CN103124626A - 具有阻挡性能的多层塑料物品及其生产方法 - Google Patents

具有阻挡性能的多层塑料物品及其生产方法 Download PDF

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CN103124626A
CN103124626A CN2011800455919A CN201180045591A CN103124626A CN 103124626 A CN103124626 A CN 103124626A CN 2011800455919 A CN2011800455919 A CN 2011800455919A CN 201180045591 A CN201180045591 A CN 201180045591A CN 103124626 A CN103124626 A CN 103124626A
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layer
barrier properties
polymer
extruding
hydro carbons
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D·尤利茨
R·赫尔米格
H·莱曼
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Kautex Textron GmbH and Co KG
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Abstract

本发明涉及多层塑料物品，包括基于非极性聚烯烃的至少两层，和位于所述两层之间且与之直接接触的对烃类具有阻挡性能的层，和还涉及其生产方法。

Description

具有阻挡性能的多层塑料物品及其生产方法
本发明涉及多层塑料物品，它包括基于非极性聚烯烃的至少两层和包括位于所述两层之间并与之接触的对烃类具有阻挡性能的层，本发明还涉及其生产方法。
当今由塑料制成的容器被广泛用于运输和储存危险的液体和气体产品，因为它们具有耐化学性，机械强度，良好的可加工性，具体地包括在复杂成型工艺中的加工性，和低重量。在车辆的构造中，作为例举，由塑料制成的燃料容器几乎完全替代了先前常规的金属燃料容器。当今，便携式或非-固定的容器，例如用于可燃液体和类似物的汽油罐(petrol canister)，瓶子，圆筒和油箱也几乎仅仅由塑料生产。特别地在较低重量/体积比，避免腐蚀问题和低成本生产中发现塑料容器的特别的优点。
具体地，在所述应用部分中，对位于容器/油箱内部内的液体和/或气体不可渗透是重要的。因此，作为例举，当今塑料容器必须符合就烃的渗透而言的严格的排放法规。
聚烯烃树脂，例如聚乙烯，聚丙烯及其共聚物，具有非常良好的可模塑性和可加工性以及高的机械强度。然而，它们对挥发性的非极性有机物质，尤其烃类的渗透性相对高。因此，重要的是提供运输和/或储存包括烃类，例如汽油或柴油在内的危险物质用容器合适的处理。尤其借助氟化，涂布或等离子聚合，由这些聚烯烃制造的塑料容器的阻挡性能可得到显著改进。
表面改性和涂布方法的通常的缺点是，阻挡层必然施加在容器的内部和/或外部表面上，因此未受保护地暴露于环境影响下。因此，随着时间流逝，可出现上述阻挡层的分离和/或化学改变，和这自然会导致阻挡性能的显著损害。
