之外,共轭二烯类聚合物还可以包含基于其它单体的结构单元。其它单体的实例包括乙烯类芳香烃、乙烯腈以及不饱和羧酸酯。
在本发明中,只要本发明的目标热熔粘合剂是可获得的,对于“共轭二烯类聚合物”就没有特别限制。例如,共轭二烯类聚合物优选是由乙烯类芳香烃与共轭二烯化合物的嵌段共聚合得到的共聚物,即含有乙烯类芳香烃嵌段与共轭二烯化合物嵌段的那些。
“乙烯类芳香烃”是指具有乙烯基基团的芳香烃化合物,并且其具体实例包括苯乙烯、邻甲基苯乙烯、对甲基苯乙烯、对叔丁基苯乙烯、1,3-二甲基苯乙烯、α-甲基苯乙烯、乙烯基萘与乙烯基蒽。特别地,苯乙烯是优选的。这些乙烯类芳香烃可以被单独使用或组合使用。
在本发明中,包含极性官能团改性的共轭二烯类聚合物作为A组分的共轭二烯类聚合物可以是非氢化型共轭二烯类聚合物或氢化型共轭二烯类聚合物,并且氢化型共轭二烯类聚合物是更优选的。
“非氢化型共轭二烯类聚合物”的实例包括苯乙烯-异戊二烯-苯乙烯嵌段共聚物(也被称为“SIS”)与苯乙烯-丁二烯-苯乙烯嵌段共聚物(也被称为“SBS”)。“氢化型共轭二烯类聚合物”的实例包括氢化苯乙烯-异戊二烯-苯乙烯嵌段共聚物(也被称为苯乙烯-乙烯/丙烯-苯乙烯嵌段共聚物“SEPS”)与氢化苯乙烯-丁二烯-苯乙烯嵌段共聚物(也被称为苯乙烯-乙烯/丁烯-苯乙烯嵌段共聚物“SEBS”)。其中,组成作为组分A含有的极性官能团改性的共轭二烯类聚合物的共轭二烯类聚合物优选是SEBS,并且更优选具有3-40重量%的苯乙烯含量的SEBS。
“极性官能团改性的共轭二烯类聚合物”的“极性官能团”的实例包括酸酐基团如马来酸酐基团、羧基基团、马来酸基团、氨基基团、亚氨基基团、烷氧基甲硅烷基基团、硅烷醇基团、甲硅烷基醚基团、羟基基团以及环氧基基团。在这些基团中,马来酸基团和氨基基团是更优选的。
关于制备极性官能团改性的共轭二烯类聚合物的方法,其可以通过首先合成共轭二烯类聚合物,然后引入极性官能团来制备,或者通过使用具有极性官能团的单体进行共聚反应来制备。
“极性官能团改性的共轭二烯类聚合物”的实例包括:例如氨基基团改性的SEBS、马来酸基团改性的SEBS等。
在极性官能团改性的共轭二烯类共聚物中,对于引入极性基团如氨基基团或马来酸基团的位置没有特别限制。例如,优选地,至少在共轭二烯类共聚物的一端引入极性基团。
作为极性官能团改性的共轭二烯类共聚物,可以使用可商购的产品,并且其实例包括由Asahi Kasei Chemicals Corporation制备的TAFTEC MP10;由JSR Corporation制备的DYNARON 8630P;以及由Asahi Kasei Chemicals Corporation制备的TAFTEC M1913与TAFTEC M1943。
在本发明中,组分A优选包含具有1.0×104至3.0×105的重均分子量(Mw)的极性官能团改性的聚合物,特别优选具有2.0×104至2.0×105的重均分子量的极性官能团改性的共轭二烯类聚合物。
如在本文中所用,重均分子量通过使用凝胶渗透色谱法(GPC)被测量,通过使用校正曲线换算分子量,所述曲线通过使用具有单分散分子量的聚苯乙烯作为标准参考物质得到。
在本发明的热熔粘合剂中,基于100重量份的组分A-E的总重量,组分A优选以1-20重量份、更优选2-10重量份的量混合。
<(B)脂肪族聚酯类树脂>
本发明的热熔粘合剂包含脂肪族聚酯类树脂(B)(组分B),因此,有可能降低使用石油作为原料的物质的含量,并且提高对聚酯基材的粘合性。由于同时包含脂肪族聚酯类树脂(B)与组分A,可以获得不经历脆化且还具有高剥离强度的热熔粘合剂。
