CN115485328B - 树脂组合物 - Google Patents
树脂组合物 Download PDFInfo
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- CN115485328B CN115485328B CN202180031730.6A CN202180031730A CN115485328B CN 115485328 B CN115485328 B CN 115485328B CN 202180031730 A CN202180031730 A CN 202180031730A CN 115485328 B CN115485328 B CN 115485328B
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- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/001—Combinations of extrusion moulding with other shaping operations
- B29C48/0022—Combinations of extrusion moulding with other shaping operations combined with cutting
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Abstract
本发明的树脂组合物包含40~98质量份的改性淀粉(A)、2~60质量份的皂化度为75.0摩尔%以上的聚乙烯醇(B)、并任意地包含粘土(C),该(A)、(B)和(C)的总计含量为100质量份,测定20℃~150℃范围的动态粘弹性时的tanδ的峰值温度为128℃以下。
Description
技术领域
本发明涉及用于食品包装等的树脂组合物、包含该树脂组合物的含水组合物、包含该含水组合物的包覆物及其制造方法、包含该包覆物的多层结构体、包含该包覆物或多层结构体的粘接体、以及由该粘接体构成的包装材料。
背景技术
以往,包含改性淀粉和水溶性高分子的树脂组合物因生物降解性或阻气性优异,而广泛用于包装食品的容器(例如专利文献1)。然而,在使用这样的树脂组合物形成容器等的情况下,需要使用热熔粘接剂等粘接性材料,因此费钱,而且生物降解性下降。因此,对该树脂组合物要求热封性,使即使没有粘接性材料也可进行粘接。
现有技术文献
专利文献
专利文献1:日本特开2019-6900号公报。
发明内容
发明所要解决的课题
然而,根据本发明人的研究可知:像专利文献1这样的树脂组合物虽然阻气性较高,但热封性不充分。另外,还可知:如果要提高热封性,则有时阻气性反而降低,难以兼具热封性和阻气性。
因此,本发明的目的在于提供:热封性和阻气性优异的树脂组合物、包含该树脂组合物的含水组合物、包含该含水组合物的包覆物及其制造方法、包含该包覆物的多层结构体、包含该包覆物或多层结构体的粘接体、以及由该粘接体构成的包装材料。
用于解决课题的手段
本发明人为了解决上述课题进行了深入研究,结果发现:在包含40~98质量份的改性淀粉(A)、2~60质量份的皂化度为75.0摩尔%以上的聚乙烯醇(B)、并任意包含粘土(C)的树脂组合物中,如果将测定20℃~150℃范围的动态粘弹性时的tanδ的峰值温度调整至128℃以下,则可解决上述课题,从而完成了本发明。即,本发明包括以下的方案。
[1] 树脂组合物,其包含40~98质量份的改性淀粉(A)、2~60质量份的皂化度为75.0摩尔%以上的聚乙烯醇(B)、并任意地包含粘土(C),该(A)、(B)和(C)的总计含量为100质量份,测定20℃~150℃范围的动态粘弹性时的tanδ的峰值温度为128℃以下。
[2] [1]所述的树脂组合物,其中,相对于树脂组合物的质量,改性淀粉(A)、聚乙烯醇(B)和粘土(C)的总计含量为80质量%以上。
[3] [1]或[2]所述的树脂组合物,其中,改性淀粉(A)的平均直链淀粉含量为45质量%以上。
[4] [1]~[3]中任一项所述的树脂组合物,其中,聚乙烯醇(B)的皂化度为75.0~98.9摩尔%。
[5] [1]~[4]中任一项所述的树脂组合物,其中,粘土(C)的含量为0质量份以上且小于2质量份。
[6] [1]~[5]中任一项所述的树脂组合物,其中,改性淀粉(A)为选自醚化淀粉、酯化淀粉、阳离子化淀粉和交联淀粉的至少1种。
[7] [1]~[6]中任一项所述的树脂组合物,其中,改性淀粉(A)为选自具有碳原子数为2~6个的羟烷基的醚化淀粉和具有来自二羧酸酐的结构单元的酯化淀粉的至少1种。
[8] [1]~[7]中任一项所述的树脂组合物,其中,聚乙烯醇(B)依据JIS Z 8803测定的4%水溶液在20℃下的粘度为1~50mPa·s。
[9] 含水组合物,其是包含[1]~[8]中任一项所述的树脂组合物的含水组合物,且含水率为1~50质量%。
[10] 包覆物,其是将[9]所述的含水组合物包覆于纸或薄膜而形成的。
[11] 多层结构体,其包含[10]所述的包覆物和1个以上的层(X)。
[12] 粘接体,其是[10]所述的包覆物或[11]所述的多层结构体的含水组合物与粘附层进行热粘接而成的粘接体,其中,粘附层为选自包含在该包覆物、该多层结构体、其他包覆物或其他多层结构体中的上述含水组合物、上述纸、上述薄膜和上述层(X)的层、或除这些以外的粘附体中所含的层。
[13] [12]所述的粘接体,其中,上述粘附层为包含在包覆物、多层结构体、其他包覆物或其他多层结构体中的上述含水组合物。
[14] 包装材料,其由[12]或[13]所述的粘接体构成。
[15] [14]所述的包装材料,该包装材料为两边封袋、三边封袋、扁平袋、直立袋、角撑袋、双袋或吸嘴袋。
[16] [10]所述的包覆物的制造方法,该制造方法包括:使用挤出机将[9]所述的含水组合物包覆于由牵引机输送的薄膜或纸的工序。
发明效果
本发明的树脂组合物,其热封性和阻气性优异。
附图说明
[图1]是显示本发明的一个实施方案中的包覆物的层构成的示意截面图。
[图2]是显示本发明的一个实施方案中的粘接体及其制作方法的示意图。
[图3]是显示本发明的一个实施方案中的粘接体及其制作方法的示意图。
[图4]是实施例中使用的双螺杆挤出机的示意图。
[图5]是实施例5和比较例8的通过动态粘弹性测定得到的tanδ曲线。
具体实施方式
[树脂组合物]
本发明的树脂组合物包含40~98质量份的改性淀粉(A)、2~60质量份的皂化度为75.0摩尔%以上的聚乙烯醇(B)、并任意包含粘土(C),测定20℃~150℃范围的动态粘弹性时的tanδ的峰值温度为128℃以下。
