CN1701107A - 用于聚酯的基于共接枝线性低密度聚乙烯和茂金属聚乙烯以及茂金属聚乙烯的共挤出粘合剂 - Google Patents
用于聚酯的基于共接枝线性低密度聚乙烯和茂金属聚乙烯以及茂金属聚乙烯的共挤出粘合剂 Download PDFInfo
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- CN1701107A CN1701107A CNA038252481A CN03825248A CN1701107A CN 1701107 A CN1701107 A CN 1701107A CN A038252481 A CNA038252481 A CN A038252481A CN 03825248 A CN03825248 A CN 03825248A CN 1701107 A CN1701107 A CN 1701107A
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- 229960004419 dimethyl fumarate Drugs 0.000 description 1
- 150000002009 diols Chemical class 0.000 description 1
- FPAFDBFIGPHWGO-UHFFFAOYSA-N dioxosilane;oxomagnesium;hydrate Chemical compound O.[Mg]=O.[Mg]=O.[Mg]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O FPAFDBFIGPHWGO-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明涉及一种共挤出粘合剂，其包括：5－35％重量的聚合物(A)，聚合物(A)包括80－20％重量的密度为0.863－0.915的茂金属聚乙烯(A1)和20－80％重量的密度为0.9－0.95的非茂金属LLDPE(A2)的混合物，聚合物A1和A2的混合物进行了共接枝；和95－65％重量的茂金属聚乙烯(B)均聚物或共聚物，其共聚单体含有3－20个碳原子，优选4－8个碳原子，其密度为0.863－0.915，其MFI为0.5－30，优选3－15g/10min；合计为100％。A和B的混合物使得其MFI为0.1－15，优选1－13g/10min。
Description
本发明涉及一种粘合到聚酯层上的共挤出粘合剂(tie)，该粘合剂含有共接枝的茂金属聚乙烯(本文以下简称为mPE)和非茂金属线性低密度聚乙烯以及未接枝茂金属聚乙烯的共混物。本发明还涉及含有该粘合剂的多层结构和含有该结构的物体。
到目前为止，用于粘合由PE或聚酯制备的层或薄膜的粘合剂是基于乙烯/(甲基)丙烯酸烷基酯和/或乙烯/醋酸乙烯酯共聚物的。但是，这些粘合剂具有发出强烈气味的缺点，这带来了操作问题。而且，它们的粘附性并不是特别有效并且无论如何不持久。这些粘合剂还具有不允许聚酯或聚烯烃层粘附到EVOH(防渗材料)层上的缺点。
申请人公司的文献FR 2806734公开了一种组合物，该组合物含有用不饱和羧酸或其衍生物共接枝的茂金属聚乙烯和非茂金属线性低密度聚乙烯，所述组合物被稀释到聚乙烯或弹性体中。在此申请中，聚乙烯可以是聚乙烯均聚物或共聚合物，在此情况下为与作为共聚单体的α-烯烃的共聚物，并且该聚乙烯可以是HDPE(高密度聚乙烯)，LDPE(低密度聚乙烯)，VLDPE(甚低密度聚乙烯)型的LLDPE(线性低密度聚乙烯)或是茂金属聚乙烯。当后者证明是茂金属聚乙烯的时候，没有给出关于稀释剂的信息或实例。
申请人公司现在发现了一种粘合剂，该粘合剂不再带来像前一代粘合剂一样的嗅觉问题，而且该粘合剂在其应用中显示出有意义的粘附性，该粘附性一直增加直到达到平台。此外，该粘合剂可粘到EVOH(防渗材料)层上，与乙烯/(甲基)丙烯酸烷基酯或乙烯/醋酸乙烯酯型粘合剂相反。
该粘合剂展示了在现有技术其它文献中没有记载的粘合特性。这些特性稍后将在本文中描述。
该粘合剂在挤出机或其它任何等同设备的出口以颗粒形式回收；申请人公司已经发现该造粒比用于接枝的乙烯/醋酸乙烯酯型粘合剂的造粒要容易得多。
这样该粘合剂使制备不同的结构成为可能，这些结构特别包含聚乙烯层、聚酯层和/或防渗材料层。本领域技术人员会根据所选择的转换方法改变对聚酯的选择。
这些结构在制造软或硬包装时有用，例如袋、瓶、容器、管、共挤出软管或车辆的多层储气罐。
本发明的一个主题是共挤出粘合剂，其含有：
-5-35％重量的聚合物(A)，聚合物(A)本身由80-20％重量的密度为0.863-0.915的茂金属聚乙烯(A1)和20-80％重量的密度为0.900-0.950的非茂金属LLDPE(A2)的共混物组成，聚合物(A1)和(A2)的共混物用选自不饱和羧酸及其衍生物的接枝单体进行共接枝，接枝单体在所述共混物中的含量介于30-100000ppm之间，优选介于600-5000ppm之间；
-95-65％重量的茂金属聚乙烯(B)均聚物或共聚物，其共聚单体含有3-20个碳原子，优选4-8个碳原子，其密度为0.863-0.915，在190℃2.16kg下根据标准ASTMD 1238测量的其熔体流动指数MFI为0.5-30，优选3-15，g/10min；