因此，目前的研发主要集中在例如通过共挤出工艺，生产并构造多层体系，其中具有阻挡性能的聚合物，主要是乙烯-乙烯醇共聚物(EVOH)和聚酰胺(PA)与聚烯烃和其他成分一体化，得到多层复合材料。阻挡聚合物的常见位置大致是容器壁的中间；这导致的第一结果是最小化在阻挡聚合物内产生的弯曲应力，其中当施加机械负载时，所述阻挡聚合物大多数相对脆，和第二结果是，基体材料保护阻挡聚合物避免环境影响。同样可能的情况是使用共挤出技术，将仍然进一步的层一体化到多层复合材料内，和因此这一方法得到仅仅使用单一聚合物不可能实现的具有宽泛的各种有利性能的材料。
然而，缺点是通常作为具有阻挡性能使用的聚合物，例如乙烯-乙烯基共聚物和聚酰胺通常具有极性，且相对于非极性的基础材料，例如聚乙烯和聚丙烯，不具有任何种类的粘合性能。即使在熔融状态下共挤出所述材料的两层并“粘合”到彼此上，在冷却工艺之后或者更早，它们也分离成两个空间分离的层。
因此，使用共挤出，在由低成本的聚烯烃制造的基础材料制成的层和由明显更加昂贵的阻挡聚合物制成的阻挡层(它所使用的层厚因此也最小化)之间引入粘合促进层，所述粘合促进层确保在其他情况下不相容的极性和非极性层耐久粘结。作为例举，当今，在机动车辆部分内的容器通常具有通过共挤出获得的六层结构，所述六层结构包括(从容器的内侧到外侧)由“原始(virgin)”的HDPF制成的基础层，包括循环材料，例如再粉碎材料(实质上同样是HDPE)或由其组成的粉碎材料层，粘合促进层，阻挡层，另一粘合促进层和由“原始”HDPE制成的另一层。
然而，例如对于两个额外的挤出机来说，引入至少两层额外的粘合促进层到共挤出物内的装置成本，以及挤出工艺所使用的体系的其他昂贵的重新建造也具有对这类体系的基本建设费用成本巨大增加的影响。
另一方法提供使用聚芳基酰胺作为阻挡材料，再者此处需要粘合促进剂，以便确保稳定粘结到基于聚烯烃的基础材料上。然而，在这一情况下，在基础材料和阻挡层之间的两个独立层内没有施加粘合促进剂，而是在加工之前，将其加入到基础材料中。然而，这一方法要求非常大量的粘合促进剂，这同样昂贵。
因此，本发明的一个目的是在没有损害塑料物品阻挡性能的情况下，提供简化的工艺，该工艺就材料成本和/或基本建设费用来说是有利的，所述成本和/或费用随着生产具有阻挡性能的多层塑料物品用的每一挤出层的增加而升高。而且还应当优选对塑料物品的耐化学性，耐热性或机械强度没有损害。
令人惊奇地，现已发现，允许生产具有阻挡层的多层塑料物品的方法，所述阻挡层兼有对烃类的阻挡性能和对非极性聚烯烃的粘合促进性能，且它可与(来自其他挤出机的)其他挤出层通过共挤出工艺结合，不过它本身可通过挤出机挤出。
通过本发明方法生产的容器对烃类具有良好的阻挡性能，而且，还具有非常好的机械稳定性，所述机械稳定性还适用于(applies to)单独的挤出层之间的粘结强度。
因此，本发明提供生产多层塑料物品的方法，它包括基于非极性聚烯烃的至少两层挤出层和位于所述两层之间并与之直接接触的对烃类具有阻挡性能的挤出层，其中该方法包括在共挤出的吹塑体系内生产管状多层塑料型坯的步骤，和其中通过恰好一个挤出机，由共混物发生具有阻挡性能的层的挤出，所述共混物包括对烃类具有阻挡性能的聚合物和包括具有粘合促进性能的聚合物，并在挤出机中在共混物内部发生对烃类具有阻挡性能的聚合物和具有粘合促进性能的聚合物的至少一些分层(demixing)时的熔融温度下进行所述挤出。
在所使用的温度下因两种聚合物粘度差别引起的具有阻挡性能的共混物中两种聚合物的分层以下述方式发生，所述方式使得大多数具有阻挡性能的聚合物大致布置在挤出层的中间。