本发明人意外地发现了:如果以特定的比例包含改性淀粉(A)和皂化度为75.0摩尔%以上的聚乙烯醇(B)、且上述tanδ的峰值温度为128℃以下,则可兼具优异的热封性和优异的阻气性。
<改性淀粉(A)>
从容易提高热封性、阻气性和生物降解性的观点来看,改性淀粉(A)例如优选为选自醚化淀粉、酯化淀粉、阳离子化淀粉和交联淀粉的至少1种。
作为淀粉,可列举:来自木薯、玉米、马铃薯、甘薯、西米、木薯粉、高粱、豆、蕨菜、莲(荷花)、丘角菱、小麦、大米、燕麦、竹芋、豌豆等的淀粉。其中,优选来自玉米、木薯的淀粉,进一步优选来自高直链淀粉的玉米的淀粉。淀粉可单独使用或组合两种以上进行使用。
作为醚化淀粉,可列举:例如甲基醚化淀粉等烷基醚化淀粉;例如羧甲基醚化淀粉等羧烷基醚化淀粉;例如具有碳原子数为2~6个的羟烷基的醚化淀粉等羟烷基醚化淀粉等。另外,也可使用烯丙基醚化淀粉等。
作为酯化淀粉,可列举:例如具有来自乙酸的结构单元的酯化淀粉等具有来自羧酸的结构单元的酯化淀粉;例如具有来自马来酸酐的结构单元的酯化淀粉、具有来自邻苯二甲酸酐的结构单元的酯化淀粉、具有来自辛烯基琥珀酸酐的结构单元的酯化淀粉等具有来自二羧酸酐的结构单元的酯化淀粉;例如硝酸酯化淀粉、磷酸酯化淀粉、尿素磷酸酯化淀粉等具有来自含氧酸的结构单元的酯化淀粉。作为其他例子,可列举:黄原酸酯化淀粉、乙酰乙酸酯化淀粉等。
作为阳离子化淀粉,可列举:淀粉与2-二乙氨基乙基氯的反应物、淀粉与2,3-环氧基丙基三甲基氯化铵的反应物等。
作为交联淀粉,可列举:甲醛交联淀粉、环氧氯丙烷交联淀粉、磷酸交联淀粉、丙烯醛交联淀粉等。
作为改性淀粉(A),从容易提高热封性、阻气性和生物降解性的观点来看,优选为选自具有碳原子数为2~6个的羟烷基的醚化淀粉和具有来自二羧酸酐的结构单元的酯化淀粉的至少1种,更优选为选自羟乙基醚化淀粉、羟丙基醚化淀粉、羟丁基醚化淀粉、具有来自马来酸酐的结构单元的酯化淀粉、具有来自邻苯二甲酸酐的结构单元的酯化淀粉和具有来自辛烯基琥珀酸酐的结构单元的酯化淀粉的至少1种。改性淀粉(A)可单独使用或组合两种以上进行使用。需要说明的是,在本说明书中,“淀粉”的前面记载的碳原子数表示取代淀粉中的1个羟基的基团(将淀粉中的1个羟基改性而形成的基团)的碳原子数。例如,具有碳原子数为2~5的羟烷基的醚化淀粉表示将该淀粉中的1个羟基改性而形成的羟烷基的碳原子数为2~5。
具有碳原子数为2~6个的羟烷基的醚化淀粉例如可以是通过环氧乙烷、环氧丙烷、环氧丁烷等环氧烷烃与淀粉的反应得到的产物。在淀粉中的每1个葡萄糖单元中,用于改性的羟基的平均数优选为0.05~2。
关于改性淀粉(A),改性淀粉(A)中的平均直链淀粉含量优选为45质量%以上、更优选为50质量%以上、进一步优选为55质量%以上、更进一步优选为60质量%以上。若平均直链淀粉含量为上述的下限以上,则容易提高热封性、阻气性和生物降解性。改性淀粉(A)中的平均直链淀粉的含量通常为90质量%以下。在本说明书中,直链淀粉含量例如可通过“Starch 50 No.4 158-163 (1998)”中记载的碘显色法来测定。需要说明的是,平均直链淀粉含量在改性淀粉为1种的情况下表示该1种改性淀粉的直链淀粉含量,在使用2种以上的改性淀粉的情况下表示将2种以上的改性淀粉的直链淀粉含量进行加权平均而得的值。因此,例如在使用2种以上的改性淀粉、且将平均直链淀粉含量设为45质量%以上的情况下,可包含直链淀粉含量小于45质量%的改性淀粉。
关于改性淀粉(A),改性淀粉(A)中的含水率优选可以是5~15质量%。
改性淀粉(A)也可使用市售品。作为改性淀粉(A)的代表性的市售品的例子,例如可列举:Ingrediоn公司制造的作为羟丙基醚化淀粉的ECOFILM (商标)或National1658(商标)等。
相对于成分(A)、(B)和(C)的总计100质量份,改性淀粉(A)的含量为40~98质量份。若改性淀粉(A)的含量少于40质量份或超过98质量份,则热封性、阻气性和生物降解性有下降的倾向。
改性淀粉(A)的含量优选为50质量份以上、更优选为60质量份以上、更进一步优选为65质量份以上,且优选为95质量份以下。若改性淀粉(A)的含量为上述的下限以上,则容易提高热封性和生物降解性,而且若改性淀粉(A)的含量为上述的上限以下,则容易提高阻气性和热封性。
<聚乙烯醇(B)>
聚乙烯醇(B)是具有来自乙烯醇的构成单元(有时称为乙烯醇单元)的聚合物。聚乙烯醇(B)的皂化度为75.0摩尔%以上。若聚乙烯醇(B)的皂化度小于75.0摩尔%,则阻气性有下降的倾向。本发明的树脂组合物因聚乙烯醇(B)的皂化度为75.0摩尔%以上,故可提高阻气性。聚乙烯醇(B)的皂化度优选为78摩尔%以上、更优选为85摩尔%以上、进一步优选为90摩尔%以上,且优选为98.9摩尔%以下、更优选为98摩尔%以下、更进一步优选为97摩尔%以下。若聚乙烯醇(B)的皂化度为上述的下限以上,则容易提高阻气性,而且若聚乙烯醇(B)的皂化度为上述的上限以下,则容易提高热封性。需要说明的是,皂化度表示聚乙烯醇中的羟基相对于羟基与酯基的总计的摩尔分数。皂化度可依据JIS K 6726 (聚乙烯醇试验方法)来测定,例如可利用实施例中记载的方法进行测定。
聚乙烯醇例如可通过乙酸乙烯酯单体的聚合得到的聚乙酸乙烯酯的水解来制造。
聚乙烯醇(B)依据JIS Z 8803测定的4%水溶液在20℃下的粘度优选为1mPa·s以上、更优选为3mPa·s以上、进一步优选为5mPa·s以上,且优选为50mPa·s以下、更优选为45mPa·s以下、进一步优选为35mPa·s以下。若聚乙烯醇(B)的粘度为上述范围,则容易提高热封性、阻气性和生物降解性。需要说明的是,上述粘度可通过实施例中记载的方法进行测定。
聚乙烯醇(B)可进一步包含除乙烯醇单元以外的其他单体单元。作为其他单体单元,可列举:来自烯键式不饱和单体的单体单元等。作为烯键式不饱和单体,可示例:乙烯、丙烯、正丁烯、异丁烯、1-己烯等α-烯烃类;丙烯酸及其盐;具有丙烯酸酯基的不饱和单体;甲基丙烯酸及其盐;具有甲基丙烯酸酯基的不饱和单体;丙烯酰胺、N-甲基丙烯酰胺、N-乙基丙烯酰胺、N,N-二甲基丙烯酰胺、二丙酮丙烯酰胺、丙烯酰胺丙磺酸及其盐、丙烯酰胺丙基二甲基胺及其盐(例如季胺盐);甲基丙烯酰胺、N-甲基甲基丙烯酰胺、N-乙基甲基丙烯酰胺、甲基丙烯酰胺丙磺酸及其盐、甲基丙烯酰胺丙基二甲基胺及其盐(例如季胺盐);甲基乙烯基醚、乙基乙烯基醚、正丙基乙烯基醚、异丙基乙烯基醚、正丁基乙烯基醚、异丁基乙烯基醚、叔丁基乙烯基醚、十二烷基乙烯基醚、硬脂基乙烯基醚、2,3-二乙酰氧基-1-乙烯基氧基丙烷等乙烯基醚类;丙烯腈、甲基丙烯腈等氰化乙烯类;氯乙烯、氟乙烯等卤代乙烯类;偏二氯乙烯、偏二氟乙烯等偏卤代乙烯类;乙酸烯丙酯、2,3-二乙酰氧基-1-烯丙基氧基丙烷、烯丙基氯等烯丙基化合物;马来酸、衣康酸、富马酸等不饱和二羧酸及其盐或酯;乙烯基三甲氧基硅烷等乙烯基甲硅烷基化合物、乙酸异丙烯酯;甲酸乙烯酯、乙酸乙烯酯、丙酸乙烯酯、丁酸乙烯酯、异丁酸乙烯酯、新戊酸乙烯酯、新癸酸乙烯酯、己酸乙烯酯、辛酸乙烯酯、月桂酸乙烯酯、棕榈酸乙烯酯、硬脂酸乙烯酯、油酸乙烯酯、苯甲酸乙烯酯等乙烯基酯单体。相对于构成聚乙烯醇(B)的构成单元的总计摩尔量,其他单体单元的含量优选为10摩尔%以下、更优选为5摩尔%以下。