合计为100％，(A)和(B)的共混物使得其MFI为0.1-15，优选为1-13，g/10min。
根据一个实施方案，该粘合剂的粘合强度在对应于在挤出后立刻应用的时间t＝0和时间t＝8天之间增加了5-50％。
根据一个实施方案，该粘合剂的接枝单体是马来酸酐。
根据一个实施方案，该粘合剂另外含有乙烯/(甲基)丙烯酸烷基酯共聚物(C)。
根据一个实施方案，该粘合剂的(A)的MFI为0.1-5g/10min(ASTMD1238，190℃2.16kg下)。
本发明的另一个主题是多层结构，该多层结构包括含有上述粘合剂的层(L)和直接附着在所述层(L)的两面中的一面上的层(E)，所述层(E)是聚烯烃或聚酯层。
根据一个实施方案，在多层结构中，层(F)直接附着到层(L)的第二个面上，层(L)夹在层(E)和层(F)之间，所述层(F)可以是聚合物层，该聚合物可以选自聚酰胺，乙烯和醋酸乙烯酯的皂化共聚物(EVOH)，聚烯烃和聚酯，或者是金属层。
另外本发明涉及到含有上述结构的物体以及该结构在制备薄膜或片材中的应用。
现在对本发明进行详细介绍。
关于(A1)，术语“茂金属聚乙烯”表示通过乙烯和α-烯烃在单点催化剂存在下共聚合得到的聚合物，该α-烯烃具有3-30个碳原子，优选3-8个碳原子，例如诸如丙烯，丁烯，戊烯，己烯或辛烯。
作为可能共聚单体的具有3-30个碳原子的α-烯烃的例子包括丙烯，1-丁烯，1-戊烯，3-甲基-1-丁烯，1-己烯，4-甲基-1-戊烯，3-甲基-1-戊烯，1-辛烯，1-癸烯，1-十二碳烯，1-十四碳烯，1-十六碳烯，1-十八碳烯，1-二十碳烯，1-二十二碳烯，1-二十四碳烯，1-二十六碳烯，1-二十八碳烯和1-三十碳烯。这些α-烯烃可以单独使用或者使用两种或多于两种的混合物。
单点催化剂通常由一个金属原子和两个结合到该金属原子上的环烷基分子组成，金属原子可以是例如锆或钛。更具体而言，茂金属催化剂通常由结合到该金属上的两个环戊二烯环组成。这些催化剂经常与作为共催化剂或活化剂的铝氧烷一起使用，优选甲基铝氧烷(MAO)。铪也可以用作金属，环戊二烯结合在其上。其它茂金属可以包括来自IVA，VA和VIA的过渡金属。来自镧系的金属也可以使用。
这些茂金属聚乙烯也可以通过它们的
Mw/
Mn比＜3，优选＜2来区别，其中
Mw和
Mn分别表示重均摩尔质量和数均摩尔质量。术语“茂金属聚乙烯”也表示那些具有小于6.53的MFR(熔体流动比)并且Mw/
Mn比大于MFR减去4.63的聚乙烯。MFR表示MFI10(在10kg载荷下的MFI)和MFI2(在2.16kg载荷下的MFI)的比值。其它茂金属聚乙烯通过MFR等于或大于6.13并且
Mw/
Mn比小于或等于MFR减去4.63来定义。
有利地，(A1)的密度介于0.863和0.915之间。mPE(A1)的MFI介于0.5和30g/10min之间(190℃，2.16kg下根据标准ASTM D1238)。
关于(A2)，聚合物(A2)是LLDPE(线性低密度聚乙烯)型的乙烯和α-烯烃的共聚物并且不是茂金属型共聚物。α-烯烃有利地具有3-30个碳原子。这些α-烯烃的列表前面已经给出了。优选具有3-8个碳原子的α-烯烃。
有利地，(A2)的密度在0.900和0.950之间。
(A2)的MFI或熔体流动指数在0.1和8g/10min之间(190℃，2.16kg下根据标准ASTM D1238)。
聚合物(A1)和(A2)的共混物用接枝单体进行接枝，也就是说，聚合物(A1)和(A2)被共接枝。接枝单体选自不饱和羧酸或其官能衍生物。
不饱和羧酸的例子是那些具有2-20个碳原子的羧酸，如丙烯酸，甲基丙烯酸，马来酸，富马酸和衣康酸。这些不饱和羧酸的官能衍生物包括酸酐，酯衍生物，酰胺衍生物，酰亚胺衍生物和这些不饱和羧酸的金属盐(如碱金属盐)。
具有4-10个碳原子的不饱和羧酸和其官能衍生物，尤其是它们的酸酐，是特别优选的接枝单体。
这些接枝单体包括例如马来酸，富马酸，衣康酸，柠康酸，烯丙基琥珀酸，环己4-烯-1，2-二羧酸，4-甲基环己-4-烯-1，2-二羧酸，双环[2.2.1]庚-5-烯-2，3-二羧酸和x-甲基双环[2.2.1]庚-5-烯-2，3-二羧酸及其官能衍生物和马来酸，衣康酸，柠康酸，烯丙基琥珀酸，环己-4-烯-1，2-二羧酸，4-甲基环己-4-烯-1，2-二羧酸，双环[2.2.1]庚-5-烯-2，3-二羧酸和x-甲基双环[2.2.1]庚-5-烯-2，2-二羧酸[原文如此]的酸酐。
其它接枝单体的例子包括不饱和羧酸的C1-C8烷基酯或缩水甘油酯衍生物，例如丙烯酸甲酯，甲基丙烯酸甲酯，丙烯酸乙酯，甲基丙烯酸乙酯，丙烯酸丁酯，甲基丙烯酸丁酯，丙烯酸缩水甘油酯，甲基丙烯酸缩水甘油酯，马来酸一乙酯，马来酸二乙酯，富马酸一甲酯，富马酸二甲酯，衣康酸一甲酯和衣康酸二乙酯；不饱和羧酸的酰胺衍生物，例如丙烯酰胺，甲基丙烯酰胺，马来一酰胺，马来二酰胺，N-一乙基马来酰胺，N，N-二乙基马来酰胺，N-一丁基马来酰胺，N，N-二丁基马来酰胺，富马一酰胺，富马二酰胺，N-一乙基富马酰胺，N，N-二乙基富马酰胺，N-一丁基富马酰胺和N，N-二丁基富马酰胺；不饱和羧酸的酰亚胺衍生物，如马来酰亚胺，N-丁基马来酰亚胺和N-苯基马来酰亚胺；和不饱和羧酸的金属盐，如丙烯酸钠，甲基丙烯酸钠，丙烯酸钾和甲基丙烯酸钾。优选马来酸酐。