作为脂肪族聚酯类树脂(B),可以使用已知的树脂,并且其实例包括聚乳酸类树脂、聚丁二酸丁二醇酯、聚丁二酸己二酸丁二醇酯(polybutylene succinate adipate)、聚丁二酸对苯二甲酸丁二醇酯(polybutylene succinate terephthalate)、聚丁二酸乙二醇酯、聚丁二酸碳酸丁二醇酯(polybutylene succinate carbonate)、聚乙醇酸、聚己酸内酯、聚羟基丁酸、聚羟基戊酸、羟基丁酸-羟基戊酸共聚物等。其中,聚乳酸类树脂、聚丁二酸丁二醇酯与聚羟基丁酸是优选的,并且聚乳酸树脂和聚丁二酸丁二醇酯是更优选的。这些脂肪族聚酯类树脂可以被单独使用,或者其中两种或多种也可以被组合使用。
聚乳酸类树脂是含有L-乳酸和/或D-乳酸作为主要成分的聚合物,或者可以包含除乳酸以外的其它共聚组分。这些其它共聚组分单元的实例包括多元羧酸、多元醇、羟基羧酸、内酯等,并且其它共聚组分单元的具体实例包括来自多元羧酸,例如草酸、丙二酸、丁二酸、戊二酸、己二酸、壬二酸、癸二酸、十二烷二酸、富马酸、环己烷二羧酸、对苯二甲酸、间苯二甲酸、邻苯二甲酸、2,6-萘二羧酸、蒽二羧酸、间苯二甲酸-5-磺酸钠、以及间苯二甲酸-5-四丁基磺酸鏻(5-tetrabutylphosphonium sulfoisophthalic acid);多元醇,例如乙二醇、丙二醇、丁二醇、庚二醇、己二醇、辛二醇、壬二醇、癸二醇、1,4-环己烷二甲醇、新戊二醇、甘油、季戊四醇、双酚A、双酚与氧化乙烯的加成反应得到的多元芳香醇、二甘醇、三甘醇、聚乙二醇、聚丙二醇以及聚丁二醇;羟基羧酸,例如乙醇酸、3-羟基丁酸、4-羟基丁酸、4-羟基戊酸、6-羟基己酸与羟基苯甲酸;以及内酯,例如乙交酯、ε-己内酯乙交酯、ε-己内酯、β-丙内酯、δ-丁内酯、β-或γ-丁内酯、新戊内酯与δ-戊内酯所衍生的单元。基于100摩尔%的全部单体单元,除了乳酸单元,这些其它共聚组分单元的含量通常在0-30摩尔%、优选0-10摩尔%的范围内调节。
在本发明的热熔粘合剂中,基于100重量份的组分A-E的总重量,组分B优选被包含的量是在5-50重量份、更优选10-35重量份的范围内。
<(C)无定形烯烃类聚合物>
本发明的热熔粘合剂含有无定形烯烃类聚合物(C),因此,对聚烯烃基材的粘合性增大。对聚烯烃基材粘合性的改善使本发明的热熔粘合剂变得适合于生产汽车内部材料以及一次性产品如聚烯烃卫生材料,特别是汽车内部材料。
在本发明中,无定形烯烃类聚合物(C)是指不具有明确熔点的烯烃类聚合物,并且优选在180℃或低于180℃下熔化。在本文中,“无定形”通常是指非晶态,并且更具体地是指其中聚合物分子链不规则排列的状态。
无定形烯烃类聚合物(C)通常被称为无定形聚α-烯烃,并且只要根据本发明的热熔粘合剂是可获得的,其就不特别受限制。
如本文中所使用的,“烯烃类聚合物”是指包括基于烯烃的结构单元的聚合物,并且可以是烯烃均聚物,或者通过与能够和烯烃共聚合的化合物共聚合而得到的共聚物。在本发明中,聚烯烃类共聚物包含50重量%或以上的烯烃,优选80重量%或以上(包括100重量%)的烯烃。烯烃类聚合物可以包含基于能够和烯烃共聚合的化合物的结构单元,优选烯烃类共聚物包含少于50重量%,优选少于20重量%(包括0重量%)的能够和烯烃共聚合的化合物。
本发明的无定形烯烃类聚合物(C)可以是均聚物或共聚物,优选是共聚物,并且优选包含乙烯类共聚物。如在本文中所使用,“乙烯类共聚物”是指乙烯与其它可聚合单体的共聚物。
“其它可聚合单体”是指具有碳原子之间的双键的单体,所述双键可以与乙烯加成聚合。
“其它可聚合单体”的具体实例包括:例如“除乙烯之外的烯烃类烃”以及“具有乙烯双键的羧酸酯”。
“除乙烯之外的烯烃类烃”的实例包括具有3-20个碳原子的α-烯烃,其具体实例包括丙烯、1-丁烯、1-戊烯、1-己烯、1-庚烯、1-辛烯、1-壬烯、1-癸烯、顺-2-丁烯、反-2-丁烯、异丁烯、顺-2-戊烯、反-2-戊烯、3-甲基-1-丁烯、2-甲基-2-丁烯以及2,3-二甲基-2-丁烯。