对聚乙烯醇的制造方法没有特别限定。例如可列举:将乙酸乙烯酯单体任意地与其他单体聚合,将所得到的聚合物皂化以转换成乙烯醇单元的方法。作为聚合时的聚合方式,可列举:间歇聚合、半间歇聚合、连续聚合、半连续聚合等。作为聚合方法,可列举:本体聚合法、溶液聚合法、悬浮聚合法、乳液聚合法等已知方法。聚合物的皂化可适用已知的方法。例如可在该聚合物溶解于醇或含水醇的状态下进行。此时可使用的醇例如为甲醇、乙醇等低级醇。聚乙烯醇(B)可单独使用或组合两种以上进行使用。
相对于成分(A)、(B)和(C)的总计100质量份,聚乙烯醇(B)的含量为2~60质量份。若聚乙烯醇(B)的含量小于2质量份或超过60质量份,则热封性、阻气性和生物降解性有下降的倾向。
聚乙烯醇(B)的含量优选为5质量份以上、更优选为50质量份以下、进一步优选为40质量份以下、特别优选为35质量份以下。若聚乙烯醇(B)的含量为上述的下限以上,则容易提高阻气性和热封性,而且若聚乙烯醇(B)的含量为上述的上限以下,则容易提高热封性和生物降解性。
<粘土(C)>
本发明的树脂组合物可任意地包含粘土(C)。需要说明的是,在本说明书中,“任意地包含”是指可包含也可不包含该成分。粘土(C)可以是天然粘土、合成粘土或有机化粘土。作为粘土,可列举:合成或天然层状硅酸盐粘土、例如蒙脱石、膨润土、贝得石、云母(mica)、锂蒙脱石、皂石、绿脱石、锌蒙脱石、蛭石、伊利石(ledikite)、麦羟硅钠石(magadite)、水羟硅钠石(kenyaite)、硅镁石(stevensite)、铬膨润石(volkonskoite)等。粘土(C)可单独使用或组合两种以上进行使用。
有机化粘土是利用有机化剂(或改质剂)对上述粘土进行有机化处理(或改质)而得的物质。对该有机化剂没有特别限定,例如可列举:具有烷基、苄基、吡啶基、牛脂(兽脂)或将牛脂氢化后的氢化牛脂的季铵盐;叔铵盐、仲铵盐等。作为烷基,例如可列举:甲基、乙基、丙基、丁基、戊基、己基、庚基、辛基、壬基、癸基等碳数为1~20的烷基等。
粘土(C)可使用市售品,对市售品没有特别限定,例如可列举:CLOISITE (注册商标) 20A (用二甲基二(氢化牛脂)季铵盐进行了有机化处理的蒙脱石、Southern ClayIndustries制造)等。
相对于成分(A)、(B)和(C)的总计100质量份,粘土(C)的含量优选小于2质量份、更优选为1.5质量份以下、进一步优选为1质量份以下、更进一步优选为0.5质量份以下、特别优选为0.2质量份以下,且优选为0质量份以上。若粘土(C)的含量为上述的上限以下,则容易将tanδ的峰值温度调整至128℃以下,容易体现优异的热封性。
<添加剂>
(聚氧化烯(D))
本发明的树脂组合物可任意地包含聚氧化烯(D)。聚氧化烯(D)表示聚环氧烷烃和聚亚烷基二醇,具有下述式(1)所表示的构成单元(也称为构成单元(1))。聚氧化烯(D)可具有2种以上的不同的构成单元(1)。
[化学式]
[式中,R为亚烷基,n为1以上]
式(1)中,作为亚烷基,例如可列举:亚乙基、亚丙基、三亚甲基、亚丁基、异亚丁基、亚戊基、亚己基、亚庚基、亚辛基、亚壬基、亚癸基等碳原子数为2~10个的亚烷基。这些之中,从热封性和阻气性的观点来看,优选碳原子数为2~6个的亚烷基、更优选亚乙基和/或亚丙基。在n为2以上的情况下,这些亚烷基可单独使用或组合两种以上进行使用。
从热封性和阻气性的观点来看,式(1)中的n优选为5以上、更优选为50以上、进一步优选为100以上,且优选为120,000以下、更优选为70,000以下。在聚氧化烯(D)包含不同的构成单元(1)的情况下,各构成单元的重复数n可相同也可不同。
作为聚环氧烷烃,例如可列举:具有来自碳原子数为2~6个的环氧烷烃的构成单元的聚合物,具体而言,可列举:聚环氧乙烷、聚环氧丙烷、聚氧杂环丁烷(polyoxethane)、聚环氧丁烷、聚异环氧丁烷、或构成它们的单体的共聚物等。作为聚亚烷基二醇,例如可列举:具有来自碳原子数为2~6个的亚烷基二醇的构成单元的聚合物,具体而言,可列举:聚乙二醇、聚丙二醇、聚三亚甲基二醇、聚丁二醇、聚异丁二醇、或构成它们的单体的共聚物等。这些之中,从热封性和阻气性的观点来看,聚氧化烯(D)优选为聚环氧乙烷、聚环氧丙烷、聚乙二醇、聚丙二醇或构成它们的单体的共聚物。作为该共聚物,优选环氧乙烷与环氧丙烷的共聚物、乙二醇与丙二醇的共聚物等。
聚氧化烯(D)可在不损及本发明效果的范围内包含除构成单元(1)以外的来自其他单体的构成单元。在聚氧化烯(D)为共聚物的情况下,对共聚物的聚合方式没有特别限定,可以是无规式、嵌段式、接枝式或递变式的任一种。聚氧化烯(D)可单独使用或组合两种以上进行使用。
从热封性和阻气性的观点来看,聚氧化烯(D)的重均分子量优选为10,000以上、更优选为50,000以上,且优选为5,000,000以下、更优选为3,000,000以下。
聚氧化烯(D)也可使用市售品。作为聚氧化烯(D)的代表性的市售品的例子,可列举:明成化学工业公司制造的ALKOX (商标) E-75G、ALKOX (商标) L-11、ALKOX (商标) L-6、ALKOX (商标) EP1010N、住友精化公司制造的PEO (商标) PEO-1、PEO-2等。
从热封性和阻气性的观点来看,相对于树脂组合物的质量,聚氧化烯(D)的含量优选为10质量份以下、更优选为5质量份以下,且优选为0质量份以上。
(多元醇增塑剂(E))
本发明的树脂组合物可任意地包含多元醇增塑剂(E)。对多元醇增塑剂(E)没有特别限定,例如可列举:山梨糖醇、麦芽糖醇、木糖醇、赤藓糖醇、蔗糖、甘露糖醇、乳糖醇、阿拉伯糖、木糖、果糖、葡萄糖、半乳糖、核糖、海藻糖、甘油、乙二醇、丙二醇等,这些多元醇增塑剂(E)可单独使用或组合两种以上进行使用。这些之中,从热封性和氧阻隔性的观点来看,多元醇增塑剂(E)优选包含选自山梨糖醇、麦芽糖醇、木糖醇、赤藓糖醇、蔗糖、甘露糖醇、乳糖醇、阿拉伯糖、木糖、果糖、葡萄糖、半乳糖、核糖、海藻糖和甘油的至少1种,更优选包含选自山梨糖醇、木糖醇和蔗糖的至少1种。需要说明的是,多元醇增塑剂(E)例如可使用市售品。对市售品没有特别限定,例如可列举:物产Food Science公司制造的Sorbitol SP等。
