CN116419948A - 塑料树脂改性剂组合物和使用该组合物制备热塑性材料和制品的方法 - Google Patents
塑料树脂改性剂组合物和使用该组合物制备热塑性材料和制品的方法 Download PDFInfo
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- CN116419948A CN116419948A CN202180063126.1A CN202180063126A CN116419948A CN 116419948 A CN116419948 A CN 116419948A CN 202180063126 A CN202180063126 A CN 202180063126A CN 116419948 A CN116419948 A CN 116419948A
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- thermoplastic resin
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- vinyl
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Abstract
本公开涉及热塑性树脂改性剂组合物、将该组合物转化成功能性树脂的方法以及由该树脂制备的塑料制品。
Description
技术领域
本公开涉及热塑性树脂改性剂组合物、将该组合物转化成功能性树脂的方法以及由该树脂制备的塑料制品。
背景技术
在本说明书中对现有技术的任何讨论都不应被认为是承认这种现有技术是众所周知的或构成本领域公知常识的一部分。
将防污、抗菌和抗生物膜性质赋予无生命基材以减少粘附和抑制微生物生长/定植的现有技术分为以下六个一般类别:(i)释放式杀灭,(ii)接触式杀灭,(iii)受控消耗涂层,(iv)自抛光涂层,(v)污垢释放涂层,以及(vi)上述方法的组合。
诸如释放式杀灭的技术涉及将抗菌化合物固定到表面,所述抗菌化合物随时间释放以提供抗菌作用。随着时间的推移,此类表面可能会失去其抗菌性质,因为固定的抗菌化合物被耗尽。固定的抗菌化合物也可以对其释放到的环境有害。
替代技术包括通过创建仿生表面形貌来最小化微生物粘附。然而,制造工艺复杂且昂贵,因此不适合低端行业中的批量生产。进一步的技术利用坚固的封装、刺激响应性材料、固体载体,甚至细菌自身来触发或维持灭微生物剂从载体基质中的释放。虽然抗菌性质强,但这些技术依赖于释放式杀灭,因此其有效性随着时间的推移而降低。附加技术依赖于附加装置或外部能量场,以将防污性赋予基材表面。
最近,已开开发了可扩展涂覆和无杀生物剂技术,用于生产固有的抗菌塑料配制物,而不会影响改性后基材的物理性质。然而,制造方法涉及使用由短链脂族醚、杂官能低聚(亚烷基二醇)和聚山梨醇酯组成的几种非离子表面活性剂,当在单个罐中与热自由基聚合引发剂组合时,所述非离子表面活性剂易遭受氧化降解和过氧化物的增强形成。
本公开寻求克服或改善上述缺点中的至少一些。
发明内容
在第一方面,提供了一种热塑性树脂改性剂组合物,其包含以下、由以下组成或基本上由以下组成:
(i)乙烯基单体;
(ii)可共聚酸酐;
(iii)热自由基聚合引发剂;和
(iv)热塑性树脂。
乙烯基单体可以以在约0.5%(w/w)和约4%(w/w)之间的量存在于组合物中。