“具有乙烯双键的羧酸酯”的实例包括(甲基)丙烯酸酯,例如(甲基)丙烯酸甲酯、(甲基)丙烯酸丁酯和(甲基)丙烯酸-2-乙基己酯;以及羧酸乙烯酯与烯丙酯,例如乙酸乙烯酯与乙酸烯丙酯。
这些“其它可聚合单体”可以被单独使用,或者其中两种或更多种可以被组合使用。
在本发明中,乙烯类共聚物优选包含“乙烯与除乙烯之外的烯烃的共聚物”。因此,“其它可聚合单体”优选是“除乙烯之外的烯烃类烃”,特别优选具有3-20个碳原子的α-烯烃,并且更优选丙烯、丁烯或者辛烯。
“乙烯与除乙烯之外的烯烃的共聚物”优选是乙烯与具有3-20个碳原子的α-烯烃的共聚物,具体而言,乙烯与辛烯的共聚物、乙烯与丙烯和1-丁烯的共聚物、乙烯与丙烯的共聚物、乙烯与丁烯的共聚物等,更优选乙烯与辛烯的共聚物、乙烯与丙烯和1-丁烯的共聚物,并且特别优选乙烯与丙烯和1-丁烯的共聚物。这些乙烯与除乙烯之外的烯烃的共聚物可以被单独使用,或者其中两种或更多种可以被组合使用。
可以使用市售产品作为乙烯与除乙烯之外的烯烃的共聚物。
“乙烯与丙烯和1-丁烯的共聚物”的实例包括:例如EVONIK DEGUSSA制备的VESTPLAST 703(商品名)、VESTPLAST 708(商品名)、VESTPLAST 750(商品名)等。
“乙烯与辛烯的共聚物”的实例包括:例如由The Dow Chemical Company制备的AFFINITY GA1900(商品名)、AFFINITY GA1950(商品名)、AFFINITY EG8185(商品名)、AFFINITY EG8200(商品名)、ENGAGE 8137(商品名)、ENGAGE 8180(商品名)、ENGAGE 8400(商品名)等。
“乙烯与丙烯的共聚物”的实例包括:例如由Eastman Chemical Company制备的Eastoflex E1016PL-1等。
在本发明中,乙烯类共聚物可以包含乙烯与至少一种选自“具有乙烯双键的羧酸酯”的共聚物,并且可以使用市售产品。这些共聚物可以被单独使用,或其中两种或更多种可以被组合使用。
“乙烯与具有乙烯双键的羧酸酯的共聚物”的实例包括:例如乙烯-乙酸乙烯酯共聚物、乙烯-甲基丙烯酸甲酯共聚物、乙烯-丙烯酸-2-乙基己酯共聚物、乙烯-丙烯酸丁酯共聚物、乙烯-甲基丙烯酸丁酯共聚物等。这些共聚物中,乙烯-乙酸乙烯酯共聚物和乙烯-甲基丙烯酸甲酯共聚物是更优选的,并且乙烯-乙酸乙烯酯共聚物是特别优选的。
上述的无定形烯烃类聚合物(C)可以被单独使用,或其中两种或更多种可以被组合使用。
在本发明的热熔粘合剂中,基于100重量份的组分A-E的总重量,组分C的量优选是5-60重量份,更优选15-50重量份,并且更优选20-40重量份。当无定形烯烃类聚合物(C)以上述范围内的量被混合时,热熔粘合剂与聚烯烃基材的粘合性提高。
<(D)结晶聚丙烯树脂>
本发明的热熔粘合剂包含结晶聚丙烯树脂(D),因此,耐热性被提高。具有优异耐热性的热熔粘合剂非常适合于需要在夏季高温下的耐久性的汽车内部材料的应用。
在本发明中,结晶聚丙烯树脂(D)是指具有熔点的聚丙烯树脂。在本文中,“结晶”通常是指非无定形的,并且更具体是指其中聚合物分子链是规则排列的状态。
在本发明中,可以使用均聚丙烯、无规聚丙烯及其改性物质作为结晶聚丙烯树脂(D)。
结晶聚丙烯树脂(D)优选具有120℃或更高的熔点,并且更优选为130℃或更高,优选170℃或更低。更优选地,熔点是120℃或更高,并且熔化热的量是50J/g或以上。更优选地,熔点是120℃或更高,熔化热的量是50J/g或以上,并且熔体流量[JIS K7210]是200-1,500(g/10min)。特别优选熔点是120℃或更高,熔化热的量是50J/g或以上,并且熔体流量[JIS K7210]是200-1,200(g/10min)。