从热封性和阻气性的观点来看,相对于树脂组合物的质量,多元醇增塑剂(E)的含量优选为20质量份以下、更优选为10质量份以下、进一步优选为5质量份以下,且优选为0质量份以上。
(其他添加剂)
本发明的树脂组合物可包含碳原子数为12~22的脂肪酸和/或其脂肪酸盐。作为碳原子数为12~22的脂肪酸及其脂肪酸盐,例如可列举:硬脂酸、硬脂酸钙、硬脂酸钠、棕榈酸、月桂酸、肉豆蔻酸、亚油酸、二十二烷酸等。这些之中,从加工性的观点来看,优选硬脂酸、硬脂酸钙、硬脂酸钠。碳原子数为12~22的脂肪酸及其脂肪酸盐各自可单独使用或组合两种以上进行使用。
在本发明的树脂组合物含有碳原子数为12~22的脂肪酸和/或其脂肪酸盐的情况下,相对于树脂组合物的质量,其含量优选为0.01~3质量%、更优选为0.03~2质量%、进一步优选为0.1~1质量%。若碳原子数为12~22的脂肪酸和/或其脂肪酸盐的含量为上述范围,则在加工性方面存在有利的倾向。
本发明的树脂组合物可包含除多元醇增塑剂(E)以外的其他增塑剂(F)。作为增塑剂(F),例如可列举:水、三油酸甘油酯、环氧基化亚麻籽油、环氧基化大豆油、柠檬酸三丁酯、乙酰柠檬酸三乙酯、三乙酸甘油酯、2,2,4-三甲基-1,3-戊二醇二异丁酸酯。增塑剂(F)可单独使用或组合两种以上进行使用。这些增塑剂(F)中,从得到良好的成膜性和涂布性的观点来看,优选水。
从容易提高树脂组合物的成膜性和阻气性的观点来看,相对于树脂组合物的质量,树脂组合物中的含水率(含水量)优选为3~20质量%、更优选为4~18质量%、进一步优选为7~15质量%。需要说明的是,含水率例如可使用加热干燥式水分计、在130℃下测定60分钟来求出。
本发明的树脂组合物根据需要可进一步包含填充剂、加工稳定剂、耐候性稳定剂、着色剂、紫外线吸收剂、光稳定剂、抗氧化剂、抗静电剂、阻燃剂、其他的热塑性树脂、润滑剂、香料、消泡剂、消臭剂、增量剂、剥离剂、脱模剂、加固剂、交联剂、防霉剂、防腐剂、结晶化速度延迟剂等添加剂(G)。
在本发明的树脂组合物中,相对于树脂组合物的质量,改性淀粉(A)、聚乙烯醇(B)和粘土(C)的总计含量优选为60质量%以上、更优选为80质量%以上、进一步优选为85质量%以上、更进一步优选为90质量%以上,且优选为100质量%以下。若成分(A)、(B)和(C)的总计含量为上述范围,则容易提高热封性和阻气性。
<树脂组合物>
本发明的树脂组合物包含40~98质量份的上述改性淀粉(A)、2~60质量份的上述聚乙烯醇(B)、并任意地包含上述粘土(C),测定20℃~150℃范围的动态粘弹性时的tanδ的峰值温度为128℃以下,因此可兼具优异的热封性和优异的阻气性。而且,该树脂组合物的生物降解性也优异。因此,如果使用本发明的树脂组合物,则无需使用粘接性材料,即可简便地形成食品用包装材料等。而且,这种包装材料可具有优异的生物降解性和阻气性。需要说明的是,在本说明书中,热封性表示可通过热进行粘接的特性。
上述tanδ表示在动态粘弹性测定中得到的储能弹性模量(E’)与损耗弹性模量(E”)的比例即损耗角正切(E”/E’)。另外,tanδ的峰值温度表示在20℃~150℃的范围测定动态粘弹性时得到的曲线图(横轴为温度(℃)、纵轴为tanδ)中的tanδ的峰值时的温度。该动态粘弹性的测定可使用动态粘弹性测定装置,在20℃~150℃的范围边以3℃/分钟的速度升温边以11赫兹的正弦波拉伸树脂组合物(薄片)来实施。需要说明的是,在20℃~150℃范围的上述曲线图(有时称为tanδ曲线)中,在有2个以上的tanδ峰值的情况下,以存在于最高温侧的峰值时的温度作为tanδ的峰值温度。另外,为了防止因升温引起的树脂组合物中的水的挥发,测定前可在树脂组合物(薄片)的两面涂布凡士林等。这样的tanδ的峰值温度例如可通过实施例中记载的方法算出。
本发明的树脂组合物的tanδ的峰值温度为128℃以下。若tanδ的峰值温度超过128℃,则阻气性和热封性、特别是热封性有显著下降的倾向。
本发明的树脂组合物的tanδ的峰值温度优选为125℃以下、更优选为120℃以下、进一步优选为118℃以下,且优选为50℃以上、更优选为70℃以上、进一步优选为80℃以上。若tanδ的峰值温度为上述范围,则容易提高阻气性和热封性、特别是热封性。
本发明的树脂组合物的tanδ的峰值温度例如可通过适当变更改性淀粉(A)、聚乙烯醇(B)和粘土(C)的种类及其含量、聚乙烯醇(B)的皂化度、改性淀粉(A)中的直链淀粉含量等来调整。例如,改性淀粉(A)的含量、粘土(C)的含量和聚乙烯醇(B)的皂化度越小、或者聚乙烯醇(B)的含量越大,则tanδ的峰值温度越有下降的倾向。特别是,若粘土(C)的含量大,则tanδ的峰值温度有显著增加的倾向,因此在树脂组合物中粘土(C)的含量优选调整至1质量%以下。
本发明的树脂组合物,其阻气性、特别是氧阻隔性优异。本发明的树脂组合物在23℃、50%RH下的氧透过度(mL.20μm/[m2·atm·24小时])优选为8.0以下、更优选为5.0以下、进一步优选为4.0以下、更进一步优选为3.5以下、特别优选为3.0以下。若树脂组合物的氧透过度为上述的上限以下,则可体现优异的氧阻隔性。另外,该氧透过度(mL.20μm/[m2·atm·24小时])通常为0.01以上。树脂组合物的氧透过度可在23℃、50%RH下保管两周进行湿度调节后,使用氧透过量测定装置进行测定,例如可利用实施例中记载的方法进行测定。需要说明的是,在本说明书中,氧阻隔性上升或升高表示氧透过度降低,氧阻隔性优异表示氧透过度低。
本发明的树脂组合物即使在对包含改性淀粉(A)的树脂组合物不利的低湿环境下也可体现优异的热封性。因此,本发明的树脂组合物在低湿环境下的热封强度优异。本发明的树脂组合物在20℃、30%RH下的热封强度优选为1.0N/15mm以上、更优选为3.0N/15mm以上、进一步优选为4.0N/15mm以上、更进一步优选为5.0N/15mm以上、特别优选为5.5N/15mm以上。若热封强度为上述的下限以上,则容易体现优异的热封性。该热封强度的上限通常为30N/15mm以下。需要说明的是,在20℃、30%RH下的热封强度例如可通过实施例所记载的方法进行测定。
本发明的树脂组合物可以是颗粒和薄膜或薄片的形式。在将本发明的树脂组合物以薄膜或薄片的形式使用的情况下,薄膜的厚度通常为5μm~100μm,薄片的厚度通常为100μm~1000μm。另外,薄膜或薄片可以是单层体或多层体。需要说明的是,在本说明书中,术语“薄片”可用“薄膜”代替,术语“薄膜”可用“薄片”代替。
[树脂组合物的制造方法]