可共聚酸酐可以以在约0.5%(w/w)和约4%(w/w)之间的量存在于组合物中。
热塑性树脂可以以在约90%(w/w)和约98%(w/w)之间的量存在于组合物中。
热自由基聚合引发剂可以以在约0.05%(w/w)和约4%(w/w)之间的量存在于组合物中。
乙烯基单体可包含一个或多个具有抗菌、抗病毒或防污性质的部分。
一个或多个具有抗菌、抗病毒或防污性质的部分可以是羟基、氨基或羧基。
所述一个或多个具有抗菌、抗病毒或防污性质的部分可以是:天然肽、N-取代酰胺、角鲨烯、单宁、皂苷、类黄酮、生物碱、类固醇、内酯、凝集素、内酰胺、抑菌毛剂(pilicide)、抑卷毛剂(curlicide)、烷基糖苷、氨基糖苷、含糖聚合物、糖脂类、糖酯、季铵化合物、萜烯、萜类化合物、脂肪酸、脂肪酸酯、烷基胺、烷基胺氧化物、醇烷氧基化物、硝基氧、卤胺、二芳基醚、氧杂蒽酮、醌、香豆素、聚乙炔、胍、卤素、磷酸基(phospho)衍生物、磺酸基(sulfo)衍生物、酚衍生物、苯甲酸衍生物、有机金属、吡啶鎓衍生物、哌嗪衍生物、吡咯烷酮衍生物、苯胺衍生物、双胍和相关化合物、肟和相关化合物、异噻唑啉酮和相关化合物、吲哚衍生物、杂唑衍生物、杂吡咯啉衍生物、酰肼-腙衍生物、吡喃和相关化合物、呋喃和相关化合物、大环内酯、四环素、噁唑烷酮、喹诺酮、氨肟、酰胺胺和聚丙烯亚胺。
乙烯基单体可以是短链烯烃、苯乙烯、丙烯酸烷基酯、烷基丙烯酸酯、乙酸乙烯酯、乙烯醇、乙烯基苯酚、乙烯基烷基醚、乙烯基卤化物、乙烯基乙酸、丙烯腈、丙烯酰胺、乙烯基硅烷、乙烯基硫化物、乙烯基砜、乙烯基亚砜、碳酸乙烯亚乙酯、乙烯基吡咯烷酮、乙烯基咔唑、乙烯基降冰片烯、不饱和脂肪酸或不饱和脂肪酸酯。
在一个实施方案中,乙烯基单体是苯乙烯、α-甲基苯乙烯、乙烯基萘、异丁烯、乙烯基降冰片烯、丁基乙烯基醚或2-氯乙基乙烯基醚。
热塑性树脂改性剂组合物可包含多个乙烯基单体。
在一些实施方案中,多个乙烯基单体可以选自乙酸乙烯酯、丙烯酰胺、N-异丙基丙烯酰胺、N-乙烯基吡咯烷酮、N-羟甲基丙烯酰胺、丙烯酰胺基乙醇酸、丙烯腈、甲基丙烯酸、甲基丙烯酸甲酯、甲基丙烯酸2-羟乙酯、甲基丙烯酸2-氨基乙酯、甲基丙烯酸2-(二甲基氨基)乙酯、3-甲基丙烯酰氧基丙基三甲氧基硅烷、丙烯酸2-羧乙酯、甲基丙烯酸2-氮杂环庚烷乙酯、甲基丙烯酸缩水甘油酯、2-乙烯基吡啶、4-叔丁氧基苯乙烯和4-乙烯基邻苯二酚缩丙酮。
可共聚酸酐可以是有机酸酐,诸如马来酸酐或四氢化邻苯二甲酸酐。
热自由基聚合引发剂可以是过氧化物或偶氮化合物。
在一个实施方案中,自由基聚合引发剂可以是过氧化苯甲酰和过氧化二异丙苯的混合物。
过氧化苯甲酰和过氧化二异丙苯可以约20∶80和约80∶20之间的摩尔比存在。
热塑性树脂可以是中至高流动均聚烯烃、多嵌段共聚物、无规共聚物或其混合物。
热塑性树脂可以是加成聚合物、聚烯烃弹性体、热塑性烯烃或橡胶。
热塑性树脂可以是PE、PP、PB、COC、PMP、PVB、PAN、NBR、EPR、PI、SEBS、SEPS、SBS、SIS、MBS、ABS、EBA、EVA、EVOH、EAA、EMA、EPDM、ETFE、ECTFE、EVCL、聚(乙烯-共-1-辛烯)、聚(乙烯-共-1-己烯)、氯丁橡胶、烯烃复分解产物或其任何组合。
热塑性树脂改性剂组合物可进一步包含有机溶剂。
热塑性树脂改性剂组合物可进一步包含除臭剂。
