CN1636710A - 在不进行固态处理情况下改进rpet的耐环境应力开裂性的方法 - Google Patents

在不进行固态处理情况下改进rpet的耐环境应力开裂性的方法 Download PDF

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CN1636710A
CN1636710A CNA2004101046136A CN200410104613A CN1636710A CN 1636710 A CN1636710 A CN 1636710A CN A2004101046136 A CNA2004101046136 A CN A2004101046136A CN 200410104613 A CN200410104613 A CN 200410104613A CN 1636710 A CN1636710 A CN 1636710A
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layer
pen
ndc
rpet
mixture
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CN100484756C (zh
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塞德·法哈
斯里雷姆·R·塔马普雷姆
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Pepsico Inc
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Abstract

未固态处理RPET和按重量计算小于大约10％数量的PEN和/或NDC的混合物被用作具有一个热塑性材料内层的物品，如容器或用于吹模容器的预型件的至少一层。少量PEN和/或NDC的添加允许直接使用RPET而不进行固态处理，并且提供了具有可与纯PET相比的耐环境应力开裂性、颜色和器官感觉特性的物品。

Description

在不进行固态处理情况下改进 RPET的耐环境应力开裂性的方法
技术领域
本发明涉及直接由消费后、再循环和/或再粉碎的聚对苯二甲酸乙二醇酯制成的物品，以及制作这种物品的方法。具体地说，本发明涉及包含消费后、再循环和/或再粉碎的聚对苯二甲酸乙二醇酯和按混合物重量计算小于大约10％数量的聚萘二甲酸乙二醇酯和/或萘二羧酸酯的混合物的物品，其中再循环和/或再粉碎的聚对苯二甲酸乙二醇酯没有在任何实质上真空状态或惰性气体中进行固态处理。
技术背景
聚对苯二甲酸乙二醇酯(“PET”)广泛用于容器，如饮料瓶中。结果，至少部分由于普遍的再循环法规，所以有大量的再粉碎PET和再循环或消费后PET(共称为“RPET”)存在。RPET可以是原始材料经济的替代品。RPET主要从材料回收设施中处理的塑料饮料瓶中获得。但是，RPET可能包含杂质并且具有相对较低的特性粘度(“IV”)。结果，由RPET制成的容器通常具有很差的耐环境应力开裂性(“ESCR”)、感官感觉和颜色。树脂的IV也容易因为由不同制造者生产的混合材料而不同，这在再循环中是必然会发生的。例如，未处理、低IV的RPET被用于衣服绝热的填充纤维，并用作地毯纤维。但是，低IV妨碍了其在需要更高和/或更均匀IV的产品中的应用。
一般而言PET，具体地说RPET的IV、感官感觉和颜色可以通过实施聚合物树脂的固态聚合，即通过固态处理PET或RPET来改进，这增加了分子量并从树脂中去除不想要的杂质。例如，属于普什等人的美国专利No.4392804公开了或者在真空下或者在惰性气体如氮气环境中加热PET以增加低级PET或RPET的IV。PET在一种注射模制装置的隔离部分内加热到大约172°至仅仅230°的温度，以提供PET的固态聚合，由此提供增加的IV。
属于鲁宾逊的美国专利No.6284808和6376563公开了一种用于在线进行固态聚合PET切片的方法，其中RPET和PET材料被切成切片和大块的非均匀混合物。大块然后在一种去除大部分大块的除粒器或分类器中被除去，包括大部分来自再循环瓶的无定形的，即非晶态的颈部。据报道无定形的颈部在处理中是不想要的，因为非晶态材料的快速结晶化释放出大量干扰处理的热量。在所公开的方法中仅仅结晶的PET和RPET切片经受固态聚合。
