CN105934470A - 聚交酯的用途以及纸或板的经热封接的容器或包装物的制造方法 - Google Patents

聚交酯的用途以及纸或板的经热封接的容器或包装物的制造方法 Download PDF

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Publication number
CN105934470A
CN105934470A CN201580005774.6A CN201580005774A CN105934470A CN 105934470 A CN105934470 A CN 105934470A CN 201580005774 A CN201580005774 A CN 201580005774A CN 105934470 A CN105934470 A CN 105934470A
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polyactide
purposes
paper
covering
pla
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CN201580005774.6A
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CN105934470B (zh
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J.拉萨宁
O.凯尔利艾宁
K.内瓦莱宁
V.里布
A.罗斯林
M.卡耶海安
E.林德斯特姆
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Stora Enso Oyj
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Stora Enso Oyj
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • C08J7/12—Chemical modification
    • C08J7/16—Chemical modification with polymerisable compounds
    • C08J7/18—Chemical modification with polymerisable compounds using wave energy or particle radiation
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Abstract

本发明涉及聚交酯(PLA)作为在用于生产容器和包装物的纸或板上的经挤出的聚合物覆盖物的用途，所述容器和包装物在烘炉或微波炉中加热。根据本发明，使多官能性交联剂例如三烷基异氰脲酸酯(TAIC)与PLA共混，并且，使所述经挤出的覆盖物层经受交联电子束(EB)辐射。PLA可原样使用或者与另外的可生物降解的聚酯例如聚丁二酸丁二醇酯(PBS)共混。已经发现，EB辐射改善了覆盖物与纸或板基材的粘附、覆盖物的热封接性能、以及最终容器和包装物的耐热性。

Description

聚交酯的用途以及纸或板的经热封接的容器或包装物的制造方法
技术领域
本发明涉及聚交酯(聚丙交酯，polylactide)用于纤维质基材例如纸或板上的经挤出的覆盖物的用途，所述纤维质基材可通过热封接变成容器和包装物。本发明的特别的目标是实现覆盖有聚交酯的经热封接的包装物，所述包装物可在烘炉或微波炉中加热。成型为盘的容器可甚至用于在炉中烘烤食品。本发明还涵盖了这样的经热封接的容器和包装物的制造方法。
背景技术
由于聚交酯(PLA)的可生物降解性，其成为包装技术中广泛使用的聚合物。PLA可用作纤维质基材例如纸或板上的经挤出的覆盖物，使所述纤维质基材变成可生物降解的容器和包装物。PLA具有相对良好的水蒸汽和气体阻挡性质，但具有可加工性及耐热性弱、与纤维质基材的粘附弱以及熔融温度高的问题，导致差的热封接性能。