对于本发明来说，措辞“基于非极性聚烯烃的挤出层”是指以重量计，主要由聚烯烃组成的挤出层，其中这些聚烯烃分别可牵涉“原始”聚烯烃，其中聚烯烃的比例占主要量的粉碎材料(“再粉碎材料”)，或这些的混合物。在这一意义上的措辞“非极性”是指不带有任何极性基团，例如酸基，酸酐基，酰胺基，酯基或羟基的聚烯烃。
对于本发明的目的来说，措辞“直接接触”是指对烃类具有阻挡性能的层在其上侧和其下侧分别粘结到基于非极性烯烃的层上。
对于本发明的目的来说，措辞“挤出层”是指在共挤出工艺中，可通过恰好一个挤出机挤出的任何层，而与在每一个尺寸上它是否具有均一的结构无关。相反，对于本发明的目的来说，在所述层内不同的形貌或不均匀度不是挤出层，即使它们本身具有层状的结构。
由于通过本发明实现在共混物内两种聚合物之间的分层，因此具有阻挡性能的聚合物在具有阻挡性能的挤出层内部存在以颗粒和相互交叠的层状结构形式的非均匀的分布。这一方法使用仅仅一个挤出机和仅仅一种共混物生产出实现了阻挡效果的可称为涂布/多层结构的制品，在所述结构内，可称为三层壁的结构对应于具有六层壁结构的已知塑料容器所提供的结构。
对于本发明的目的来说，措辞“多层交叠的层状结构”是指主要平行于挤出层所在平面的结构，所述结构空间有限且优选借助相互接触形成最大连续性的内聚材料层。
在本发明的方法中，在具有阻挡性能的层的挤出过程中的熔融温度范围优选为160℃-260℃，优选范围为180℃-240℃，优选范围为200℃-225℃，尤其优选的范围为205℃-215℃，和尤其范围为208℃-212℃。然而，若温度高于260℃，则在具有阻挡性能的挤出层内两种聚合物混合物和所得层具有明显较差的阻挡性能。
为了在本发明的方法中挤出具有阻挡性能的层，优选使用不具有剪切部分和/或混合部分的螺杆挤出机，和尤其优选使用不具有剪切部分且不具有混合部分的螺杆挤出机。
在本发明的方法中，基于聚烯烃的至少两层挤出层中的聚烯烃优选彼此独立地分别选自由下述组成的组：非极性高密度聚乙烯(HDPE)，低密度聚乙烯(LDPE)，线性低密度聚乙烯(LLDPE)，聚丙烯(PP)，乙烯-丙烯共聚物和这些的混合物，和此处可使用或者“原始”材料，或者粉碎材料(“再粉碎材料”)，或者要么这些的混合物。优选这两层分别基于非极性高密度聚乙烯(HDPE)。
作为对烃类具有阻挡性能的聚合物，优选使用在210℃的温度下和在2160g的负载下，溶体流动速度为2-10g/10min,优选3-5g/10min的聚合物(根据ISO1133测定)。聚合物的密度优选为约1.0-1.3g/cm3(根据ISO1183测定)。所使用的阻挡聚合物的熔点范围优选为160℃-200℃，优选范围为180℃-190℃(根据ISO11357测定)。
作为对烃类具有阻挡性能的聚合物，本发明方法中所使用的聚合物优选是选自由下述组成的组中的聚合物：乙烯-乙烯醇共聚物(EVOH)，聚芳基酰胺，聚酰胺(PA)，聚乙烯醇(PVOH)，聚对苯二甲酸乙二酯(PET)，和它们的混合物。对烃类具有阻挡性能的聚合物尤其优选是乙烯-乙烯醇共聚物(EVOH)，和尤其优选基于共聚物的分子组成，乙烯比例为28-36mol%的乙烯-乙烯醇共聚物。在一个尤其优选的实施方案中，具有阻挡性能的层不包括与乙烯-乙烯醇共聚物一起的聚酰胺。