属于凡艾登等人的美国专利No.5886058公开了RPET和PET的固态聚合对切片比对球粒发生得更快。结果，就不需要现有技术的PET制粒步骤。
属于米尔斯等人的美国专利No.5266413公开了固态处理降低PET的乙醛含量，并且降低PET形成乙醛的趋势。不用固态处理，据报道就需要大量的聚酰胺将乙醛水平降低到可接受的水平，这消极影响了混合物的透明度。据报道具有耐冲击性、耐应力裂纹性和耐热性的共聚酯/聚酰胺的混合物通过将非晶态的PET与0.06至2.0重量百分比的非羟官能的聚酰胺混合而获得。
属于布鲁斯特等人的美国专利No.5888598公开了由0.1至95重量百分比的PET与5至99.9重量百分比的聚萘二甲酸乙二醇酯(“PEN”)共聚物的混合物制成的预型件和容器，这里PEN包含90至95摩尔百分比的萘二羧酸酯(“NDC”)和5至10摩尔百分比的二酸，如对苯二酸酯。所公开的混合物的使用为容器提供了阻隔特性，而不需要另外的阻隔层。但是，仅仅单层预型件和容器得到公开，这排除了RPET的使用。
属于施密特等人的美国专利No.5902539、6194536、6395865和6586558公开了一种用于制作PEN/PET混合物的方法，其中IV的变化率和酯交换反应的水平在固态处理中得到控制。该方法在惰性气体流或低至2托的真空下进行。在所公开的方法中，具有第一IV的PEN和具有第二IV的PET或RPET在获得需要的最终IV的足够数量的烷撑二醇化合物，如乙二醇化合物的存在下进行反应。混合物包含大约50至大约90重量百分比的PET和大约50至大约10重量百分比的PEN。
属于哈钦森的美国专利No.6109006、6312641和6391408以及属于哈钦森等人的美国专利No.63525426中公开了使用overmolding方法，如inject-over-inject(“IOI”)方法制作涂层PET预型件的方法。在所公开的IOI方法中，注射模制被用于在一个现存的预型件上注射一层或多层材料。术语“overinjecting”和“overmolding”被用于描述一种涂层方法，其中通常在下面的预型件还没有完全固化时将一层材料注射到一个现存的预型件上面。所公开的overinjecting被用于在一个涂层或非涂层的预型件上设置一个或多个另外的材料层，如阻隔材料、再循环PET或其他热塑性材料。但是，没有公开在非固态处理状态下使用PEN或NDC改进RPET的ESCR和其他特性。
使用RPET的现有方法需要材料的固态处理，这增加了由RPET制作的任何产品的成本。因此，就需要一种方法和由未固态处理RPET制成的物品，允许在预型件、容器和其他物品中使用RPET，而不需要固态处理。本发明提供了这种方法和物品。
发明内容
本发明涉及一种物品，它包括至少一个至少一种热塑性材料的内层和至少一个额外层，基于RPET和PEN和/或NDC的混合物的重量，所述额外层包括未固态处理RPET和按重量计算小于大约10％数量的PEN和/或二羧酸萘(“NDC”)。该物品最好为一种容器或用于吹模容器的预型件，更优选的是，内层中的热塑性材料为未使用PET。该物品还可以包括至少一个位于热塑性内层和第二层之间或者位于第二层外面的气体阻隔层。根据本发明的一种特别有用的容器或用于吹模容器的预型件包括一个包含未使用PET的模制内层、一个位于内层的至少一部分周围的第二模制层以及，作为选择，至少一个气体阻隔层，其中第二层包含未固态处理RPET和按重量计算小于大约10％数量的PEN和/或NDC，而气体阻隔层最好为环氧类或苯氧基类材料，并且最优选的为聚羟基氨基醚(“PHAE”)。
本发明的方法包括获得物品，如预型件或容器的内热塑性层，获得包含未固态处理RPET和PEN和/或NDC的混合物，其中PEN和/或NDC按重量计算以小于大约10％的数量存在，形成至少一个包含混合物的层，并在内层的至少一部分周围定位混合物以形成物品的至少一部分。
附图说明
图1显示了根据本发明的一种预型件；
图2显示了图1中预型件的横截面；
图3显示了本发明的一种多层预型件的横截面；
图4显示了一种inject-over-inject模制装置；和
图5显示了一种多层注射模制装置。
具体实施方式
用在这里的术语“固态处理(solid stating)”是指在真空或惰性气体环境下加热聚合物以在固体状态下实现聚合的方法，如在属于普什等人的美国专利No.4329804中公开的方法，其内容在需要说明固态处理的范围内在此被引作参考。