在本文中,“熔点”是指用差示扫描量热计(DSC)测得的值。测量试样与标准参考物质之间的热量的差异由差示扫描量热计测量,从而计算出测量样品的熔点。具体地,通过以10℃/min的速度从-50℃升温至220℃,观测到的吸热峰的峰顶被视为熔点。
“熔化热量”是指当物质被熔化时,从外部吸收的热的量,因此是一种潜热。熔化的热量可以由DSC来测量。通常,它是通过熔化1克物质所需要的热量来表示的。
“熔体流速”是指代表树脂的流动性的指标,并且以下面的方式被确定;给定量的合成树脂在230℃下被加热,并且在由加热器加热的圆筒状容器内被加压,然后测量每10分钟内通过设置在容器底部的开口(喷嘴)被挤出的树脂量。使用的单位是“g/10min。”
在本发明的热熔粘合剂中,当结晶聚丙烯树脂(D)具有在上述范围内的熔点和熔体流量时,耐热性被提高,并且将热熔粘合剂施加到聚烯烃基材与聚酯基材还变得容易。
在本发明中,通过使用DSC,无定形烯烃类聚合物(C)也可以与结晶聚丙烯树脂(D)容易地区分。DSC测量使得能够在温度上升时以吸热峰形式观察结晶聚丙烯类树脂(D)的熔点,并且使得能够在温度下降时以放热峰形式观察熔点。由于在用DSC测量时未明确地观察到无定形烯烃类聚合物(C)的熔点,可以将其与结晶聚丙烯树脂(D)相区分。
这些结晶聚丙烯树脂(D)可以被单独使用,或者其中两种或更多种可以被组合使用。
可以使用市售产品作为结晶聚丙烯树脂(D)。市售产品的实例包括:例如由JapanPolypropylene Corporation制备的NOVATEC、由Grand Polymer Co.,Ltd.制备的GrandPolypro、由Prime Polymer Co.,Ltd.制备的Prime Polypro等。
在本发明的热熔粘合剂中,基于100重量份的组分A-E的总重量,组分D的量优选是3-30重量份,更优选5-25重量份,并且更加优选7.5-20重量份。当热熔粘合剂含有在上述范围内的量的结晶聚丙烯树脂(D)时,热熔粘合剂的耐热性被提高,并且将热熔粘合剂施加到基材上还变得容易。
<(E)增粘剂树脂>
本发明的热熔粘合剂含有增粘剂树脂(E)(组分E),因此,胶粘性可以被改善。只要它是在热熔粘合剂中常用的,并且本发明的目标热熔粘合剂是可获得的,对于“增粘剂树脂”就没有特别的限制。
增粘剂树脂的实例包括天然松香、改性松香、氢化松香、天然松香的甘油酯、改性松香的甘油酯、天然松香的季戊四醇酯、改性松香的季戊四醇酯、氢化松香的季戊四醇酯、天然萜的共聚物、天然萜的三元共聚物、氢化萜的共聚物的氢化衍生物、多萜树脂、苯酚类改性萜树脂的氢化衍生物、脂肪族石油烃树脂、脂肪族石油烃树脂的氢化衍生物、芳香族石油烃树脂、芳香族石油烃树脂的氢化衍生物、脂环石油烃树脂以及脂环石油烃树脂的氢化衍生物。这些增粘剂树脂可以被单独使用或组合使用。此外,也可以使用液体类增粘剂树脂作为增粘剂树脂,只要它有无色至淡黄色的色调,并且基本上没有气味,并且还具有良好的热稳定性。全面考虑这些特性,增粘剂树脂优选是树脂的氢化衍生物。
可以使用市售产品作为增粘剂树脂。这些市售产品的实例包括:由MaruzenPetrochemical CO,LTD.制备的MARUKACLEAR H(商品名);由YASUHARA CHEMICAL CO.,LTD.制备的CLEARON K100(商品名);由Arakawa Chemical Industries,Ltd.制备的Alkon M100(商品名);由Idemitsu Petroleum Chemical Co.,Ltd.制备的I-MARV S100(商品名);由YASUHARA CHEMICAL CO.,LTD.