各种已知方法可用来将接枝单体接枝到聚合物(A1)和(A2)的共混物上。共混物可含有聚烯烃加工中通常使用的添加剂，含量在10ppm到50000ppm之间，例如基于取代苯酚分子的抗氧剂，UV稳定剂，加工助剂如脂肪酰胺、硬脂酸及其盐，作为防止挤塑缺陷剂的含氟聚合物，胺基防雾剂，防粘连剂如硅土或滑石粉，色母粒和成核剂，等等。
例如，可以通过在高温，约150℃到约300℃，在存在或不存在溶剂以及含有或不含有自由基引发剂的情况下，加热聚合物(A1)和(A2)实施接枝。该反应中可以使用的适当的溶剂是苯，甲苯，二甲苯，氯苯或异丙基苯，等等。可以使用的适当的自由基引发剂包括叔丁基过氧化氢，氢过氧化枯烯，过氧化氢二异丙苯，过氧化二叔丁基，过氧化叔丁基异丙苯，过氧化二枯基，1，3-双(过氧化叔丁基异丙基)苯，过氧化乙酰，过氧化苯甲酰，过氧化异丁酰，双(3，5，5-三甲基-己酰)过氧化物和过氧化甲乙酮。
用上述方法得到的接枝改性的聚合物(A1)和(A2)的共混物中，接枝单体的量可以有利地选择，但优选0.01-10％重量，即优选600ppm-5000ppm，相对于共接枝的(A1)和(A2)的重量。
接枝单体的量通过利用FTIR光谱定量测量琥珀酸官能团而确定。(A)即(A1)和(A2)共接枝的共混物，其熔体流动指数MFI为0.1-15g/10min(ASTM D1238，190℃，2.16kg)，有利地为0.1-5g/10min，优选为0.1-3g/10min。
关于聚乙烯(B)，它是茂金属聚乙烯均聚物或共聚物，在此情况下共聚物是与选自具有3-20个碳原子，优选4-8个碳原子的α-烯烃的共聚单体的共聚物。
具有3-20个碳原子的α-烯烃的例子包括丙烯，1-丁烯，1-戊烯，3-甲基-1-丁烯，1-己烯，4-甲基-1-戊烯，3-甲基-1-戊烯，1-辛烯，1-癸烯，1-十二碳烯，1-十四碳烯，1-十六碳烯，1-十八碳烯或1-二十碳烯。这些α-烯烃可以单独使用或者使用两种或者多于两种的混合物。
茂金属聚乙烯(B)的密度在0.863和0.915之间，MFI(190℃，2.16kg下根据标准ASTM D1238测量)为0.5-30g/10min，优选为3-15g/10min。
共挤出粘合剂的MFI为0.1-15g/10min，优选1-13g/10min(ASTMD1238，190℃，2.16kg)。
本发明的粘合剂可用于多层结构，例如诸如薄膜、片材、管材和空心体。
本发明的多层结构包括含有上述粘合剂的层(L)和直接附着到所述层(L)的第一个面上的层(E)。层(E)是一个选自聚烯烃和聚酯的聚合物层。
层(F)也可以直接附着到层(L)的第二个面上，层(L)夹在层(E)和(F)之间，所述层(F)可以是聚合物层，该聚合物选自聚酰胺和皂化的乙烯和醋酸乙烯酯共聚物(EVOH)，或者是金属层。
但是，多层结构也可以包括夹在两个层(F)之间含有粘合剂的层(L)。
通过举例的方式可以列出如下结构：PA表示聚酰胺，L表示粘合剂，PE表示聚乙烯，PET表示聚对苯二甲酸乙二酯，EVOH表示皂化的乙烯和醋酸乙烯酯共聚物：
-层(E)/层(L)/层(F)型结构：PE/L/EVOH/PET，PE/L/PA或PE/L/PA/L/PE；和
-层(E)/层(L)/层(E)和层(F)/层(L)/层(F)型结构：PET/L/PE，PE/L/PE，PET/L/PET或PA/L/PA，
-混合结构：PE/L/EVOH/L/PA。
更具体而言，聚酰胺是长链合成聚酰胺，在主链中具有酰胺基团结构单元，如PA-6，PA-6，6，PA-6，10，PA-11，PA-6/6，6和PA-12。
皂化的乙烯和醋酸乙烯酯共聚物的皂化度约是90-100mol％，通过对乙烯含量约15-约60mol％的乙烯/醋酸乙烯酯共聚物进行皂化得到。
聚酯是均聚或共聚物。均聚酯可以取自聚对苯二甲酸乙二酯，聚对苯二甲酸丁二酯和聚萘二甲酸乙二酯或芳香族聚酯，如聚合物液晶。
本发明使用的合适的共聚酯可以形成自芳香族二羧酸，二羧酸酯，二羧酸酸酐，二醇或它们的混合物。部分形成自如下重复单元的芳香族共聚酯也适合，重复单元包括对苯二甲酸，对苯二甲酸二甲酯，间苯二甲酸，间苯二甲酸二甲酯，2，6-萘二甲酸二甲酯，2，6-萘二甲酸，1，2-，1，3-和1，4-亚苯基二氧二乙酸，乙二醇，二甘醇，1，4-环己烷二甲醇，1，4-丁二醇或它们的混合物。
优选地，聚酯的结构包括以下重复单元：对苯二甲酸，对苯二甲酸二甲酯，间苯二甲酸，间苯二甲酸二甲酯和/或2，6-萘二甲酸二甲酯。聚酯的二羧酸可以用一种或多种不同的二羧酸(优选最多达到约20mol％)改性。这种二羧酸包括芳香族二羧酸，优选具有8-14个碳原子，脂肪族二羧酸，优选具有4-12个碳原子或环脂族二羧酸，优选具有8-12个碳原子。二羧酸的例子有：对苯二甲酸，邻苯二甲酸，间苯二甲酸，萘-2，6-二甲酸，环己烷二甲酸，环己烷二乙酸，4，4’-联苯二甲酸，琥珀酸，戊二酸，己二酸，壬二酸，癸二酸或它们的混合物。
此外，二醇可被除乙二醇以外的一种或多种不同的二醇(优选最高达到约20mol％)改性。这样的二醇包括：环脂族二醇，优选具有6-20个碳原子或脂肪族二醇，优选具有25[原文如此]-20个碳原子。这样的二醇的例子包括：二甘醇，三甘醇，1，4-环己烷二甲醇，1，3-丙二醇，1，4-丁二醇，1，5-戊二醇，1，6-己二醇，3-甲基-2，4-戊二醇，2-甲基-1，4-戊二醇，2，2，4-三甲基-1，3-戊二醇，2-乙基-1，3-己二醇，2，2-二乙基-1，3-丙二醇，1，3-己二醇，1，4-二(羟乙氧基)苯，2，2-双(4-羟基环己基)丙烷，2，4-二羟基-1，1，3，3-四甲基环丁烷，2，2-双(3-羟乙氧基苯基)丙烷，2-双(4-羟丙氧基苯基)丙烷[原文如此]，(羟乙基)间苯二酚或它们的混合物。可以采用两种或者多于两种上述的二醇制备聚酯。