为了改善PLA的热封接性能，US2002-0065345A1描述了PLA与由二醇和二羧酸制成的可生物降解的脂族聚酯(例如，聚己内酯(PLC)或聚(丁二酸丁二醇酯-己二酸丁二醇酯)(PBSA))的共混，所述可生物降解的脂族聚酯在混合物中的份额为至少9％。
根据US2005-0192410A1，通过向PLA中共混入聚己内酯和矿物颗粒来改善PLA的可加工性。US2007-0259195A1进一步描述了基于PLA的膜和聚合物覆盖物，它们被挤出到纤维质基材上并且其中使聚(己二酸丁二醇酯-对苯二甲酸丁二醇酯)(PBAT)与PLA共混以改善其耐热性。
WO2011/110750描述了基于PLA的双层覆盖物，其被挤出到纤维质基材上并且其中外层具有与内层相比更大份额的与其共混的(不同于PLA的)可生物降解的聚酯，目的在于使PLA和纤维质基材之间的粘附以及PLA的热封接性能最优化。
当通过与PLA共混的另一种聚酯或类似添加物来改善PLA的热封接性能时，存在这样的缺点——这些添加物比PLA更为昂贵。此外，聚合物的共混构成了复杂工艺中的额外的加工步骤。
WO2011/135182描述了不同的方法，其教导：对PLA层进行紫外(UV)辐射以改善其热封接性能。根据试验，热封接温度降低，但对于其发生的原因未给出任何解释。
由于聚对苯二甲酸乙二醇酯(PET)的高的耐热性和热稳定性，其成为通常用于能够烘烤的食品容器和包装物的聚合物。PET还具有良好的水及气体阻挡性质，这对于密封食品包装物来说是重要的。但是，缺点在于PET难以热封接。而且，常规的PET不是可生物降解的。
为了改善PLA的耐热性，已知的是使其经受产生交联且同时保持材料的生物降解能力的电子束(EB)辐射。作为实例，可列举公开CN101824211A、CN101735409A和CN101225221A。交联剂例如三烯丙基异氰脲酸酯(TAIC)或其衍生物可作为催化剂使用。但是，该相关现有技术的教导涉及模制物品或颗粒，不涉及位于纤维质基材上的其中要求热封接性能以及与该基材的粘附性的覆盖物。交联提高了分子量，这通常被认为是对热封接性能有害的。
WO98/04461教导了EB辐射在改善纸板基材上的聚烯烃(例如低密度聚乙烯(LDPE))的热封接中的用途。EB辐射诱发了聚合物的交联且因此提高了其分子量，降低了其熔融指数，并且引起了其熔体粘度的升高。据描述，EB改善了热封接的强度(其为这些现有技术教导的目标)。但是，对于可烘烤性来说，所述升高的熔体粘度和热稳定性可能仍然太低，而且，这样的覆盖有聚烯烃的纸板的烘炉或微波炉用途还未被提出。
发明内容
因此，仍然需要经改善的覆盖有PLA的纸或板，其满足同时存在的以下要求：可生物降解性；PLA与纸或板基材的粘附性；热封接性能，从而允许制造最终物品；以及足够的耐热性，从而容许在微波炉或烘炉中在最高达约240℃的温度下进行加热。
概括地说，本发明的解决方案是包含交联催化剂作为与PLA共混的组分，将该共混物作为覆盖物层挤出到纸或板上，并且对该覆盖物层进行EB辐照以使PLA交联。然后，可将该经覆盖且经EB照射的材料用于生产将要经受烘炉或微波炉加热的容器或包装物。
根据本发明，已经令人惊讶地发现：引导至覆盖物层(其包含交联催化剂以及单独的或者与其它聚酯共混的PLA)的EB辐射(β-射线)显著地改善了PLA与纸或板基材的粘附性，改善了PLA的热封接性能(尽管由于交联而在熔体粘度(剪切以及振荡)方面具有可测量的若干个数量级的升高)，而且，提高了PLA的耐热性和热稳定性，从而满足烘箱用途的要求。
本发明可通过如下来实践：(i)使PLA与交联催化剂共混，(ii)将所述共混物挤出到纤维质的纸或板基材的移动网幅上，以形成聚合物覆盖物层，(iii)使所述网幅在线地经受以所述覆盖物层作为目标的交联EB辐射，(iv)通过对所述覆盖物聚合物进行热封接，使所述经EB照射的经覆盖的材料变成容器或包装物，以及(v)将这样的容器或包装物在烘炉或微波炉中加热。本发明可应用于例如经封接的预制食品包装物(其在食品被消费之前被加热)。