热塑性树脂改性剂组合物可以不含或基本上不含表面活性剂,例如非离子表面活性剂。
在第二方面,提供了一种制备改性热塑性树脂组合物的方法,该方法包括以下、由以下组成或基本上由以下组成:将
(i)乙烯基单体;
(ii)可共聚酸酐;
(iii)热自由基聚合引发剂;和
(iv)热塑性树脂组合以便提供混合物,
并使该混合物经受熔融处理或溶剂辅助固相聚合。
乙烯基单体可以以在约0.5%(w/w)和约4%(w/w)之间的量存在于混合物中。
可共聚酸酐可以以在约0.5%(w/w)和约4%(w/w)之间的量存在于混合物中。
热塑性树脂可以以在约90%(w/w)和约98%(w/w)之间的量存在于混合物中。
热自由基聚合引发剂可以以在约0.05%(w/w)和约4%(w/w)之间的量存在于混合物中。
熔融处理可包括挤出、模塑、吹膜、纺丝、拉伸、挤压、捏合、辊轧或热成型。在一个实施方案中,熔融处理包括挤出。
乙烯基单体、可共聚酸酐、热自由基聚合引发剂和热塑性树脂中的每一种可以如第一方面中所定义。
该混合物可以进一步包含有机溶剂。
该混合物可以进一步包含除臭剂。
该混合物可以不含或基本上不含表面活性剂,例如非离子表面活性剂。
该混合物可以仅包含组分(i)-(iv)。
可以使改性的热塑性树脂组合物经受表面处理。
表面处理可以是将防污、防油和/或防水性质赋予给改性热塑性树脂组合物的处理。
在第三方面,提供了每当通过第二方面的方法制备的改性热塑性树脂组合物。
在第四方面,提供了一种制备功能性树脂组合物的方法,包括将第三方面的改性热塑性树脂组合物与一种或多种添加剂组合以形成混合物,并使该混合物经受熔融处理。
一种或多种添加剂可以以在约90%(w/w)和约99%(w/w)之间的量存在于组合物中。
一种或多种添加剂可包括一种或多种具有抗菌、抗病毒或防污性质的化合物。
一种或多种具有抗菌、抗病毒或防污性质的化合物可以以在约0.05%(w/w)和约2%(w/w)之间的量存在于组合物中。
一种或多种具有抗菌、抗病毒或防污性质的化合物可以是亲水化合物。
一种或多种具有抗菌、抗病毒或防污性质的化合物可以是两亲化合物。
一种或多种具有抗菌、抗病毒或防污性质的化合物可以是一种或多种醇乙氧基化物。
两亲化合物可以具有大于约7的HLB值。
两亲化合物可以具有在约7和约20之间的HLB值。
一种或多种添加剂可以包括芯材树脂。
芯材树脂可以以在约90%(w/w)和约99%(w/w)之间的量存在于组合物中。
一种或多种添加剂可以包括抗氧化剂。
熔融处理可包括挤出、模塑、吹膜、纺丝、拉伸、挤压、捏合、辊轧或热成型。
熔融处理可以包括挤出。
在第五方面,提供了每当通过第四方面的方法制备的功能性树脂组合物。
在第六方面,提供了一种用于生产塑料制品的方法,包括使第五方面的功能性树脂组合物成形。
成形可以通过模塑实现。
模塑可以是注射模塑、旋转模塑、吹塑或压缩模塑。
在第六方面的实施方案中,提供了一种制备塑料制品的方法,包括:
(i)将:
(a)改性热塑性树脂组合物;
(b)芯材树脂;和
(c)选自醇乙氧基化物、环氧烷和聚乙二醇的化合物组合以形成混合物;
(ii)使该混合物经受熔融处理或溶剂辅助固相聚合,以提供功能性树脂组合物;和
(iii)使所述功能性树脂组合物成形以提供塑料制品,
并且其中所述改性热塑性树脂组合物通过混合:
(d)乙烯基单体;
(e)可共聚酸酐;
(f)热自由基聚合引发剂;和