具有粘合促进性能的聚合物优选选自用极性基团官能化的聚烯烃，优选用不饱和羧酸或用羧酸酐官能化的聚乙烯。这类聚合物的实例是乙烯与不饱和羧酸或羧酸酐，例如丙烯酸，甲基丙烯酸，马来酸或马来酸酐的共聚物。尤其优选乙烯与马来酸酐的共聚物，其中共聚物优选包括基于聚合物的总重量，0.05-5wt%马来酸酐，更优选0.1-1wt%，和尤其优选0.2-0.3wt%马来酸酐。
在共混物内具有阻挡性能的聚合物的重量份与具有粘合促进性能的聚合物的重量份之比的范围优选为15:85-40:60，尤其优选范围为20:80-35:75，和尤其范围为25:75-30:70，在每一情况下基于该共混物的总重量。
具有阻挡性能的挤出层的厚度优选是所述层和两层聚烯烃层的层厚之和的2-10%,优选3-8%，和尤其优选5.5-7.5%。
通过本发明方法生产的多层塑料物品可与基于聚烯烃的两层和具有阻挡性能的层一起包括进一步的挤出层，所述挤出层彼此独立地通过共挤出施加到聚烯烃-基层的一层或两层上，并与对烃类具有阻挡性能的挤出层直接接触。作为例举，在燃料容器情况下，(从内侧起，即从面向燃料的一侧起)可优选下述层结构：HPDE，对于本发明的目的来说，具有阻挡性能的挤出层，包括HDPE作为主要成分，着黑色的HPDE的由再粉碎材料制成的粉碎材料。
同样可能的是，塑料物品中的一层或更多层挤出层，尤其基于聚烯烃的挤出层包括添加剂，例如纤维，填料，颜料，抗氧剂等，但不限于这些。然而，优选具有阻挡性能的挤出层不包括填料，例如称为粘土的材料。
优选的是，用于运输或用于储存液体和/或气态烃类，尤其燃料，例如汽油或柴油的多层中空塑料体，或者用于所述中空塑料体的零配件构成在本发明的方法中生产的塑料制品，例如填料颈(fillerneck)，泵，填料管，填充-变平指示器(fill-level indicators)，和通风装置，例如阀门，或固定设备，但不限于这些。多层塑料物品尤其优选包括燃料容器。
本发明进一步提供多层塑料物品，它包括基于非极性聚烯烃的至少两层，和位于所述两层之间且与之直接接触的对烃类具有阻挡性能的层，其中具有阻挡性能的层包括对烃类具有阻挡性能的聚合物且包括具有粘合促进性能的聚合物，和其中具有阻挡性能的聚合物在具有阻挡性能的层内部存在以颗粒和相互交叠的层结构形式的非均匀的分布。
本发明具有阻挡性能的层形成阻挡材料集中在中间的所谓的三层结构，和这是挤出工艺和在挤出工艺过程中共混物的特定分层的结果。使用仅仅三个挤出机，这一方法得到所谓的五层壁结构。
本发明的这些多层塑料物品优选通过以上所述的本发明方法生产，以便基于非极性聚烯烃的两层，和在其间且与之直接接触的具有阻挡性能的层分别牵涉挤出层。
进一步的步骤，或者加工在本发明方法中生产的型坯得到实际的塑料物品的可能性分别是本领域技术人员已知的。
可为了这一目的，按照已知方式，以具有轴向或径向原料的头形式设计在本发明方法中所使用的挤出头，其中从挤出机中出来的熔体物流在心轴周围轴向或径向流动。也可通过合适地设计的流动通道，使熔体物流在挤出头内偏离。在此处另一可能的布局中，可提供分离装置，侧面切割或细分多层管状型坯，通过多个伸长的、笔直的线形模头间隙，以片材-或网状物形状的型坯形式出现。
作为例举，因此可按照已知方式，通过挤出吹塑，由所述管状型坯获得燃料容器。作为替代方案，也可切割开型坯，得到至少两个片材状的半成品产品，然后热成形，得到半-壳(half-shells)，然后焊接，得到中空体，但本发明没有限制到这些以上提及的可能性上。
本发明也可包括挤出半成品产品，所述半成品产品为片材或网状物形式，且拟用于热成形。

Claims (13)