用在这里的术语“未固态处理RPET”和“未固态处理RPET/PEN和/或NDC混合物”是指一种RPET和RPET/PEN和/或NDC混合物，它们还没有在惰性气体环境或者任何大体真空下固态处理RPET足够的时间，以至明显增加RPET或RPET/PEN和/或NDC混合物的平均分子量和特性粘度(“IV”)。本领域的技术人员将认识到，在RPET模制过程中发生的正常干燥过程中可能发生少量固态处理。但是，由于在正常干燥处理中没有产生平均分子量和IV的明显增加，所以在本说明书中，具有这种少量固态处理的RPET被认为是未固态处理的RPET。
本发明涉及包含RPET的物品，所述物品在不固态处理RPET或包括RPET的混合物而克服了现有技术在ESCR(EnvironmentalStretch Crack Resistance)、器官感觉和颜色方面的缺陷。上面已经提到，RPET切片通常包含杂质并且具有很低的IV。因此，由于很差的ESCR、器官感觉和颜色，在容器，如瓶子和分配袋以及用于制作这种容器的预型件中使用未处理RPET是不可接受的。在现有技术中这种问题通常通过固态处理RPET以去除挥发物并增加RPET的分子量和IV而克服。但是固态处理显著增加了容器成本的数量。与现有技术相比，本发明允许直接使用未固态处理RPET以提供具有可接受的ESCR、器官感觉和颜色的物品，具体地说，是容器和预型件。也就是说，本发明提供一种热塑性物品，它包含RPET和PEN和/或NDC的未固态处理混合物，并具有可与未使用材料(virgin material)相比的、可接受的ESCR、器官感觉和颜色。另外，在本发明物品中PEN和/或NDC的存在也增加了物品对紫外辐射(“UV”)的抵抗力。
用于本发明中的、RPET和PEN和/或NDC的未固态处理混合物包含按重量计算小于大约10％数量的PEN和/或NDC。但是，已经发现，在未固态处理的RPET/PEN和/或NDC混合物中低水平的PEN和/或NDC提供了用于食品和饮料的容器，特别是由采用IOI技术制作的预型件制成的容器中所需的ESCR的必要水平。基于未固态处理RPET/PEN和/或NDC混合物的重量，未固态处理的RPET/PEN和/或NDC混合物最好包含按重量计算超过90％的未固态处理RPET和按重量计算小于大约10％的PEN和/或NDC，更优选的是，按重量计算大约90％至大约99.5％的未固态处理RPET和按重量计算大约10％至大约0.5％的PEN和/或NDC，最优选的是，按重量计算大约95％至大约99％的未固态处理RPET和按重量计算大约5％至大约1％的PEN和/或NDC。
本发明的未固态处理RPET/PEN和/或NDC混合物可以采用本领域公知的、用于制作共混聚合物的任何方法制成，包括但是不限于共挤出，并且可以用于形成具有可与原始PET相比的ESCR和颜色的物品。这种物品包括但是不限于容器，如用于分配流体和流体类粉末的瓶子和袋子，例如，衬袋盒，以及用于制作这种容器的预型件。
对于用于食品和饮料的容器以及用于制作这种容器的预型件，最好通过首先形成一层未使用PET或其他可接受的FDA批准材料，然后在第一层上形成一层本发明的未固态处理RPET/PEN和/或NDC混合物而克服器官感觉问题。包括未固态处理RPET/PEN和/或NDC混合物、未使用PET和活性或惰性气体隔层中一些的额外层也可以采用任何本领域公知的方法施加。各层最好使用IOI技术通过注射模制形成。
本发明中气体阻隔层所需的对气体，如氧气和二氧化碳具有需要的低渗透性的热塑性树脂包括但是不限于两种树脂，对苯二甲酸、间苯二甲酸和至少一种二醇的共聚酯，如属于贾巴林的美国专利No.4578295中公开的，以及苯氧基类热塑性塑料，例如，羟官能的聚酰胺-醚，如美国专利No.5089588和5143998中描述的，聚羟基酰胺醚，如美国专利No.5134218中描述的，聚醚，如美国专利No.5115075和5218075中描述的，羟官能的聚醚，如美国专利No.5164472中描述的，羟官能的聚醚磺酰胺，如美国专利No.5149768中描述的，聚羟基酯醚，如美国专利No.5171820中描述的，羟基-苯氧基醚聚合物，如美国专利No.5814373中描述的，和聚羟基氨基醚(“PHAE”)，如美国专利No.5275853中描述的。上述共聚酯阻隔材料可以称为“共聚酯阻隔材料”。上述其他化合物共同归类并在这里称为术语“苯氧基类热塑性”材料。本段中参考的所有专利其内容在需要说明共聚酯阻隔材料和苯氧基类热塑性材料的范围内在此被引作参考。