金属层可以是例如金属的薄膜或片材，金属是例如铝，铁，铜，锡和镍，或是含有至少一种所述金属作为主要成分的合金。薄膜或片材的厚度可以适当地选择，例如约0.01-约0.2mm。在把本发明的粘合剂轧制到金属层上之前通常对金属层表面进行脱脂。
形成本发明结构的不同层的组合物可含有添加剂，例如填料，稳定剂，增滑剂，抗静电剂或阻燃剂。
本发明的结构可以通过热塑性领域公知的共挤出，挤压吹塑，热成型，薄膜涂布或轧制方法来制造。
本发明的粘合剂组合物(实施例1-4)和对比组合物(对比例1-7)归纳在下面的表1中。
在t0(时间＝0，此时粘合剂刚被挤出并被施用到测试样本上)和在t8(对应于时间＝8天)时的剥离强度F(N/15mm)归纳在下面的表2中。这些测试所用的薄膜是共挤出薄膜，对情况1薄膜由3层组成：PET层/粘合剂层(L)/PE层，每层的厚度分别为150/30/350μm，对情况2和3薄膜由5层组成：PET层/粘合剂层(L)/EVOH层/粘合剂层(L)/PE层，每层的厚度分别为150/30/20/30/300μm。
剥离测试在温度T为25℃、剥离速率为200mm/min下进行。使用来自Eastman的Voridian9921WPET，来自Atofina的LacqteneLD0304LDPE和来自Nippon G0hsei的含38％乙烯的SoarnolEVOH来制备这些薄膜。符号σ对应于标准偏差。
表1
| 实施例1 | 实施例2 | 实施例3 | 实施例4 | ||||||
| 共接枝聚合物(A)的特性 | PE类型 | mPE | LLDPE | mPE | LLDPE | mPE | LLDPE | mPE | LLDPE |
| 密度(g/cm3) | 0.87 | 0.92 | 0.87 | 0.92 | 0.87 | 0.92 | 0.87 | 0.92 | |
| 共聚单体 | 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 | |
| 组成 | 50％ | 50％ | 50％ | 50％ | 50％ | 50％ | 50％ | 50％ | |
| 接枝度 | 0.9％ | 0.9％ | 0.9％ | 0.9％ | |||||
| 接枝单体 | MAH | MAH | MAH | MAH | |||||
| MFI(g/10min)190℃，2.16kg | 0.7 | 0.7 | 0.7 | 0.7 | |||||
| (A)的比例 | 15％ | 25％ | 15％ | 25％ | |||||
| 聚合物(B)的特性 | mPE类型 | E/1-辛烯 | E/1-辛烯 | E/1-辛烯 | E/1-辛烯 | ||||
| 密度(g/cm3) | 0.870 | 0.870 | 0.902 | 0.902 | |||||
| MFI(g/10min)190℃，2.16kg | 5 | 5 | 10 | 10 | |||||
| (B)的比例 | 85％ | 75％ | 85％ | 75％ | |||||
| (A)和(B)共混物的MFI | 3 | 2.5 | 5.5 | 4.5 | |||||
续表1
| 对比例1 | 对比例2 | 对比例3 | 对比例4 | ||||
| mPE | LLDPE | mPE | LLDPE | mPE | LLDPE | mPE | LLDPE |
| 0.87 | 0.92 | 0.87 | 0.92 | 0.87 | 0.92 | 0.87 | 0.92 |
| 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 |
| 50％ | 50％ | 50％ | 50％ | 50％ | 50％ | 50％ | 50％ |
| 0.9％ | 0.9％ | 0.9％ | 0.9％ | ||||
| MAH | MAH | MAH | MAH | ||||
| 0.7 | 0.7 | 0.7 | 0.7 | ||||
| 25％ | 25％ | 15％ | 25％ | ||||
| E/丙烯酸甲酯 | E/醋酸乙烯酯 | E/丙烯酸甲酯和mPE** | VLDPE(E/1-辛烯) | ||||
| 0.943 | 0.950* | 0.943和0.902** | 0.911 | ||||
| 8 | 20和3* | 8和10** | 6.6 | ||||
| 75％ | 75％ | 85％** | 75％ | ||||
*37.5％MFI＝20、密度＝0.950的乙烯/醋酸乙烯酯共聚物，和37.5％MFI＝3、密度＝0.950的乙烯/醋酸乙烯酯共聚物；
**42.5％MFI＝8、密度＝0.943的乙烯/丙烯酸甲酯共聚物，和42.5％MFI＝10、密度＝0.902的以1-辛烯为共聚单体的mPE；
续表1
| 对比例5 | 对比例6 | 对比例7 | |||
| mPE | LLDPE | mPE | LLDPE | mPE | LLDPE |
| 0.87 | 0.92 | 0.87 | 0.92 | 0.87 | 0.92 |
| 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 | 1-辛烯 | 1-丁烯 |