1.生产多层塑料物品的方法，它包括基于非极性聚烯烃的至少两层挤出层和位于所述两层之间并与之直接接触的对烃类具有阻挡性能的挤出层，其中该方法包括在共挤出的吹塑体系内生产管状多层塑料型坯的步骤，其特征在于只用一个挤出机，由共混物进行具有阻挡性能的层的挤出，所述共混物包括对烃类具有阻挡性能的聚合物且包括具有粘合促进性能的聚合物，并在挤出机中在共混物内部进行对烃类具有阻挡性能的聚合物和具有粘合促进性能的聚合物的至少一些分层时的熔融温度下进行所述挤出。
2.权利要求1的方法，其特征在于具有阻挡性能的聚合物在具有阻挡性能的挤出层内部存在，以颗粒和相互交叠的层状结构的形式非均匀地分布。
3.权利要求1或2的方法，其特征在于熔体温度范围为160℃-260℃，优选范围为200℃-225℃，优选范围为205℃-215℃，尤其优选范围为208℃-212℃。
4.权利要求1-3任何一项的方法，其特征在于为了挤出具有阻挡性能的层，使用不具有剪切部分和/或混合部分的螺杆挤出机，优选不具有剪切部分且不具有混合部分的螺杆挤出机。
5.权利要求1-4任何一项的方法，其特征在于基于聚烯烃的至少两层挤出层中的聚烯烃彼此独立地分别选自由下述组成的组：非极性高密度聚乙烯(HPDE)，低密度聚乙烯(LDPE)，线性低密度聚乙烯(LLDPE)，聚丙烯(PP)，乙烯-丙烯共聚物和这些的混合物，优选这两层分别是非极性高密度聚乙烯(HDPE)。
6.权利要求1-5任何一项的方法，其特征在于对烃类具有阻挡性能的聚合物是选自由下述组成的组中的聚合物：乙烯-乙烯醇共聚物(EVOH)，聚芳基酰胺，聚酰胺(PA)，聚乙烯醇(PVOH)，和它们的混合物，优选是乙烯-乙烯醇共聚物(EVOH)，尤其优选基于共聚物的分子组成，乙烯比例为28-36mol%的乙烯-乙烯醇共聚物。
7.权利要求1-6任何一项的方法，其特征在于具有粘合促进性能的聚合物选自用极性基团官能化的聚烯烃，优选乙烯与不饱和羧酸或羧酸酐的共聚物，尤其优选乙烯与马来酸酐的共聚物。
8.权利要求1-7任何一项的方法，其特征在于在共混物内具有阻挡性能的聚合物的重量份与具有粘合促进性能的聚合物的重量份之比的范围优选为15:85-40:60，优选20:80-35:75，尤其优选25:75-30:70，在每一情况下基于该共混物的总重量。
9.权利要求1-8任何一项的方法，其特征在于具有阻挡性能的挤出层的厚度是所述层和两层聚烯烃层的层厚之和的2-10%,优选3-8%，尤其优选5.5-7.5%。
10.权利要求1-9任何一项的方法，其特征在于多层塑料物品包括进一步的挤出层，所述进一步的挤出层彼此独立地通过共挤出施加到聚烯烃基层的一层或两层上，并与对烃类具有阻挡性能的挤出层直接接触。
11.权利要求1-10任何一项的方法，其特征在于用于运输或用于储存液体和/或气态烃类的多层中空塑料体，或者用于所述中空塑料体的零配件，优选燃料容器。
12.多层塑料物品，它包括基于非极性聚烯烃的至少两层，和位于所述两层之间且与之直接接触的对烃类具有阻挡性能的层，其中具有阻挡性能的层包括对烃类具有阻挡性能的聚合物且包括具有粘合促进性能的聚合物，其特征在于，具有阻挡性能的聚合物在具有阻挡性能的层内部存在，以颗粒和相互交叠的层状结构的形式非均匀地分布。
13.权利要求12的多层塑料物品，其特征在于基于非极性聚烯烃的两层和位于其间且与之直接接触的具有阻挡性能的层分别包括通过权利要求1-12任何一项或多项的方法生产的挤出层。
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