(g)热塑性树脂以形成混合物,和
(iv)使混合物经受熔融处理或溶剂辅助固相聚合而制备。
在包含(a)、(b)、(c)的混合物中,组分(a)可以以在约0.5%(w/w)和约3%(w/w)之间的量存在,组分(b)可以以在约95%(w/w)和约99%(w/w)之间的量存在,并且组分(c)可以以在约0.05%(w/w)和约3%(w/w)之间的量存在。
在包含(d)、(e)、(f)和(g)的混合物中,组分(d)可以以在约0.5%(w/w)和约5%(w/w)之间的量存在,组分(e)可以以在约0.5%(w/w)和约5%(w/w)之间的量存在,组分(f)可以以在约0.05%(w/w)和约3%(w/w)之间的量存在,并且组分(g)可以以在约90%(w/w)和约99%(w/w)之间的量存在。
包含(d)、(e)、(f)和(g)的混合物可以仅包含组分(d)、(e)、(f)和(g)。
芯材树脂可以是聚丙烯。
聚丙烯可以是聚丙烯无规共聚物。
在步骤(c)中,所述化合物可以是醇乙氧基化物。
醇乙氧基化物可具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=3至23。
醇乙氧基化物可具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=3至9。
醇乙氧基化物可以具有在约10和11之间的HLB 10值。
步骤(ii)和(iv)中的熔融处理可以包括挤出。
步骤(i)中的混合物可进一步包含抗氧化剂。
乙烯基单体可以是苯乙烯。
可共聚酸酐可以是马来酸酐。
热自由基聚合引发剂可以是过氧化二异丙苯。
热塑性树脂可以是聚丙烯。
(d)、(e)、(f)和(g)的混合物可以不含或基本上不含表面活性剂。
步骤(iii)中的成形可以通过模塑进行。
该模塑可以是注射模塑。
塑料制品可以是抗蛋白塑料制品。
塑料制品可以是抗菌和/或抗病毒制品。
在第七方面,提供了一种生产塑料制品的方法,该方法包括将第三方面的改性热塑性树脂组合物与一种或多种添加剂组合以形成母料,将母料与芯材树脂组合以形成混合物,并处理该混合物以形成塑料制品。
在第八方面,提供了一种用于生产塑料制品的方法,包括将第三方面的改性热塑性树脂组合物与母料和芯材树脂组合以形成混合物,并处理该混合物以形成塑料制品。
母料可包含一种或多种具有抗菌、抗病毒或防污性质的化合物。
一种或多种具有抗菌、抗病毒或防污性质的化合物可以是亲水化合物。
一种或多种具有抗菌、抗病毒或防污性质的化合物可以是两亲化合物。
两亲化合物可以具有大于约7的HLB值。
两亲化合物可以具有在约7和约20之间的HLB值。
在第八方面的实施方案中,提供了一种制备塑料制品的方法,包括:
(i)将:
(a)改性热塑性树脂组合物;
(b)芯材树脂;和
(c)包含醇乙氧基化物、环氧烷或聚乙二醇的母料组合以形成混合物;和
(ii)使混合物成形以提供塑料制品,
其中所述改性热塑性树脂组合物通过混合:
(d)乙烯基单体;
(e)可共聚酸酐;
(f)热自由基聚合引发剂;和
(g)热塑性树脂以形成混合物,和
(iii)使(d)、(e)、(f)和(g)的混合物经受熔融处理或溶剂辅助固相聚合而制备。
在包含(a)、(b)、(c)的混合物中,组分(a)可以以在约5%(w/w)和约15%(w/w)之间的量存在,组分(b)可以以在约80%(w/w)和约95%(w/w)之间的量存在,并且组分(c)可以以在约1%(w/w)和约7.5%(w/w)之间的量存在。