| 50％ | 50％ | 50％ | 50％ | 50％ | 50％ |
| 0.9％ | 0.9％ | 0.9％ | |||
| MAH | MAH | MAH | |||
| 0.7 | 0.7 | 0.7 | |||
| 25％ | 25％ | 25％ | |||
| LLDPE(E/1-辛烯) | LDPE | HDPE | |||
| 0.919 | 0.924 | 0.955 | |||
| 4.4 | 2 | 4 | |||
| 75％ | 75％ | 75％ | |||
表2
| 情况1 | 情况2 | 情况3 | ||||||||||
| 在t0时的FN/15mm | σ | 在t8时的FN/15mm | σ | 在t0时的FN/15mm | σ | 在t8时的FN/15mm | σ | 在t0时的FN/15mm | σ | 在t8时的FN/15mm | σ | |
| 实施例1 | 13.4 | 0.5 | 16.7 | 0.7 | 8.2 | 0.2 | 10.7 | 0.1 | - | - | - | - |
| 实施例2 | 14.2 | 0.5 | 17.8 | 0.4 | 10.6 | 0.3 | 12.8 | 0.4 | - | - | - | - |
| 实施例3 | 11.6 | 0.6 | 15.1 | 3.4 | 8.5 | 0.1 | 10.1 | 0.2 | - | - | - | - |
| 实施例4 | 12.5 | 0.8 | 20.1 | 1.8 | 10.4 | 0.2 | 12.1 | 0.3 | - | - | - | - |
| 对比例1 | 6 | 0.5 | 5.6 | 0.4 | - | - | - | - | 5.8 | 0.5 | 5.2 | 0.4 |
| 对比例2 | 6.1 | 0.5 | 6.6 | 0.9 | - | - | - | - | 5.7 | 0.2 | 5.8 | 0.4 |
| 对比例3 | 6.5 | 0.9 | 6.8 | 0.8 | - | - | - | - | 6.2 | 0.9 | 6.1 | 0.8 |
| 对比例4 | 4.4 | 2.1 | 1.3 | 0.2 | - | - | - | - | 4.1 | 1 | 2.1 | 0.2 |
| 对比例5 | 3.2 | 0.3 | 1.2 | 0.2 | - | - | - | - | 3.2 | 0.1 | 1.4 | 0.2 |
| 对比例6 | 2.6 | 0.2 | 1 | 0.1 | - | - | - | - | 2.7 | 0.2 | 1.2 | 0.1 |
| 对比例7 | 1.2 | 0.1 | 0.5 | 0.1 | - | - | - | - | 1 | 0.1 | 0.6 | 0.1 |
情况1：PET层和粘合剂层(L)之间不能剥离
情况2：EVOH层和粘合剂层(L)之间不能剥离
情况3：PET层和粘合剂层(L)之间不能剥离
Claims (11)
1.一种共挤出粘合剂，其含有：
-5-35％重量的聚合物(A)，聚合物(A)本身由80-20％重量的密度为0.863-0.915的茂金属聚乙烯(A1)和20-80％重量的密度为0.900-0.950的非茂金属LLDPE(A2)的共混物组成，聚合物(A1)和(A2)的共混物用选自不饱和羧酸及其衍生物的接枝单体进行共接枝，在所述共混物中接枝单体的含量为30-100000ppm，优选600-5000ppm；
-95-65％重量的茂金属聚乙烯(B)均聚物或共聚物，其共聚单体含有3-20个碳原子，优选4-8个碳原子，其密度为0.863-0.915，在190℃2.16kg下根据标准ASTMD 1238测量的其熔体流动指数MFI为0.5-30，优选3-15，g/10min；
合计为100％，(A)和(B)的共混物使得其MFI为0.1-15，优选1-13，g/10min。
2.如权利要求1所述的粘合剂，其粘合强度在对应于在挤出后立刻应用的时间t＝0和时间t＝8天之间增加了5-50％。
3.如前述任意一项权利要求所述的粘合剂，其接枝单体是马来酸酐。
4.如权利要求1所述的粘合剂，其另外含有乙烯/(甲基)丙烯酸烷基酯共聚物(C)。
5.如前述任意一项权利要求所述的粘合剂，其中A的MFI为0.1-5g/10min(ASTMD 1238，190℃，2.16kg)。
6.一种多层结构，其包括含有任意一项前述权利要求所述的粘合剂的层(L)和直接附着到所述层(L)的两个表面中的一个表面上的层(E)，所述层(E)是聚烯烃或聚酯层。
7.如权利要求6所述的多层结构，其中层(F)直接附着到层(L)的第二个表面上，层(L)夹在层(E)和(F)之间，所述的层(F)可以是聚合物层，该聚合物选自聚酰胺、皂化的乙烯和醋酸乙烯酯共聚物(EVOH)、聚烯烃和聚酯，或者是金属层。
8.如权利要求7所述的多层结构，其中层(E)是聚酯共聚物层且层(F)是EVOH层。
9.含有如权利要求6-8任意一项所述的结构的物体。
10.如权利要求9所述的物体，其是袋、瓶、容器、管或软管。
11.如权利要求6-8任意一项所述的结构在制备薄膜或片材中的应用。