已经发现，除了交联以外、或者代替交联，EB辐射能够破坏PLA中的聚合物链，据信，这有助于粘附性和热封接性能，但是，这无助于改善耐热性。但是，考虑到意欲的烘箱用途，交联是必须的。为了确保可烘烤性，将适宜的多官能性交联剂(例如TAIC或其衍生物、三羟甲基丙烷三丙烯酸酯(TMPTA)、或类似物)以1-5重量％、适宜地2-3重量％的量与PLA共混。出乎意料地，本发明人所进行的试验表明：PLA与纤维质基材的粘附以及PLA层的热封接性能均未因此受到削弱。
前面所述的关于EB处理效果的发现是特别令人惊讶的，这是因为：根据普通的知识，交联以及提高的熔体粘度应当相当地损害粘附性和热封接性能。然而，在不限制本发明的情况下，可以推测：尽管存在交联剂，但是，在EB辐照期间出现了一些链断裂，产生了有利于热封接和粘附的建筑微观结构。于是，所得到的断裂的链端将增加粘附以及热封接性能，而在本体结构中同时发生的催化交联则致力于改善的耐热性。
借助于PLA与纤维质基材的改善的粘附性，PLA层的重量可降低，这带来了成本节约。
EB辐射对聚合物覆盖物层具有穿透和电离作用，尽管其被聚合物吸收并逐渐变弱。与UV辐射(其仅通过对聚合物层的表面进行加热而起作用、不穿透该层至任何更大的深度)相反，通过调节操作加速电压以具有EB辐射扩大到PLA层的整个深度的效果是可行的，同时，避免了基于纤维质的包装材料的下面的纸或板基材的燃烧或变色。适宜地，加速电压保持相对低，在50-300keV的范围内且优选为100keV或更低。
因此，为了通过EB辐照处理实现改善的粘附和改善的耐热性这两者，所述纸或板基材可仅具有单层覆盖物或者具有多层覆盖物，在所述多层覆盖物中，最上部的覆盖物层和最下部的覆盖物层这两者均包含PLA及交联催化剂。因此，同时实现了最上部层的改善的热封接性能以及最下部层的与基材的改善的粘附。
所述材料可为包装用的纸、纸板或卡纸，其中，通过挤出，在纤维质基材上产生单或多层的聚合物覆盖物，并且，使EB辐射以包含PLA和催化剂的最上部的覆盖物层作为目标。EB辐照的适宜的吸收剂量为20-200kGy、优选为50-100kGy。
当测试本发明时，EB处理已经成功地在环境空气中在室温下进行。然而，为了抑制降解并促进交联，可优选在惰性气氛(例如氮气)中、或者在真空中进行该处理。
当PLA构成基于纤维的包装材料(例如纸或板)的覆盖物聚合物时，可将其直接挤出到纤维质基体上，而无需中间的聚合物型粘合层。PLA可原样使用或者将其与其它可生物降解的聚酯(例如聚丁二酸丁二醇酯(PBS))共混。如果期望的话，PLA覆盖物中可包括纤维或无机填料颗粒。本发明允许PLA或其它聚酯向未经覆盖的纤维质基材的热封接，这与常见的聚合物-聚合物封接相比通常更具有挑战性。
所述能够烘烤的容器和包装物(其根据本发明由如前所述地制造并经EB照射的基于纤维的覆盖有PLA的包装材料热封接)包括用于可烘箱加热的食品的经热封接的卡纸的盒和纸箱包装物、纸板或卡纸的食品托盘、以及纸板杯(例如一次性饮用杯)。至少在其内侧上具有PLA覆盖物的板托盘可通过深拉形成，而且，将盖子热封接至所述板托盘的边上的凸缘(rim flange)，从而封闭所述包装物。所述饮用杯可在内侧上覆盖有PLA且在外侧上未经覆盖，由此，在本发明中，通过将内侧表面的覆盖物封接至外部表面的未经覆盖的纸板来形成杯的纵向接缝。替代地，在盒状包装物中，包装物的外部表面可为覆盖有PLA的且内部表面未经覆盖，由此，在封接中，将外部表面的覆盖物热封接至包装物的内部的未经覆盖的板表面。然而，在杯(例如饮用杯)中以及在盒状包装物中，板经常是在两侧上均覆盖有聚合物的，由此，根据本发明，可对一侧或两侧上的覆盖物进行EB照射，而且，在热封接中，使覆盖物层彼此封接。此外，在该情况下，根据本发明的EB辐射改善了PLA的热封接性能。
此外，可使借助于本发明得到的杯或包装物经受热蒸汽的作用，通过EB辐照而交联的PLA提供了对于热蒸汽的耐受性。所述杯可用于例如咖啡自动售货机，而且，可在高压釜中对经热封接的包装物进行处理。如所要求保护的，本发明涵盖了这样的用途。
在关于本发明的试验中，已经观察到：电子束辐射改善了PLA或含PLA的共混物在以热空气进行的热封接中的封接性能。但是，预期，热封接夹具的使用也是可行的。
根据本发明，可通过如下将EB和UV处理组合起来：使聚交酯覆盖物首先根据WO2011/135182(其在此引入作为参考)的教导经受UV辐射、并然后如本文所述的那样经受EB辐射。相反的步骤顺序(即，EB辐照在UV之前)也是可行的。