本发明的树脂组合物例如可通过包括如下工序的方法来制造:工序(1),至少混合上述改性淀粉(A)和上述聚乙烯醇(B)而得到混合物;工序(2),挤出该混合物;以及工序(3),使所挤出的混合物冷却和干燥。
工序(1)是至少混合上述改性淀粉(A)和上述聚乙烯醇(B)的工序,可任意地一同混合选自上述粘土(C)、聚氧化烯(D)、多元醇增塑剂(E)和其他添加剂(例如上述碳原子数为12~22的脂肪酸和/或其脂肪酸盐、上述增塑剂(F)、上述添加剂(G)等)的至少1种。
工序(1)通常使用挤出机来进行。在挤出机中,通过螺杆对各成分施加剪切应力,且通过对滚筒适用外部热,来边进行加热边均匀地混合。
作为挤出机,例如可使用双螺杆挤出机。双螺杆挤出机可以是共转或反转的任一种。螺杆直径例如可以是20~150mm、挤出机长度(L)与螺杆直径(D)之比L/D比例如可以是20~50。螺杆的转速优选为80rpm以上、更优选为100rpm以上。另外,挤出成型压力优选为5巴(0.5MPa)以上、更优选为10巴(1.0MPa)以上。各成分可分别直接导入到挤出机中。另外,也可将上述各成分用混合机预混后导入到挤出机中。
在工序(1)中,从容易提高树脂组合物的成膜性和氧阻隔性的观点来看,相对于混合物的质量,优选混合下限优选为0.1质量%以上、更优选为1质量%以上、进一步优选为10质量%以上、特别优选为15质量%以上、最优选为20质量%以上、且上限优选为50质量%以下、更优选为45质量%以下、进一步优选为40质量%以下的增塑剂(F)、优选水。这里,该混合物的质量表示包括增塑剂(F)在内的混合物的总质量。在工序(1)中,可在挤出的初期阶段导入增塑剂(F),也可在达到上述加热温度之前、例如100℃以下时导入增塑剂(F)。可通过水分、热和剪切应力的组合对改性淀粉(A)施行烹调处理(cooking treatment),使其明胶(凝胶)化。另外,可通过另外导入增塑剂(F)、优选水来溶解聚乙烯醇(B)等水溶性聚合物,将树脂组合物软化,降低模量和脆性。
在工序(1)中,加热至优选超过100℃且150℃以下、更优选115℃以上且140℃以下的温度以进行烹调处理。这里,烹调处理是指将淀粉颗粒粉碎、使其凝胶化的处理。加热可通过从外部对挤出机的滚筒适用热来进行。通过对各滚筒适用阶段性地变化的温度,可加热至目标温度。在超过120℃的温度下进行烹调处理的情况下,在加工性方面有利。
进行了烹调处理的混合物,为了防止起泡,优选边降至优选85~120℃、更优选90~110℃的温度边压入口模中。另外,通过从滚筒排气,可防止起泡、去除水分。
挤出机中的滞留时间可根据温度曲线或螺杆速度来设定,优选为1~2.5分钟。
在挤出混合物的工序(2)中,将边熔融混炼边挤入挤出机中的熔融的混合物从口模挤出。口模的温度优选为85~120℃、更优选为90~110℃的温度。
在将所挤出的混合物(熔融物)进行冷却和干燥的工序(3)中,混合物(熔融物)可挤出成膜状或片状、或线料状(strand shape)。
在将混合物挤出成膜状的情况下,混合物可从薄膜成型用口模挤出,然后边用牵引辊卷绕边进行冷却和干燥。在口模和辊之间,优选进行冷却以防止混合物附着于辊。可在口模和辊之间设置成型用辊。成型用辊的材质例如为橡胶制、树脂制、金属制。为了干燥,辊可进行加热,也可在卷绕时供给脱湿空气。在吹入管法的情况下,为了在薄膜退出口模时使薄膜膨胀而使用脱湿空气。也可将滑石夹带在空气流中以防止薄膜的粘连。
在将混合物挤出成线料状的情况下,从多个孔的线料喷嘴挤出,用旋转刀具切割,从而将线料制成颗粒状。为了防止颗粒的粘着,可定期或恒定地施加振动,利用热风、脱湿空气或红外线加热器去除颗粒中的水分。
[含水组合物]
本发明包含含水组合物,该含水组合物包含上述树脂组合物、且含水率为1~50质量%。在本发明的一个实施方案中,在使用树脂组合物形成后述的包覆物的情况下,为了提高树脂组合物的成膜性,例如在将树脂组合物涂布于纸或薄膜时,可在该树脂组合物中加入水以调制含水组合物。含水率可使用加热干燥式水分计在130℃下用60分钟测定已粉碎至最大粒径1mm以下的树脂组合物或含水组合物而求出。在本说明书中,含水组合物是指在包含水的树脂组合物中包括所有通过上述方法测定的含水率为1~50质量%的含水组合物。即,含水组合物的意思是除了包括在树脂组合物中加入水而将含水率调整至上述范围的组合物,还包括在制造时含水率为上述范围的树脂组合物。
本发明的含水组合物的含水率优选为5质量%以上、更优选为8质量%以上,且优选为45质量%以下、更优选为40质量%以下。若含水率为上述范围,则容易提高阻气性和包覆物形成时的牵引性。
在本发明的一个适当的实施方案中,本发明的含水组合物可通过在上述树脂组合物中添加水、例如进行搅拌混合而得到。为了防止树脂组合物之间的粘着、并使颗粒整体吸附水,优选边将水分2次以上添加边进行搅拌。另外,为了保持含水率恒定,含水组合物可在密闭容器内保管。
[包覆物及其制造方法]
本发明包含包覆物,该包覆物是将本发明的含水组合物包覆于纸或薄膜(或薄片)而形成的。即,包覆物成为具有由含水组合物构成的层和由纸或薄膜(或薄片)构成的层的层叠体。本发明的包覆物因阻气性和生物降解性优异、同时可体现热封性,因此例如即使不使用粘接性材料,也可通过热而简便且有效地制作包装材料等。
在将含水组合物包覆于纸的情况下,对该纸没有特别限定,例如可列举:牛皮纸、优质纸、模造纸、玻璃纸、羊皮纸、合成纸、白板纸、马尼拉纸板、牛奶盒用原纸、纸杯用原纸、象牙纸、银白纸、薄页纸、板纸、人造纤维纸等。对包覆物中的纸的厚度没有特别限定,优选为1~500μm、更优选为10~300μm。若包覆物中的纸的厚度为上述范围,则可提高包覆物制造时的牵引速度,产率容易提高。
在将含水组合物包覆于薄膜的情况下,对该薄膜没有特别限定,例如可列举:聚对苯二甲酸乙二醇酯(PET)膜、双轴拉伸聚丙烯(BOPP)膜、聚乙烯(PE)膜(优选低密度聚乙烯(LDPE)膜)和聚乳酸膜等。对包覆物中的薄膜的厚度没有特别限定,优选为1~500μm、更优选为10~300μm、进一步优选为50~100μm。
本发明的包覆物中的含水组合物的厚度优选为1~300μm、更优选为5~100μm、进一步优选为10~50μm。若包覆物中的含水组合物的厚度为上述范围,则容易得到良好的成膜性、热封性和阻气性。
本发明的包覆物,其阻气性、特别是氧阻隔性优异。该包覆物的氧透过度可选自与树脂组合物的上述氧透过度同样的范围。
对本发明的包覆物的制造方法没有特别限定,只要是可将含水组合物包覆于纸或薄膜的方法即可。在优选的实施方案中,本发明的包覆物可通过包括如下工序(记作工序(A))的方法来制造,工序(A)为使用挤出机将上述含水组合物包覆于由牵引机输送的薄膜或纸。