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| FR0211992A FR2845094B1 (fr) | 2002-09-27 | 2002-09-27 | Liant de coextrusion pour polyester a base de polyethylene metallocene et lldpe cogreffes et de polyethylene metallocene |
| FR02/11992 | 2002-09-27 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1701107A true CN1701107A (zh) | 2005-11-23 |
| CN1302082C CN1302082C (zh) | 2007-02-28 |
Family
ID=31985293
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CNB038252481A Expired - Lifetime CN1302082C (zh) | 2002-09-27 | 2003-09-26 | 用于聚酯的基于共接枝线性低密度聚乙烯和茂金属聚乙烯以及茂金属聚乙烯的共挤出粘合剂 |
Country Status (14)
| Country | Link |
|---|---|
| US (1) | US7794806B2 (zh) |
| EP (1) | EP1543089B1 (zh) |
| JP (2) | JP4879489B2 (zh) |
| KR (1) | KR100695042B1 (zh) |
| CN (1) | CN1302082C (zh) |
| AT (1) | ATE463546T1 (zh) |
| AU (1) | AU2003299097B8 (zh) |
| CA (1) | CA2500208C (zh) |
| DE (1) | DE60332031D1 (zh) |
| DK (1) | DK1543089T3 (zh) |
| ES (1) | ES2342934T3 (zh) |
| FR (1) | FR2845094B1 (zh) |
| PT (1) | PT1543089E (zh) |
| WO (1) | WO2004029173A1 (zh) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101781446A (zh) * | 2010-03-22 | 2010-07-21 | 福建师范大学 | 一种聚对苯二甲酸乙二醇酯瓶回收料制备塑料管件的方法 |
| CN102294867A (zh) * | 2011-07-13 | 2011-12-28 | 佛山新长盛塑料薄膜有限公司 | 一种光学级自粘性聚乙烯保护膜及其制备方法 |
| CN106574156A (zh) * | 2014-08-06 | 2017-04-19 | 伊奎斯塔化学有限公司 | 聚烯烃基组合物、粘合剂以及由其制备的相关多层结构 |
| CN107759893A (zh) * | 2017-11-17 | 2018-03-06 | 南京棠城塑胶有限公司 | 一种pbt/pe流延复合薄膜粘接用材料的制备方法 |
Families Citing this family (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP1557256A1 (en) * | 2004-01-26 | 2005-07-27 | Arkema | Copolyester-based structure for manufacturing transparent hollow bodies by coextrusion blow-molding |
| JP5208512B2 (ja) | 2004-11-30 | 2013-06-12 | アーケマ・インコーポレイテッド | 流体輸送用物体に有用なアロイ組成物 |
| FR2896249A1 (fr) * | 2006-01-16 | 2007-07-20 | Arkema Sa | Liant a base de polyethylene greffe et de polystyrene choc ou cristal a rupture cohesive |
| KR101360366B1 (ko) * | 2007-12-14 | 2014-02-11 | 삼성에스디아이 주식회사 | 전극조립체 및 이를 구비하는 이차 전지 |
| EP2855150B1 (en) * | 2012-06-05 | 2016-09-14 | Dow Global Technologies LLC | Films containing functional ethylene-based polymer compositions |
| EP2890556B1 (en) * | 2012-08-28 | 2022-08-03 | Dow Brasil Indústria e Comércio de Produtos Químicos Ltda. | Films containing functional ethylene-based polymer compostions |