在包含(d)、(e)、(f)和(g)的混合物中,组分(d)可以以在约0.5%(w/w)和约5%(w/w)之间的量存在,组分(e)可以以在约2%(w/w)和约10%(w/w)之间的量存在,组分(f)可以以在约0.05%(w/w)和约3%(w/w)之间的量存在,并且组分(g)可以以在约90%(w/w)和约99%(w/w)之间的量存在。
母料可以进一步包含芯材树脂。
母料可以是通过熔融混合醇乙氧基化物、环氧烷或聚乙二醇和芯材树脂来制备的母料。
芯材树脂可以是聚丙烯。
聚丙烯可以是聚丙烯无规共聚物。
芯材树脂可以是热塑性弹性体。
母料可以包含醇乙氧基化物。
醇乙氧基化物可具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=3-9。
醇乙氧基化物可具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=5。
醇乙氧基化物可以具有在10和11之间的HLB值。
步骤(ii)中的成形可以通过模塑进行。
该模塑可以是注射模塑。
步骤(iii)中的熔融处理可以包括挤出。
乙烯基单体可以是苯乙烯。
热塑性树脂可以是热塑性弹性体。
可共聚酸酐可以是马来酸酐。
热自由基聚合引发剂可以是过氧化二异丙苯。
(d)、(e)、(f)和(g)的混合物可以不含或基本上不含表面活性剂。
塑料制品可以是抗蛋白塑料制品。
塑料制品可以是抗菌和/或抗病毒制品。
在第九方面,提供了每当通过第六至第八方面中任一个的方法获得的塑料制品。
定义
以下是可能有助于理解本公开的描述的一些定义。这些旨在作为一般定义,并且决不应将本公开的范围仅限于这些术语,而是为了更好地理解以下描述而提出的。
在本说明书中,除非上下文另有要求,否则词语“包含(comprise)”或变体诸如“包含(comprises)”或“包含(comprising)”将被理解为暗示包含所述元素、整数或步骤,或元素、整数和步骤组,但不排除任何其他元素、整数或步骤,或元素、整数或步骤组。
术语“一(a)”和“一个(an)”在本文中用于指该冠词的语法对象中的一个或多于一个(即,至少一个)。举例来说,“元素(an element)”是指一种元素或多于一种元素。
在本说明书的上下文中,术语“约”被理解为是指本领域技术人员在实现相同功能或结果的上下文中认为等同于所述值的一系列数字。
本文所述的任何数值范围旨在包括包含在所述范围内的相同数值精度的所有子范围。例如,1.0至5.0的范围旨在包括所述最小值1.0和所述最大值5.0之间的所有子范围,即,具有等于或大于1.0的最小值和等于或小于5.0的最大值,诸如2.1至4.5。本文所述的任何最大数值限制旨在包括其中包含的所有较低数值限制,并且本文所述任何最小数值限制旨在包含其中包含的所有较高数值限制。
在提及表面活性剂含量时使用的术语“基本上不含”是指表面活性剂占混合物或组合物的小于约3%(w/w)、或小于约2%(w/w)、或小于约1%(w/w)、或小于约0.5%(w/w)、或小于约0.1%(w/w)、或小于约0.05%(w/w)、或小于约0.01%(w/w)、或小于约0.005%(w/w)。
附图说明
图1:生产根据本公开的实施方案的塑料制品的方法。
图2:与市售塑料制品的蛋白结合能力相比,根据本公开的一个实施方案制备的塑料制品的蛋白结合能力。