多层结构最好使用本领域公知的共注射技术或者属于哈钦森的美国专利No.6391408中公开的inject-over-inject(“IOI”)技术形成，其内容在需要说明IOI技术和有用材料的范围内在此被引作参考。inject-over-inject是一种在现有的注射模制物品上使用注射模制技术注射一层或多层热塑性材料的过程。例如，使用IOI形成根据本发明的预型件，预型件的内层和颈部瓶口首先通过注射模制一种FDA批准的材料，如未使用PET，在模具内形成。然后将内层和颈部瓶口从模具中移走，并且在仍然位于模芯的同时，被转移到第二模具中，在这里未固态处理RPET和PEN和/或NDC被注射到第一层上。然后可以使用IOI或其他可用技术施加一个气体阻隔材料的外层。inject-over-inject也可以称为“overinjecting”和“overmolding”。最好当内层还没有完全固化时外层或各层被overmolding，以帮助各层之间的结合。本领域的技术人员将容易理解，用于形成模制到预型件上的各层的材料最好具有与用于形成预型件的材料相似的玻璃态转化温度，以便层叠的预型件不会在吹模过程中裂开、模糊或离层。
各种inject-over-inject使用分层注射模制(“LIM”)，其中熔流包括不同材料的多个薄层。如哈钦森‘408专利中所公开的，LIM可以在inject-over-inject中用作LIM-over-inject或inject-over-LIM。当需要时，也可以使用LIM-over-LIM以同时提供RPET和PEN和/或NDC层以及气体阻隔或其他层。
上面已经提到，本发明的未固态处理RPET/PEN和/或NDC混合物特别适用于瓶子、分配袋和其他容器，以及用于形成这种容器的预型件。使用本发明的未固态处理RPET/PEN和/或NDC混合物制作的预型件和容器可以使用本领域公知的、可以提供热塑性预型件或容器的可用模制方法模制。但是，预型件最好用注射模制。一种用于本发明中的预型件10示于图1中，其横截面示于图2中。该预型件10包括一个瓶口或颈部12、一个主体或容器部分14和一个支撑环16，瓶口12和主体14最好无缝结合。如图所示，瓶口12包括螺纹18，在容器部分14吹模之后，该螺纹可以通过一个封闭件用于密封产生的容器。但是，瓶口12的结构并不限于螺纹18，而是可以使用任何允许采用封闭件密封的可用结构。
用于本发明的一种多层预型件20的横截面示于图3中。对于图1和2中所示的预型件10，多层预型件20包括一个无缝连接的瓶口12和容器部分14以及一个支撑环16。容器部分14包括一个内层22以及至少一个外层24，所述内层无缝连接到瓶口12，最好与瓶口12模制成整体件。最好外层24由本发明的未固态处理RPET/PEN和/或NDC混合物形成，并且内层22由未使用PET形成。
外层24可以使用本领域的任何可用方法形成。预型件最好使用inject-over-inject方法模制，如图4中所示。使用inject-over-inject方法处理，预型件40在第一模具(未示出)中注射模制在型芯42上，这里型芯42和第一模具都最好是冷的。预型件40和型芯42然后转移到第二冷却模具44中。然后至少一层热塑性树脂注射模制到形成于外表面46和第二模具44之间的间隙48内、预型件40的外表面46上。冷却之后，获得如图3所示类型的多层预型件。
这种多层预型件也可以使用一种用于LIM-over-inject、inject-over-LIM或LIM-over-LIM模制的分层注射模制系统模制。一种分层注射模制装置49示于图5中。尽管装置49适合于LIM-over-inject、inject-over-LIM模制和LIM-over-LIM模制，可以使用单个LIM模制步骤制成一个完整的预型件。装置49包括一个进料漏斗50和另一个进料漏斗54，前者设计为将第一种热塑性树脂，最好为PET，供应到第一注射缸52，后者设计为将第二种热塑性树脂，如阻隔材料，供应到第二注射缸55。输出物53和56分别以需要的相对数量结合到层生成器57中，并用于形成预型件的至少一部分(未示出)。
因此，可以认为，本发明已经参考目前设计的特别的最佳实施例得到说明。但是本发明并不限于这里公开的实施例，并且可以认为，本领域的技术人员将可以设计很多修改例和其它实施例。因此，所希望的是，所附权利要求书覆盖属于本发明的精神和范围内的所有这些修改例和实施例。