| EP2938490B1 (en) * | 2012-12-28 | 2020-04-15 | Dow Global Technologies LLC | Multilayer films containing functional ethylene-based polymer compositions |
| KR101316941B1 (ko) * | 2013-05-03 | 2013-10-18 | 주식회사 애트 | 핫팩에 적용되는 통기성 필름 조성물 및 이를 포함하는 핫팩용 통기성 필름의 제조방법 |
| FR3014891B1 (fr) * | 2013-12-18 | 2016-11-04 | Arkema France | Liant pour structure multicouche |
| US20150344744A1 (en) * | 2014-05-30 | 2015-12-03 | Equistar Chemicals, Lp | Tie-layer adhesives having improved adhesion and melt strength |
| ES2927248T3 (es) * | 2017-05-31 | 2022-11-03 | Univation Tech Llc | Combinaciones de polietilenos de baja densidad lineales |
Family Cites Families (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP3337777B2 (ja) * | 1993-10-05 | 2002-10-21 | 昭和電工株式会社 | 接着性樹脂組成物 |
| JPH0841261A (ja) * | 1994-07-29 | 1996-02-13 | Ube Ind Ltd | 接着性ポリエチレン組成物 |
| CA2175609C (en) * | 1995-05-12 | 2004-06-22 | Hata, Nobuhiko | Fuel tank |
| US5709915A (en) * | 1995-08-04 | 1998-01-20 | Reynolds Consumer Products, Inc. | Adhesive structure for heat sealing |
| JP2000007859A (ja) * | 1998-06-19 | 2000-01-11 | Mitsubishi Chemicals Corp | ポリエチレン系樹脂組成物 |
| FR2788528B1 (fr) * | 1999-01-19 | 2001-02-16 | Atochem Elf Sa | Composition a base d'un copolymere de l'ethylene et de l'alcool vinylique et son utilisation |
| ES2265886T3 (es) * | 1999-04-06 | 2007-03-01 | Arkema France | Ligante de coextrusion, su utilizacion para una estructura multicapa yla estructura asi obtenida. |
| ATE256720T1 (de) * | 1999-04-06 | 2004-01-15 | Atofina | Koextrusionbindung, die verwendung für eine multischichtstruktur und die struktur hergestellt davon |
| EP1122060A1 (en) * | 2000-02-07 | 2001-08-08 | Atofina | Multilayer structure and tank consisting of this structure, which has a barrier layer in direct contact with the fluid contained |
| FR2806734A1 (fr) * | 2000-03-24 | 2001-09-28 | Atofina | Liant de coextrusion a base de polyethylene metallocene cogreffe |
-
2002
- 2002-09-27 FR FR0211992A patent/FR2845094B1/fr not_active Expired - Fee Related
-
2003
- 2003-09-26 KR KR1020057005307A patent/KR100695042B1/ko active IP Right Grant
- 2003-09-26 AT AT03798232T patent/ATE463546T1/de not_active IP Right Cessation
- 2003-09-26 AU AU2003299097A patent/AU2003299097B8/en not_active Ceased