制备的CLEARON K4090(商品名)、CLEARON K4100与CLEARONM105(商品名);由Exxon Mobil Corporation制备的ECR 5380(商品名)、ECR 179EX(商品名)、ECR 5400(商品名)以及ECR 5600(商品名);由Eastman Chemical Company制备的Rigarite R7100(商品名)与Eastotac H-100W;由Exxon Corporation制备的ECR179EX(商品名);由Arakawa Chemical Industries,Ltd.制备的Alkon P100(商品名);由IdemitsuKosan Co.,Ltd.制备的I-MARV S110(商品名)、I-MARV Y135(商品名)、I-MARV P100(商品名)以及I-MARV P125(商品名);由Easttack Corporation制备的Easttack C100-R(商品名);以及由Arakawa Chemical Industries,Ltd.制备的KR-85(商品名)。这些市售增粘剂树脂可以被单独使用或组合使用。
在本发明的热熔粘合剂中,基于100重量份的组分A-E的总重量,组分E优选被包含的量是20-60重量份,更优选30-50重量份。
本发明的热熔粘合剂可以包含上述组分A-E,并且优选的实施方案包括其中组分A包含氨基基团改性的共轭二烯类共聚物,组分B包含聚乳酸,组分C包含无定形乙烯类共聚物并且组分D包含结晶聚丙烯树脂的那些。
本发明特别优选的实施方案包括热熔粘合剂,其中组分A包含氨基基团改性的苯乙烯-乙烯/丁烯-苯乙烯嵌段共聚物(“SEBS”),组分B包含聚乳酸,组分C包含乙烯与具有3-20个碳原子的α-烯烃的共聚物,并且组分D包含结晶无规聚丙烯树脂。
本发明的最优选的实施方案包括热熔粘合剂,其中组分A包含氨基基团改性的苯乙烯-乙烯/丁烯-苯乙烯嵌段共聚物(“SEBS”),组分B包含聚乳酸,组分C包含乙烯与丙烯和1-丁烯的共聚物,并且组分D包含具有120℃或更高的熔点的结晶无规聚丙烯树脂。
优选地,除了组分A、组分B、组分C、组分D和组分E之外,本发明的热熔粘合剂还包含(F)稳定剂(在下文也被称为“组分F”)。基于100重量份的组分A-E的总量,组分F的混合比例优选是0.1-2.0重量份,更优选0.2-0.5重量份。
“稳定剂”被使用,以便防止热导致的热熔粘合剂的分子量降低、凝胶化发生、着色、气味等,从而改善热熔粘合剂的稳定性,并且只要本发明的目标热熔粘合剂是可获得的,就没有特别的限制。“稳定剂”的实例包括:例如抗氧化剂和紫外线吸收剂。
“紫外线吸收剂”被使用,从而提高热熔粘合剂的耐光性。“抗氧化剂”被使用,从而防止热熔粘合剂的氧化降解。
抗氧化剂的实例包括:例如酚类抗氧化剂、硫类抗氧化剂与磷类抗氧化剂。紫外线吸收剂的实例包括:例如苯并***类紫外线吸收剂与二苯甲酮类紫外线吸收剂。还可以加入内酯类稳定剂。这些抗氧化剂与紫外线吸收剂可以被单独使用或组合使用。以下产品可以被用作抗氧化剂的市售产品。
其具体实例包括由Sumitomo Chemical Co.Ltd.制备的SUMILIZER GM(商品名)、SUMILIZER TPD(商品名)与SUMILIZER TPS(商品名);由Ciba Specialty Chemicals Inc.制备的IRGANOX 1010(商品名)、IRGANOX HP2225FF(商品名)、IRGAFOS 168(商品名)与IRGANOX 1520(商品名);TINUVIN P;由Johoku Chemical Co.,Ltd.制备的JF77(商品名);由API Corporation制备的TOMINOX TT(商品名);以及由ADEKA Corporation制备的AO-412S(商品名)。这些稳定剂可以被单独使用或组合使用。