具体实施方式
本发明人已经开发了树脂改性剂组合物和可用于制备塑料制品的基于热塑性树脂的功能性树脂组合物。制品的表面可以调整为具有抗菌、抗病毒和/或防污性质。抗菌、抗病毒和/或防污性质内置于表面,并且不依赖于灭微生物剂的迁移、表面涂层的使用或制品的化学损耗。另外,制品的性能是稳定的,因为抗菌性、抗病毒性和/或防污性的效力受到制品的表面形态、接触介质的组成和外部环境压力(诸如辐照和高压灭菌和清洗的重复循环)的影响最小。所述制品提供优于现有技术的那些的显著优点,因为它们不易遭受分层或磨损,并且它们的抗菌、抗病毒和防污性质不会随时间而降低。
组合物
在一个方面,提供了一种热塑性树脂改性剂组合物,其包含以下、由以下组成或基本上由以下组成:
(i)乙烯基单体;
(ii)可共聚酸酐;
(iii)热自由基聚合引发剂;和
(iv)热塑性树脂。
该组合物可包含至少85%(w/w)、或至少86%(w/w)、或至少87%(w/w)、或至少88%(w/w)、或至少89%(w/w)、或至少90%(w/w)、或至少91%(w/w)、或至少92%(w/w)、或至少93%(w/w)、或至少94%(w/w)、或至少95%(w/w)、或至少96%(w/w)、或至少97%(w/w)、或至少98%(w/w)的热塑性树脂。在一些实施方案中,该组合物包含在约85%(w/w)和约98%(w/w)之间、或在约86%(w/w)和约98%(w/w)之间、或在约87%(w/w)和约98%(w/w)之间、或在约88%(w/w)和约98%(w/w)之间、或在约89%(w/w)和约98%(w/w)之间、或在约90%(w/w)和约98%(w/w)之间、或在约91%(w/w)和约98%(w/w)之间、或在约92%(w/w)和约98%(w/w)之间、或在约93%(w/w)和约98%(w/w)之间的热塑性树脂。
可共聚酸酐可以是以下通式(I)的有机酸酐,其中R1和R2是有机残基。
R1和R2以及它们所连接的碳和中心氧原子可以形成环结构。环结构可以是单环、双环、三环或四环的。有机酸酐的非限制性实例包括马来酸酐、邻苯二甲酸酐、四氢化邻苯二甲酸酐、萘四羧酸二酐以及它们的同构类似物,包括马来酰亚胺(例如,马来酰亚胺、降冰片烯二甲酰亚胺、N-乙氧羰基马来酰亚胺、N-氨基甲酰基马来酰亚胺、N-苯基马来酰亚胺、N-(4-羧基苯基)马来酰亚胺和具有不同N-取代基的N-乙基马来酰亚胺)、马来酸酯(例如,马来酸二丁酯和蓖麻油酸噁唑啉马来酸酯)、富马酸,以及柠康酸和衣康酸的酸酐、酯和酰亚胺衍生物。
在一个实施方案中,乙烯基单体包含一个或多个具有抗菌、抗病毒或防污性质的部分。具有抗菌、抗病毒或防污性质的部分包括例如羟基、氨基、羧基、醚、取代环、稠环和杂环基团。一些部分是典型的由亲水和疏水单元组成的表面活性剂结构。抗菌和抗病毒部分的非限制性实例包括但不限于天然肽、N-取代酰胺、角鲨烯、单宁、皂苷、类黄酮、生物碱、类固醇、内酯、凝集素、内酰胺、抑菌毛剂、抑卷毛剂、烷基糖苷、氨基糖苷、含糖聚合物、糖脂类、糖酯、季铵化合物、萜烯、萜类化合物、脂肪酸、脂肪酸酯、烷基胺、烷基胺氧化物、醇烷氧基化物、硝基氧、卤胺、二芳基醚、氧杂蒽酮、醌、香豆素、聚乙炔、胍、卤素、磷酸基衍生物、磺酸基衍生物、酚衍生物、苯甲酸衍生物、有机金属、吡啶鎓衍生物、哌嗪衍生物、吡咯烷酮衍生物、苯胺衍生物、双胍和相关化合物、肟和相关化合物、异噻唑啉酮和相关化合物、吲哚衍生物、杂唑衍生物、杂吡咯啉衍生物、酰肼-腙衍生物、吡喃和相关化合物、呋喃和相关化合物、大环内酯、四环素、噁唑烷酮、喹诺酮、氨肟、酰胺胺和聚丙烯亚胺。