- 2003-09-26 EP EP20030798232 patent/EP1543089B1/fr not_active Expired - Lifetime
- 2003-09-26 US US10/671,758 patent/US7794806B2/en not_active Expired - Lifetime
- 2003-09-26 DK DK03798232T patent/DK1543089T3/da active
- 2003-09-26 JP JP2004539149A patent/JP4879489B2/ja not_active Expired - Lifetime
- 2003-09-26 WO PCT/FR2003/002850 patent/WO2004029173A1/fr active Application Filing
- 2003-09-26 PT PT03798232T patent/PT1543089E/pt unknown
- 2003-09-26 ES ES03798232T patent/ES2342934T3/es not_active Expired - Lifetime
- 2003-09-26 CN CNB038252481A patent/CN1302082C/zh not_active Expired - Lifetime
- 2003-09-26 DE DE60332031T patent/DE60332031D1/de not_active Expired - Lifetime
- 2003-09-26 CA CA2500208A patent/CA2500208C/fr not_active Expired - Lifetime
-
2008
- 2008-12-01 JP JP2008306525A patent/JP2009102642A/ja active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101781446A (zh) * | 2010-03-22 | 2010-07-21 | 福建师范大学 | 一种聚对苯二甲酸乙二醇酯瓶回收料制备塑料管件的方法 |
| CN102294867A (zh) * | 2011-07-13 | 2011-12-28 | 佛山新长盛塑料薄膜有限公司 | 一种光学级自粘性聚乙烯保护膜及其制备方法 |
| CN102294867B (zh) * | 2011-07-13 | 2012-11-07 | 佛山新长盛塑料薄膜有限公司 | 一种光学级自粘性聚乙烯保护膜及其制备方法 |
| CN106574156A (zh) * | 2014-08-06 | 2017-04-19 | 伊奎斯塔化学有限公司 | 聚烯烃基组合物、粘合剂以及由其制备的相关多层结构 |
| CN106574156B (zh) * | 2014-08-06 | 2018-11-09 | 伊奎斯塔化学有限公司 | 聚烯烃基组合物、粘合剂以及由其制备的相关多层结构 |
| CN107759893A (zh) * | 2017-11-17 | 2018-03-06 | 南京棠城塑胶有限公司 | 一种pbt/pe流延复合薄膜粘接用材料的制备方法 |
Also Published As
| Publication number | Publication date |
|---|---|
| ES2342934T3 (es) | 2010-07-19 |
| AU2003299097A1 (en) | 2004-04-19 |
| CA2500208A1 (fr) | 2004-04-08 |
| PT1543089E (pt) | 2010-05-10 |
| JP4879489B2 (ja) | 2012-02-22 |
| EP1543089B1 (fr) | 2010-04-07 |
| DE60332031D1 (de) | 2010-05-20 |
| CN1302082C (zh) | 2007-02-28 |
| KR100695042B1 (ko) | 2007-03-14 |
| CA2500208C (fr) | 2012-06-05 |
| FR2845094B1 (fr) | 2006-05-05 |
| ATE463546T1 (de) | 2010-04-15 |
| AU2003299097B2 (en) | 2007-12-06 |
| WO2004029173A1 (fr) | 2004-04-08 |
| DK1543089T3 (da) | 2010-06-21 |
| KR20050048656A (ko) | 2005-05-24 |
| US7794806B2 (en) | 2010-09-14 |
| JP2009102642A (ja) | 2009-05-14 |
| EP1543089A1 (fr) | 2005-06-22 |
| JP2006500454A (ja) | 2006-01-05 |
| FR2845094A1 (fr) | 2004-04-02 |
| US20050019516A1 (en) | 2005-01-27 |
| AU2003299097B8 (en) | 2008-04-24 |
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