当实践本发明时，甚至可行的是：将覆盖有PLA的纸或板首先变成例如容器或包装物的物品，并然后，使所述覆盖物层经受交联电子束(EB)辐射。在该情况中，EB辐照增强了覆盖物的热稳定性并因此改善了最终制品包装物的可消毒性和可烘烤性。
实施例
在下面，借助于所进行的试验和应用实施例，更详细地描述了本发明。
本发明的优选实施方式的实例是在由牛皮纸、CTMP或机械纸浆制成的其重量为40-500g/m2的纸或板上挤出聚合物覆盖物，所述聚合物覆盖物基本上由PLA组成、或者由40-95重量％的PLA和5-60重量％的PBS的共混物组成，且包括1-5重量％的TAIC，并具有5-20g/m2的重量。所述纸或卡纸的其它侧面可保持为未经覆盖的。将覆盖有聚合物的网幅(web)以5-600米/分钟、优选200-600米/分钟的速度输送通过EB辐射体，其中，所述覆盖有聚合物的网幅的经覆盖的侧面朝向所述EB辐射体。将经EB照射的网幅切割成坯料，将所述坯料热封接到容器(例如纸板托盘)或包装物(例如包装用的盒或箱)中。所述封接可使用热空气来实施，由此，空气温度可为约420-470℃。对于经过更强烈照射(即，在较慢网幅速度下)的材料，完全封接所需的空气温度低于接受较少辐射的材料所需的空气温度。代替热空气，可使用封接夹具，所述封接夹具的温度可为约145-160℃；此外，在该情况下，对于辐射最多的材料，所述封接夹具的温度最低。
代替移动的网幅，还可将EB辐射引导至相对于辐射体固定不动的网幅或坯料的封接路线，因此，所述路线接受了较大份额的辐射，同时，聚合物表面的其它部分未暴露于辐射。作为实例，可列举由覆盖有PLA的烘焙卡纸组成的盘坯。
为了确定EB辐射对于经挤出的覆盖物层与纤维质基材的粘附的影响，使用在纸板网幅的一侧上的经挤出的35g/m2的单层PLA(所述PLA共混有2重量％的TAIC)来实施试验系列。使所述经挤出的覆盖物层经受不同的EB辐射剂量。通过所述覆盖物的剥离的容易性，将与板网幅表面的粘附按照以下等级进行划分：
0＝无粘附
1＝轻微粘贴至网幅
2＝粘贴至网幅
3＝牢固地粘贴至网幅
4＝牢固地粘贴至网幅、撕裂了一些纤维
5＝牢固地粘贴至网幅、撕裂了许多纤维
EB辐射剂量为0(参比)、25kGy、50kGy、100kGy和200kGy，且按照前述等级的粘附水平分别为3、4、5、5和5。换句话说，50kGy的剂量产生了粘附从充分至优异的改善，因为PLA覆盖物层不再沿着板与覆盖物之间的分界线从纤维质表面剥离掉，但是，所尝试的剥离导致板内的构造体的撕裂。这是对于完美粘附的标准要求。
作为比较，针对在未加入TAIC的情况下的在纸板上的35g/m2的PLA，实施类似的粘附试验。采用0、25、50、100和200kGy的EB辐射剂量的粘附水平分别为2、3、3、5和5。换句话说，需要100kGy的剂量以实现完美粘附。
然后，使用相同的经EB照射的在纸板上的35g/m2的单层PLA(所述PLA共混有2重量％的TAIC)的样品以用于确定EB对热封接性能的影响。对于每个样品，测量热封接的引发温度，其为在碰到覆盖层表面之前的在电加热空气喷嘴处的热封接空气的温度。在所示的温度下，聚合物已经充分地熔融以用于与纤维质板的未经覆盖的相反侧的完美封接。如在粘附的情况中的那样，要求是：对于封接的尝试打开导致板构造体内的撕裂。
图1是示出了针对不同剂量的EB辐射(以kGy为单位测量)的热封接温度(℃)的图。看到：随着辐射剂量从0(参比＝无处理)提高至最高达200kGy，EB处理通过将热封接温度从最初的500℃逐渐地降低至430℃而显著地改善了热封接性能。
作为比较，图2包括来自于与图1的试验系列相对应、但针对在未加入TAIC的情况下的在纸板上的35g/m2的PLA的试验系列的结果。在该情况下，逐渐提高的EB辐射剂量使热封接温度从最初的500℃降至420℃。