本发明的热熔粘合剂还可以含有细颗粒填料。只要细颗粒填料是通常使用的并且本发明的目标热熔粘合剂是可获得的,对于细颗粒填料没有特别的限制。“细颗粒填料”的实例包括云母、碳酸钙、高岭土、滑石、氧化钛、硅藻土、尿素类树脂、苯乙烯珠、焙烧粘土、淀粉等。这些细颗粒填料的形状优选是球形,并且对于尺寸(在球状的情况下是直径)没有特别的限制。
使用公知的热熔粘合剂的制备方法,通过混合组分A、组分B、组分C、组分D与组分E,任选存在的组分F以及各种添加剂(如果需要)来制备根据本发明的热熔粘合剂。例如,热熔粘合剂可以通过混合各规定量的上述组分,然后加热熔化来制备。只要目标热熔粘合剂是可获得的,对于各组分的添加顺序、加热方法等没有特别的限制。
在本发明的优选方面,热熔粘合剂优选地在200℃下具有的粘度(或熔体粘度)是100,000mPa·s或更小,特别优选低于30,000mPa·s。能够使热熔粘合剂均匀涂布的粘度是30,000mPa·s或更小,并且使得热熔粘合剂容易地均匀涂布的粘度小于20,000mPa·s。当热熔粘合剂在200℃下具有上述范围内的粘度时,热熔粘合剂变得更适合涂布。如在本文中所用的,在200℃下的粘度(或熔体粘度)是指通过用27号转子的布氏粘度计(Brookfieldviscometer)测量的值。
根据本发明的热熔粘合剂被广泛用于纸加工、装订、一次性产品、汽车内部材料等,并且由于其对聚烯烃基材与聚酯基材的优异的粘合性,特别有效地用于汽车内部材料。
根据本发明的汽车内部材料通常将基材与被粘物通过使用其间的上述热熔粘合剂彼此层压而制备。在将被粘物层压到作为基材的塑料材料的情况下,热熔粘合剂可以被施加到基材侧或者被粘物侧。在本发明中,汽车内部材料的“基材”优选是聚烯烃或聚酯。对于“被粘物”没有特别的限制,并且优选纤维材料。纤维材料是指其中合成纤维或天然纤维通过使用纺纱机编织纤维而形成片状的材料。
汽车内部材料的具体实例包括车顶材料、后置物板(rear package tray)、车门装饰板、车顶装饰板、底板绝缘体(floor insulator)、行李箱装饰板、前隔板绝缘体(dashinsulator)、护圈(retainer)、支架、卡座等。
不必为制备本发明的汽车内部材料而使用特殊设备。可以通过利用公知的制造设备来制备汽车内部材料,包括传送器、涂布机、压制机、加热器与切割器。
只要目标产品是可获得的,对于热熔粘合剂的涂布方法没有特别的限制。这种涂布方法大致被分为接触式涂布法与非接触式涂布法。“接触式涂布”法是指,在用热熔粘合剂涂布的情况下,其中使排料器与部件或膜接触的涂布方法,而“非接触式涂布”法是指,在用热熔粘合剂涂布的情况下,其中排料器不与部件或膜接触的涂布方法。接触式涂布方法的实例包括:例如槽式涂布机涂布法、辊式涂布机涂布法等,并且非接触式涂布法的实例包括能够以螺旋形式涂布的螺旋涂布、能够以波浪形式涂布的欧米茄涂布或控制缝涂布法、能够以平面形式涂布的槽式喷涂或帘式喷涂法以及能够以点形式涂布的点涂布法。
实施例
出于以更详细、更具体的方式描述本发明的目的,将通过实施例对本发明进行说明。这些实施例仅用于说明性目的,并且不作限定性解释。
在实施例与比较例中,在热熔粘合剂中混合的组分被显示如下。
<(A)极性官能团改性的共轭二烯类聚合物>
(A1)氨基基团改性的SEBS(“DYNARON 8630P”,由JSR Corporation制备)
(A2)马来酸基团改性的SEBS(“TAFTEC M1943”,由Asahi Kasei ChemicalsCorporation制备)
<(B)脂肪族聚酯类树脂>
(B 1)聚-LD-乳酸树脂(“4060D”,由NatureWorks,LLC制备)
(B2)聚-L-乳酸树脂(“4032D”,由NatureWorks,LLC制备)
(B3)聚丁二酸丁二醇酯树脂(“AD92W”,由Mitsubishi Chemical Corporation制备)
<(C)无定形烯烃类聚合物>