Claims (24)

1.一种多层物品，包括：
一个包含热塑性材料的内层；和
一个包含未固态处理RPET和PEN和/或NDC的第二层，其中PEN和/或NDC以小于第二层重量的大约10％的数量存在。
2.根据权利要求1所述的物品，其中物品为容器或用于吹模容器的预型件。
3.根据权利要求1所述的物品，其中内层中的热塑性材料为未使用PET。
4.根据权利要求1所述的物品，其中RPET按重量计算以超过90％的数量存在于至少一个额外层中。
5.根据权利要求1所述的物品，还包括至少一个位于热塑性内层和第二层之间或位于第二层外面的阻隔层。
6.根据权利要求5所述的物品，其中阻隔层粘接到内层的一个外表面上。
7.根据权利要求5所述的物品，其中阻隔层包含热塑性环氧类、苯氧基类和聚羟基氨基醚材料中的至少一种。
8.根据权利要求5所述的物品，其中热塑性环氧类为一种聚羟基氨基醚。
9.根据权利要求1所述的物品，其中PEN和/或NDC以第二层重量的大约0.001％至小于大约10％的数量存在于第二层中。
10.根据权利要求1所述的物品，其中PEN和/或NDC以第二层重量的大约1％至大约4.5％的数量存在。
11.根据权利要求1所述的物品，其中PEN和/或NDC以第二层重量的大约3％至大约4％的数量存在。
12.一种形成多层物品的方法，该方法包括：
获得物品的内层；
获得一种包含未固态处理RPET和PEN和/或NDC的混合物，其中PEN和/或NDC以小于混合物重量的大约10％的数量存在；
形成至少一个包含混合物的层；和
在内层的至少一部分周围定位混合物以形成物品的至少一部分。
13.根据权利要求12所述的方法，其中PEN和/或NDC以混合物重量的大约0.5％至大约10％的数量存在。
14.根据权利要求12所述的方法，其中PEN和/或NDC以混合物重量的大约1％至大约5％的数量存在。
15.根据权利要求12所述的方法，其中物品为容器或制作容器的预型件。
16.根据权利要求12所述的方法，其中内层包含未使用PET。
17.根据权利要求12所述的方法，其中内层通过模制一种热塑性材料获得。
18.根据权利要求12所述的方法，其中内层通过注射模制一种热塑性材料获得。
19.根据权利要求12所述的方法，其中形成包含混合物的层包括在内层周围注射模制所述混合物。
20.根据权利要求12所述的方法，还包括在内热塑性层和第二层之间或第二层外面形成至少一个包含气体阻隔材料的层。
21.根据权利要求20所述的方法，其中气体阻隔材料包含热塑性环氧类、苯氧基类和聚羟基氨基醚材料中的至少一种。
22.根据权利要求21所述的方法，其中气体阻隔材料为一种聚羟基氨基醚材料。
23.一种容器或用于吹模容器的预型件，包括：
一个包含未使用PET的模制内层；和
一个位于内层的至少一部分周围的第二个模制层，其中第二层包含未固态处理RPET和小于第二层重量的大约10％数量的PEN和/或NDC。
24.一种制作容器或预型件的方法，包括：
模制包含未使用PET的第一层；
形成包含未固态处理RPET和PEN和/或NDC的混合物，其中PEN和/或NDC按重量计算以小于大约10％的数量存在。
在内层的至少一部分周围模制至少一个包含所述混合物的层以形成容器或预型件的至少一部分。
CNB2004101046136A 2003-12-22 2004-12-22 在不进行固态处理情况下改进rpet的耐环境应力开裂性的方法 Expired - Fee Related CN100484756C (zh)

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RU2004137459A (ru) 2006-06-20
AR050055A1 (es) 2006-09-27
RU2380225C2 (ru) 2010-01-27
BRPI0405760A (pt) 2005-08-30
CA2489850C (en) 2008-10-21
HK1080037A1 (en) 2006-04-21
EP1547768A1 (en) 2005-06-29
CA2489850A1 (en) 2005-06-22
CN100484756C (zh) 2009-05-06
NO20045538L (no) 2005-06-23
US20050136201A1 (en) 2005-06-23
AU2004240164A1 (en) 2005-07-07
MXPA04012553A (es) 2005-10-19
JP2005231346A (ja) 2005-09-02
US20060006586A1 (en) 2006-01-12

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