在本发明的一个实施方案中,在工序(A)中将含水组合物投入到挤出机中。作为挤出机,例如可列举:单螺杆挤出机、双螺杆挤出机等。挤出机的螺杆直径例如为20~150mm,挤出机长度(L)与螺杆直径(D)之比L/D比例如为15~50,螺杆的转速优选为80rpm以上、更优选为100rpm以上。挤出机中的气缸温度例如可以是80~120℃、优选为90~110℃。
投入到挤出机中的含水组合物被增塑化,从口模出口排出。另一方面,使用牵引机、优选辊式牵引机输送纸或薄膜。在所输送的该纸或薄膜上涂布从口模出口排出的含水组合物,从而得到包覆物。所得到的包覆物可在包含金属辊的多个辊之间与纸或薄膜压合的同时被输送,由卷绕机卷绕成辊状。作为多个辊,例如可列举:加压辊、浇铸辊、接触辊等。
在工序中,优选以下述式表示的拉伸比为5~20。若以这样的拉伸比制造包覆物,则产率提高,并且容易得到纸或薄膜与含水组合物的密合性和氧阻隔性优异的包覆物。需要说明的是,挤出机的口模出口的流速以(排出量)/((唇开度)×(口模宽度))表示。在以每单位时间的质量表现排出量的情况下,排出量优选为1~500kg/小时、更优选为5~200kg/小时,唇开度优选为0.01~5mm、更优选为0.1~1mm,口模宽优选为100~3000mm、更优选为200~2000mm。需要说明的是,在本发明中,在上述制造过程中含水组合物的水蒸发,因此所得到的包覆物中的含水组合物的含水率比制造前有所降低。
拉伸比=(牵引机的牵引速度)/(挤出机的口模出口的流速)
[多层结构体]
本发明包含多层结构体,该多层结构体包含上述包覆物和1个以上的层(X)。作为层(X),例如可列举:保护层、不同于上述含水组合物的阻气层、防湿层、遮光层、印刷层、加固层等。作为形成层(X)的材料,例如可列举:聚乙烯、聚丙烯、乙烯-乙酸乙烯酯共聚物、EVOH、聚氯乙烯、聚氨酯、聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯、聚萘二甲酸乙二醇酯等聚酯、尼龙等聚酰胺、聚丙烯腈、纤维素或其衍生物、玻璃、木材等。层(X)可设置1层或2层以上,也可以是单层或多层。在层(X)为2层以上的情况下,各层的厚度或材料可不同也可相同。需要说明的是,层(X)可经由粘接剂层(Y)层叠于含水组合物、纸或薄膜上。
对形成粘接剂层(Y)的粘接剂没有特别限定,例如可列举:丙烯酸系粘接剂、氨基甲酸乙酯系粘接剂、环氧系粘接剂、乙酸乙烯酯系粘接剂、乙烯-乙酸乙烯酯系粘接剂、氯乙烯系粘接剂、有机硅系粘接剂、腈纤维素系粘接剂、酚系粘接剂、聚乙烯醇系粘接剂、蜜胺系粘接剂、苯乙烯系粘接剂等。
本发明的多层结构体包含上述包覆物(将含水组合物包覆于纸或薄膜而得的包覆物)和1个以上的层(X),在本发明的适合的实施方案中,在最表面具有含水组合物(由含水组合物构成的层)。若是这样的方案,则可通过热来粘接最表面的含水组合物,因此可使用该多层结构体简便地形成食品用包装材料等。
在本发明的适合的实施方案中,在本发明的多层结构体中,优选至少1个层(X)相对于纸或薄膜配置在含水组合物的相反侧的最表面。在所述实施方案中,通过对层(X)的表面施加文字、图案等装饰等,可形成施加有标签或密封、文字或装饰的包装材料等。
对本发明的多层结构体的层构成没有特别限定,例如可列举:依次具有含水组合物/纸或薄膜/粘接层(Y)/层(X)的层构成;依次具有含水组合物/纸或薄膜/层(X)的层构成等。对层(X)的厚度没有特别限定,优选为1~1000μm、更优选为5~500μm。
[粘接体和包装材料]
本发明包含粘接体,该粘接体是上述包覆物或多层结构体的含水组合物与粘附层进行热粘接而形成的。作为该粘附层,可列举:选自包含在该包覆物、该多层结构体、其他包覆物或其他多层结构体中的上述含水组合物、上述纸、上述薄膜和上述层(X)的层、或包含在除这些以外的粘附体中的层。换言之,作为该粘附层,可列举:选自包含在该包覆物或该多层结构体中的含水组合物、纸、薄膜和层(X)的层;选自包含在其他包覆物而非该包覆物中的含水组合物、纸、薄膜和层(X)的层;选自包含在其他多层结构体而非该多层结构体中的含水组合物、纸、薄膜和层(X)的层;包含在不是该包覆物、该多层结构体、该其他包覆物和该其他多层结构体的粘附体中的层。
需要说明的是,在使用2个以上的本发明的包覆物的情况下,上述其他包覆物是指被粘接的一侧的该包覆物,在使用2个以上的本发明的多层结构体的情况下,上述其他多层结构体是指被粘接的一侧的该多层结构体。
上述粘附层优选为包含在包覆物、多层结构体、其他包覆物或其他多层结构体中的上述含水组合物。在上述粘附层为包含在包覆物或多层结构体中的上述含水组合物的情况下,可使用1张薄片制作粘接体。在上述粘附层为包含在其他包覆物或其他多层结构体中的上述含水组合物的情况下,可使用2张以上的薄片制作粘接体。
热粘接(热封)可使用传统的热封机来进行。本发明的粘接体是热封性优异的含水组合物进行热粘接而形成的,因此即使在低湿环境下也可具有充分的粘接强度。而且,阻气性和生物降解性也优异。
图2所示的粘接体(两边封袋)是由1个包覆物构成的两边封袋,是将包覆物2a折弯成2个(对折)并将两端部进行热粘接(热封)而成的。包覆物2a是具有图1所示的层构成的包覆物。
如图2所示,粘接体1a可通过将包覆物2a以含水组合物3a侧为内侧进行对折后,从纸或薄膜4a侧热压合两端的热压合部6a而得到。通过热压合粘接热压合部6a,可形成热粘接部,因此粘接体1a作为两边封袋起作用。
另外,粘接体(两边封袋) 1a具有开口部,例如在袋中装入内容物后,可通过将开口部附近进行热粘接而密封。
需要说明的是,在图2中显示粘附层5a为相同的包覆物中所含的上述含水组合物的方案,可适当变更热粘接的部位,以相同的包覆物中所含的纸或薄膜为粘附层制作粘接体;也可通过将包覆物2a变更为多层结构体、并且适当变更热压合部(热粘接部),以相同的多层结构体中所含的含水组合物、纸或薄膜、或层(X)为粘附层而制作粘接体。
图3所示的粘接体1b是由2个包覆物构成的三边封袋,是将2个包覆物2b和2c的3边附近部进行相互地热粘接而成的。包覆物2b和2c分别具有图1所示的层构成。
如图3所示,粘接体1b可通过将2个包覆物2b和2c分别以含水组合物3b和3c为内侧进行相互地重合后,从纸或薄膜4b和4c侧使位于所重合的层叠体的3边附近的热压合部6b热压合而得到。通过热压合使热压合部6b粘接,可形成热粘接部,因此粘接体1b作为三边封袋起作用。
另外,粘接体(三边封袋) 1b具有开口部,例如在袋中装入内容物后,可通过将开口部附近进行热粘接而密封。
需要说明的是,图3中显示粘附层5c为其他包覆物中所含的上述含水组合物的方案,可适当变更热粘接的部位,以其他包覆物中所含的纸或薄膜为粘附层而制作粘接体;也可至少将包覆物2c变更为多层结构体、并且适当变更热压合部(热粘接部),从而以其他多层结构体中所含的含水组合物、纸或薄膜、或层(X)为粘附层而制作粘接体。