(C)丙烯/乙烯/1-丁烯共聚物(“VESTPLAST 703”,由EVONIK DEGUSSA制备)
(C2)丙烯/乙烯/1-丁烯共聚物(“VESTPLAST 750”,由EVONIK DEGUSSA制备)
(C3)乙烯/辛烯共聚物(“AFFINITY GA1950”,由The Dow Chemical Company制备)
<(D)结晶聚丙烯树脂>
(D1)无规聚丙烯聚合物(“Prime Polypro E239”,由Prime Polymer Co.,Ltd.制备)
<(E)增粘剂树脂>
(E1)氢化萜类树脂(“CLEARON P135”,由YASUHARA CHEMICAL CO.,LTD.制备)
(E2)芳香族石油烃树脂的氢化衍生物(I-MARV P125,由Idemitsu Kosan Co.,Ltd.制备)
(E3)芳香族石油烃树脂的氢化衍生物(I-MARV P100,由Idemitsu Kosan Co.,Ltd.制备)
(E4)氢化萜类树脂(“CLEARON M115”,由YASUHARA CHEMICAL CO.,LTD.制备)。
<(F)稳定剂>
(F1)抗氧化剂(“AO-60”,由ADEKA Corporation制备)
根据表1所示的配方混合组分(A)至(F),然后使用通用搅拌器在大约160℃下熔化混合大约3小时,以制备实施例1-8和比较例1-4的热熔粘合剂。关于表1所示的热熔粘合剂的配方(组成)的所有数值均以重量份表示。
关于实施例和比较例中的相应的热熔粘合剂,热稳定性、对多种基材的剥离强度以及剪切强度被评价。下文将对相应的评价的概要进行说明。
<180°剥离强度聚丙烯(PP)板/聚酯无纺布(测量时的温度:23℃或80℃)>
热熔粘合剂的粘合性是根据PP板/聚酯无纺布(“Bonnip”,由Maeda Kosen Co.,Ltd.制备)与被粘物的剥离强度来评价的。热熔粘合剂在空气中于180℃下熔化,然后在20秒的开放时间与0.30g/inch的涂层重量的条件下被施加到PP基材,然后聚酯无纺布层压(基重是300g/m2),以制备样品。
通过使用由ORIENTEC Co.,Ltd.制备的UR-500L Road Cell(最大负载是500kg)以及由ORIENTEC Co.,Ltd.制备的试验机RTM-250,各试样在23℃下被放置在室内1天,然后以300mm/min的行程速度测量180°剥离强度。剥离强度分别在23℃与80℃的温度下被测量。评价标准如下。
(在23℃下测量的剥离强度)
A:超过16kg/inch
B:超过10kg/inch,并且是16kg/inch或更小
C:超过8kg/inch,并且是10kg/inch或更小
D:8kg/inch或更小,或者由于未形成热熔化物而不可测量(在80℃下测量的剥离强度)
A:超过5kg/inch
B:超过2kg/inch并且是5kg/inch或更小
C:超过1kg/inch并且是2kg/inch或更小
D:1kg/inch或更小,或者由于未形成热熔化物而不可测量
<剪切粘合强度(PP/PP 80℃)>
热熔粘合剂的粘合性是根据聚丙烯(PP)对被粘物的拉伸剪切强度来评价的。测量宽25mm、长100mm、厚2mm的条形样品被用作各个被粘物。热熔粘合剂在空气中在180℃下熔化,然后将两个被粘物彼此层压,以便获得各自具有25mm2的涂层面积与2mm的厚度的样品。
通过使用由ORIENTEC Co.,Ltd.制备的UR-500L Road Cell(最大负载是500kg),以及由ORIENTEC Co.,Ltd.制备的试验机RTM-250,各试样在23℃下被放置在室内1天,然后以300mm/min的行程速度测量拉伸剪切强度。测量剪切强度时的温度是80℃。评价标准如下。
A:超过0.5MPa
B:0.3MPa以上并且是0.5MPa或更小
C:0.1MPa以上并且小于0.3MPa