图3示出了这样的曲线图，其绘出了来自于经挤出的聚合物膜的所测得的剪切粘度-剪切速率，所述经挤出的聚合物膜已经在240℃下再次熔融以用于测量。曲线图1代表作为参比的未经EB辐射处理的仅PLA的膜，曲线图2和3代表共混有3重量％的TAIC的PLA的膜，其在再次熔融前已经分别以100kGy和200kGy的EB辐射剂量进行EB处理，而且，曲线图4代表共混有5重量％的TAIC的PLA的膜，其在再次熔融前已经以200kGy的EB辐射剂量进行EB处理。据估计，热封接中的条件对应于约5-50s-1的剪切速率。看到：在该范围内，EB辐照以及PLA中的TAIC的使用已经使熔体的剪切粘度相比于参比明显地降低，这指示了改善的热封接性能(即，热封接所需的热空气温度较低)。
另一个重要发现是：在低的剪切速率下，TAIC和EB辐照的使用已经显著地提高了熔体的剪切粘度，这表明，在静态条件下，经EB处理的PLA共混物相比于未经处理的PLA具有优良的热稳定性和耐热性。所述提高的粘度(即，受限的大分子长程运动)能够解释成源于聚合物链之间的交联，向经覆盖的纸或板以及由其制成的制品提供了改善的可烘烤性。因此，尽管检测到了改善的热封接性能，但保持了借助于交联EB(如由现有技术已知的那些)而提高的耐热性。
图4示出了这样的曲线图，其绘出了针对与图3中相同的熔融材料1-4的所测得的振荡粘度-角频率。所述结果与来自剪切粘度的那些非常一致，证明：通过在EB辐照中使用TAIC作为用于PLA的交联剂，实现了改善的热封接性能和热稳定性。
通常发现：在采用EB辐照处理和未采用EB辐照处理这两种情况下，PBS均具有比PLA更高的熔体粘度。可推断：PBS和PLA的共混物仍产生比单独的PLA更好的耐热性，但是，热封接性能可被削弱。找到对于这样的共混物的最佳组成以满足对于可烘烤制品的特定要求不超出技术人员的技能。

Claims (15)

1.聚交酯(PLA)的用途，用于纤维质基材例如纸或板上的经挤出的聚合物覆盖物，包括：使多官能性交联剂与聚交酯共混，并且，使经挤出的覆盖物层经受交联电子束(EB)辐射。
2.根据权利要求1的聚交酯的用途，特征在于，通过热封接，使覆盖有聚合物的纸或板变成容器或包装物，所述容器或包装物在烘炉或微波炉中加热。
3.根据权利要求1或2的聚交酯的用途，特征在于，所述覆盖物是单层覆盖物。
4.根据前述权利要求中任一项的聚交酯的用途，特征在于，所述多官能性交联剂是三烯丙基异氰脲酸酯(TAIC)。
5.根据前述权利要求中任一项的聚交酯的用途，特征在于，在具有聚交酯的共混物中，所述多官能性交联剂的份额为1-5重量％、优选2-3重量％。
6.根据前述权利要求中任一项的聚交酯的用途，特征在于，对与交联催化剂共混的聚交酯进行EB照射以改善与纸或板基材的粘附。
7.根据前述权利要求中任一项的聚交酯的用途，特征在于，EB辐射的剂量为20-200kGy、优选50-100kGy。
8.根据前述权利要求中任一项的聚交酯的用途，特征在于，EB辐照在惰性气氛例如氮气中、或者在真空中进行。
9.根据前述权利要求中任一项的聚交酯的用途，特征在于，在经挤出的覆盖物中，将另外的可生物降解的聚合物例如聚丁二酸丁二醇酯(PBS)用作与聚交酯的共混物。
10.根据前述权利要求中任一项的聚交酯的用途，特征在于，在所述覆盖物中包括纤维或无机填料颗粒。
11.根据前述权利要求中任一项的聚交酯的用途，特征在于，使经覆盖的板变成一次性饮用杯或食品托盘。
12.根据权利要求1-10中任一项的聚交酯的用途，特征在于，使经覆盖的板变成封闭的纸箱包装物。
13.根据权利要求1-10中任一项的聚交酯的用途，特征在于，使经覆盖的板变成用经热封接的盖子封闭的容器。
14.由覆盖有聚交酯的纸或板制造容器或包装物的方法，特征在于
(i)使聚交酯与多官能性交联剂共混，
(ii)将共混物作为覆盖物层挤出到所述纸或板上，
(iii)使所述覆盖物层经受交联电子束(EB)辐射，和
(iv)通过所述覆盖物层的热封接，使经覆盖的纸或板变成容器或包装物。
15.由覆盖有聚交酯的纸或板制造容器或包装物的方法，特征在于
(i)使聚交酯与多官能性交联剂共混，
(ii)将共混物作为覆盖物层挤出到所述纸或板上，
(iii)使经覆盖的纸或板变成容器或包装物，和
(iv)使所述覆盖物层经受交联电子束(EB)辐射。
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