也可使用除本发明的包覆物或多层结构体以外的粘附体来形成粘接体,例如在图3所示的方案中,可使用该粘附体代替一个包覆物。该粘附体可具有含水组合物,但也可以是不具有含水组合物的粘附体,例如可以是上述纸或薄膜等。
对形成本发明的粘接体的包覆物和多层结构体的总数没有特别限定,优选为1~3、更优选为1或2。另外,在本发明的适合的实施方案中,上述粘附层为包含在包覆物、多层结构体、其他包覆物或其他多层结构体中的上述含水组合物。这样的实施方案中的粘接体是上述包覆物或上述多层结构体的含水组合物与包含在上述包覆物、上述多层结构体、上述其他包覆物或上述其他多层结构体中的上述含水组合物进行热粘接(热封)而形成的,因此可具有更优异的粘接强度。需要说明的是,在图2所示的方案中,粘附层为相同的包覆物中所含的含水组合物,在图3所示的方案中,粘附层为其他包覆物中所含的含水组合物。另外,在图2和图3中,给出了袋作为一个例子,但粘接体的方案并不限于袋。
本发明包含由上述粘接体构成的包装材料。由于本发明的包装材料由上述粘接体构成,所以即使在低湿环境下也可具有充分的粘接强度,同时阻气性和生物降解性也优异。对本发明的包装材料的形状没有特别限定,优选两边封袋(参照图2)、三边封袋(参照图3)、扁平袋、直立袋、角撑袋、双袋或吸嘴袋。
本发明的一个实施方案中,在本发明的包装材料中,包覆物或多层结构体的含水组合物的总面积中与粘附层进行热粘接的面积优选为1~90%、更优选为5~40%。若该面积为上述范围,则可维持粘接强度,同时容易确保作为包装材料的容积。
实施例
以下,通过实施例对本发明进行详述,但本发明并不限于这些方案。
<试验方法>
(1) 氧透过度的测定
将实施例和比较例中得到的薄片在23℃、50%RH下保管两周进行湿度调节后,安装在氧透过量测定装置上,测定了氧透过度。测定条件如下。
装置:Modern Controls公司制造的“MOCON OX-TRAN2/20”;
温度:23℃;
氧供给侧和载气侧的湿度:50%RH;
氧气压力:1.0atm;
载气压力:1.0atm。
(2) 热封强度的测定
将实施例和比较例中得到的薄片在20℃、30%RH下保管两周进行湿度调节。将切割成15mm×300mm的短条状薄片沿长边方向折叠成2个(对折)。将距折痕30mm的长度(面积15mm×30mm)在刻度压力0.2MPa、温度100℃、2秒的条件下进行热封。通过使用拉伸试验机剥离密封部,测定热封强度。
热封机:安田精机制作所制造的“YSS热封机”,密封面积20mm×300mm;
拉伸试验机:Instron公司制造的“INSTRON3367”、测压元件(load cell)100N。
(3) 聚乙烯醇(B)的皂化度测定
依据JIS K 6726 (聚乙烯醇试验方法),进行实施例和比较例中的聚乙烯醇的溶解滴定,算出皂化度。
(4) 聚乙烯醇(B)的粘度测定
依据JIS Z 8803 (落球式粘度计)和JIS K 6726 (聚乙烯醇试验方法),调制实施例和比较例中的聚乙烯醇的4%水溶液,使用Hoppler粘度计测定20℃下的粘度,作为聚乙烯醇(B)的4%水溶液的粘度(20℃)。
(5) 动态粘弹性的测定
将实施例和比较例中得到的薄片在23℃、50%RH下保管两周进行湿度调节后,切割成5mm×30mm的小片。将样品设置于动态粘弹性测定装置(“RHEOGEL-E4000”、UBM公司制造)中后,在两面涂布凡士林,以防止因升温引起的水的挥发。在20℃~150℃的范围边以3℃/分钟的速度升温边以11赫兹的正弦波拉伸,测定了动态粘弹性。在所得到的tanδ曲线(横轴为温度(℃)、纵轴为tanδ)中,记录了tanδ的峰值温度。需要说明的是,在有2个以上的tanδ峰值的情况下,以存在于最高温侧的峰值作为tanδ的峰值温度。
(5) 所使用的材料
<改性淀粉(A)>
・(A-1):ECOFILM (注册商标);用环氧丙烷改性的玉米淀粉、直链淀粉含量为70质量%、从Ingredion公司获取;
・(A-2):National 1658 (注册商标):用环氧丙烷改性的玉米淀粉、直链淀粉含量为20质量%、从Ingredion公司获取。
<聚乙烯醇(B)>
・(B-1):Kuraray Poval (注册商标) 3-80;聚乙烯醇树脂、皂化度为79.8mol%、粘度为3mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-2):Kuraray Poval (注册商标) 5-88;聚乙烯醇树脂、皂化度为88.2mol%、粘度为5mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-3):Kuraray Poval (注册商标) 7-92;聚乙烯醇树脂、皂化度为91.5mol%、粘度为7mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-4):Kuraray Poval (注册商标) 17-94;聚乙烯醇树脂、皂化度为93.8mol%、粘度为17mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-5):Kuraray Poval (注册商标) 27-96;聚乙烯醇树脂、皂化度为96.0mol%、粘度为27mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-6):Kuraray Poval (注册商标) 5-98;聚乙烯醇树脂、皂化度为98.8mol%、粘度为5mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-7):ELVANOL (注册商标) 71-30;聚乙烯醇树脂、皂化度为99.5mol%、粘度为30mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-8):Kuraray Poval (注册商标) 25-100;聚乙烯醇树脂、皂化度为99.9mol%、粘度为25mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-9):Kuraray Poval (注册商标) L-8;聚乙烯醇树脂、皂化度为71.2mol%、粘度为5mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-10):Kuraray Poval (注册商标) 22-88;聚乙烯醇树脂、皂化度为88.0mol%、粘度为22mPa·s (20℃、4%水溶液)、从Kuraray公司获取;