D:小于0.1MPa,或者由于未形成热熔化物而不可测量
<热稳定性>
在70ml玻璃瓶内,装入35g热熔粘合剂,在干燥器中被静置在180℃下24小时后,视觉评价在外观上的变化。
A:未观察到任何相分离、碳化物和环(降解的热熔粘合剂以环的形式沉淀)。
B:观察到非常轻微的相分离、碳化物和环。
C:观察到轻微的相分离、碳化物和环。
D:观察到相分离、碳化物和环。
如表1所示,实施例1-8的热熔粘合剂不大可能经历脆化,并且剥离强度优异,并且还具有对聚烯烃基材与聚酯基材优异的粘合性,因为它们包含所有五种组分,例如组分A、组分B、组分C、组分D和组分E。此外,由于各组分的相容性良好,实施例1-8的热熔粘合剂也具有优异的热稳定性(热稳定性的评价)。因为包含组分B,热熔粘合剂对环境是优选的,并且因为包含组分D,还具有优异的耐热性(剪切强度在80℃下被评价)。
工业实用性
本发明可以提供热熔粘合剂,以及涂布有热熔粘合剂的汽车内部材料。根据本发明的汽车内部材料是特别有效地由聚烯烃基材与聚酯基材制备的汽车内部材料。
Claims (5)
1.热熔粘合剂,其包含:
(A)极性官能团改性的共轭二烯类聚合物,
(B)脂肪族聚酯类树脂,
(C)无定形烯烃类聚合物,
(D)结晶聚丙烯树脂,和
(E)增粘剂树脂。
2.如权利要求1所述的热熔粘合剂,其中,所述极性官能团改性的共轭二烯类聚合物(A)包含选自氨基基团改性的氢化型苯乙烯嵌段共聚物和马来酸基团改性的氢化型苯乙烯嵌段共聚物中的至少一种。
3.如权利要求1或2所述的热熔粘合剂,其中,所述脂肪族聚酯类树脂(B)包括聚乳酸类树脂。
4.通过施加根据权利要求1-3中任一项所述的热熔粘合剂得到的汽车内部材料。
5.汽车内部材料,其包含根据权利要求1-3中任一项所述的热熔粘合剂。
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PCT/JP2014/079003 WO2015060465A1 (en) | 2013-10-24 | 2014-10-24 | Hot melt adhesive |
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EP3995117A1 (en) * | 2013-05-17 | 2022-05-11 | Hollister Incorporated | Biodegradable odor barrier film |
JP6548326B2 (ja) * | 2015-07-30 | 2019-07-24 | 出光興産株式会社 | 低アウトガス性ホットメルト接着剤 |
CA3061335C (en) | 2017-05-22 | 2021-11-30 | H.B. Fuller Company | Hot melt adhesive composition |
JP2019116554A (ja) * | 2017-12-27 | 2019-07-18 | 住友化学株式会社 | 組成物、粘着剤および粘着フィルム |
WO2020049964A1 (ja) * | 2018-09-06 | 2020-03-12 | リケンテクノス株式会社 | ホットメルト接着剤、補強テープ、及び該補強テープを用いて導体端末を補強されたフレキシブルフラットケーブル |
JP7283905B2 (ja) * | 2019-01-23 | 2023-05-30 | ヘンケルジャパン株式会社 | ホットメルト組成物 |
JP6887719B2 (ja) * | 2019-07-29 | 2021-06-16 | アイカ工業株式会社 | ホットメルト組成物 |
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