・(B-11):Kuraray Poval (注册商标) 5-88;聚乙烯醇树脂、皂化度为88.0mol%、粘度为5mPa·s (20℃、4%水溶液)、从Kuraray公司获取。
<粘土(C)>
・(C-1):CLOISITE (注册商标) 20A;用二甲基二(氢化牛脂)氯化季铵盐进行了有机化处理(改质)的天然蒙脱石、从Southern Clay Industries公司获取。
<聚氧化烯(D)>
・(D-1):ALKOX (商标) L-11;聚环氧乙烷树脂、重均分子量为10万、从明成化学工业公司获取。
<多元醇增塑剂(E)>
・(E-1):山梨糖醇SP:山梨糖醇、从物产Food Science公司获取。
<实施例1>
将作为原料的90质量份改性淀粉(A-1)和10质量份聚乙烯醇(B-1)在转鼓混合机内混合2小时,将所得到的混合物供给至连接有液体泵的双螺杆挤出机。图4显示实施例1中使用的双螺杆挤出机的示意图,挤出机的螺杆直径、L/D比、转速、运转方式和温度曲线(表1)如下所示。
[表1]
温度曲线[℃]:
C1 | C2 | C3 | C4 | C5 | C6 | C7 | C8 | C9 | C10 | C11 | 适配器 | 口模 |
40 | 70 | 80 | 90 | 120 | 140 | 130 | 120 | 120 | 100 | 100 | 100 | 100 |
螺杆直径:27mm;
L/D比:48;
螺杆转速:500rpm;
运转方式:共转(啮合自擦拭)方式。
具体而言,将所得到的混合物经由双螺杆挤出机的重量送料器以3.5kg/小时的速度通过C1中的料斗供给至滚筒内。使水通过C4中的液体泵(图4的10),以26g/分钟的流速喷射到滚筒内。C5~C9的温度范围是烹调范围,在这些区域内完成了完全的明胶化。从口模挤出的树脂组合物在冷却、干燥后,以厚度达到120μm的牵引速度进行牵引,得到了厚度为120μm的薄膜。树脂组合物(薄膜)的含水率为11%。需要说明的是,使用加热干燥式水分计,在130℃下测定60分钟,求出含水率。测定含水率时,树脂组合物(薄膜)用Wonder BlenderWB-1 (大阪Chemical株式会社)粉碎至最大粒径1mm以下再进行测定。
<实施例2~14和比较例1~9>
除了如表2所记载地调整了改性淀粉(A)、聚乙烯醇(B)和其他物质的种类和添加量以外,利用与实施例1同样的方法,得到了树脂组合物(薄片)。需要说明的是,作为改性淀粉(A),在实施例10中使用了81质量份改性淀粉(A-1)和9质量份改性淀粉(A-2)的混合物,在实施例11中使用了54质量份改性淀粉(A-1)和36质量份改性淀粉(A-2)的混合物。除实施例10和11以外,与实施例1同样,使用了改性淀粉(A-1)作为改性淀粉(A)。
使用实施例1~14和比较例1~9中得到的树脂组合物(薄片),测定了动态粘弹性中的tanδ的峰值温度、氧透过度和热封强度。其结果见表2。
如表2所示,确认到了:实施例1~14中得到的树脂组合物(薄片)的氧透过度低、并且热封强度高。相对于此,确认到了:与实施例相比,比较例1~9中得到的树脂组合物(薄片)的氧透过度和热封强度的两者或任一者显著变差。
因此,可知本发明的树脂组合物的热封性和阻气性优异。
符号说明
1a、1b:粘接体;
2、2a、2b、2c:包覆物;
3、3a、3b、3c:含水组合物;
4、4a、4b、4c:纸或薄膜;
5a、5c:粘附层;
6a、6b:热压合部(热粘接部);
8:双螺杆挤出机;
9:料斗;
10:液体添加喷嘴;
11:树脂温度计
12:树脂压力计;
13:适配器;
14:口模。
Claims (13)
1.树脂组合物,其包含40~98质量份的改性淀粉(A)、2~60质量份的皂化度为75.0摩尔%以上的聚乙烯醇(B)、并任意地包含粘土(C),该(A)、(B)和(C)的总计含量为100质量份,测定20℃~150℃范围的动态粘弹性时的tanδ的峰值温度为128℃以下,
聚乙烯醇(B)依据JIS Z 8803测定的4%水溶液在20℃下的粘度为1~50mPa·s,
改性淀粉(A)的平均直链淀粉含量为45质量%以上,
改性淀粉(A)为选自醚化淀粉、酯化淀粉、阳离子化淀粉和交联淀粉的至少1种。
2.权利要求1所述的树脂组合物,其中,相对于树脂组合物的质量,改性淀粉(A)、聚乙烯醇(B)和粘土(C)的总计含量为80质量%以上。
3.权利要求1或2所述的树脂组合物,其中,聚乙烯醇(B)的皂化度为75.0~98.9摩尔%。
4.权利要求1或2所述的树脂组合物,其中,粘土(C)的含量为0质量份以上且小于2质量份。
5.权利要求1或2所述的树脂组合物,其中,改性淀粉(A)为选自具有碳原子数为2~6个的羟烷基的醚化淀粉和具有来自二羧酸酐的结构单元的酯化淀粉的至少1种。
6.含水组合物,其是包含权利要求1~5中任一项所述的树脂组合物的含水组合物,且含水率为1~50质量%。
7.包覆物,其是将权利要求6所述的含水组合物包覆于纸或薄膜而形成的。
8.多层结构体,其包含权利要求7所述的包覆物和1个以上的层(X)。
9.粘接体,其是权利要求7所述的包覆物或权利要求8所述的多层结构体的含水组合物与粘附层进行热粘接而成的粘接体,其中,粘附层为选自包含在该包覆物、该多层结构体、其他包覆物或其他多层结构体中的上述含水组合物、上述纸、上述薄膜和上述层(X)的层、或除这些以外的粘附体中所含的层。
10.权利要求9所述的粘接体,其中,上述粘附层为包含在包覆物、多层结构体、其他包覆物或其他多层结构体中的上述含水组合物。
11.包装材料,其由权利要求9或10所述的粘接体构成。
12.权利要求11所述的包装材料,该包装材料为两边封袋、三边封袋、扁平袋、直立袋、角撑袋、双袋或吸嘴袋。
13.权利要求7所述的包覆物的制造方法,该制造方法包括:使用挤出机将权利要求6所述的含水组合物包覆于由牵引机输送的薄膜或纸的工序。
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CN115485328A (zh) | 2022-12-16 |
JPWO2021220172A1 (zh) | 2021-11-04 |
JP2021172800A (ja) | 2021-11-01 |
WO2021220172A1 (ja) | 2021-11-04 |
DE112021002547T5 (de) | 2023-02-23 |
US20230167277A1 (en) | 2023-06-01 |
AU2021263141A1 (en) | 2022-10-06 |
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