在一些实施方案中,乙烯基单体是短链烯烃、苯乙烯、丙烯酸烷基酯、烷基丙烯酸酯、乙酸乙烯酯、乙烯醇、乙烯基苯酚、乙烯基烷基醚、乙烯基卤化物、乙烯基乙酸、丙烯腈、丙烯酰胺、乙烯基硅烷、乙烯基硫化物、乙烯基砜、乙烯基亚砜、碳酸乙烯亚乙酯、乙烯基吡咯烷酮、乙烯基咔唑、乙烯基降冰片烯、不饱和脂肪酸或不饱和脂肪酸酯。
在替代实施方案中,乙烯基单体是以下单体中的一种或多种:
其中R3至R7独立地选自:H、C1-C10烷基、苯基、卤素、OH、氰基和OC1-C6烷基,并且其中所述单体各自任选地包含以下中的一种或多种或与以下中的一种或多种缀合:天然肽、N-取代酰胺、角鲨烯、单宁、皂苷、类黄酮、生物碱、类固醇、内酯、凝集素、内酰胺、抑菌毛剂、抑卷毛剂、烷基糖苷、氨基糖苷、含糖聚合物、糖脂类、糖酯、季铵化合物、萜烯、萜类化合物、脂肪酸、脂肪酸酯、烷基胺、烷基胺氧化物、醇烷氧基化物、硝基氧、卤胺、二芳基醚、氧杂蒽酮、醌、香豆素、聚乙炔、胍、卤素、磷酸基衍生物、磺酸基衍生物、酚衍生物、苯甲酸衍生物、有机金属、吡啶鎓衍生物、哌嗪衍生物、吡咯烷酮衍生物、苯胺衍生物、双胍和相关化合物、肟和相关化合物、异噻唑啉酮和相关化合物、吲哚衍生物、杂唑衍生物、杂吡咯啉衍生物、酰肼-腙衍生物、吡喃和相关化合物、呋喃和相关化合物、大环内酯、四环素、噁唑烷酮、喹诺酮、氨肟、酰胺胺和聚丙烯亚胺,或其任何组合。
热自由基聚合引发剂是本领域技术人员熟知的,并且包括例如过氧化物和偶氮化合物。合适的过氧化物的实例包括二酰基过氧化物(诸如过氧化苯甲酰和过氧化二月桂酰)、二烷基过氧化物(诸如二叔丁基过氧化物和过氧化二异丙苯)、过酸酯(诸如过苯甲酸叔丁酯)、酮过氧化物(诸如过氧化甲乙酮)以及以商品名 和/>出售的商业有机过氧化物。合适的偶氮化合物的实例包括偶氮二异丁腈(AIBN)、1,1'-偶氮二(环己甲腈)(ACHN)和以商品名VazoTM出售或由Vesta Chemicals和Fujifilm Wako Chemicals提供的商业偶氮产品。
除了考虑反应温度和特定的热塑性树脂改性剂组合物之外,还基于以下几个因素选择合适的热自由基聚合引发剂,包括其油/水溶解性(相对于液体乙烯基单体)、效率因数、分解半衰期、氢可提取性(hydrogen abstractability)、初级自由基的稳定性、分解副产物的形成和对诱导/氧化还原分解的敏感性,所述因素决定了接枝与非接枝聚合,从而控制乙烯基单体和可共聚酸酐接枝到聚合物骨架上的效率、程度、长度、分布、微观结构和顺序,以防许多可能的副反应,所述副反应结束笼闭反应、β-断裂、自由基/增长链的过早终止和链转移反应为较低反应性的中间体。抑制这些副反应可能有助于防止不希望的后处理观察结果,诸如凝胶形成、变色、气味、起霜以及热塑性树脂的熔体流动指数和物理性质的显著变化。
基于过氧化物的引发剂通常更易于通过烃物质的氢提取或分子内反咬(back-biting)发生接枝反应和分支/交联形成,但与偶氮引发剂相比不太容易形成直链聚合物。为了完成接枝反应,当确定热处理的最佳状态时,在熔融处理设备内发生的总反应时间或停留时间优选在引发剂在所需反应温度下的半衰期的约1至4倍的范围内。虽然熔融处理(诸如反应挤出)通常可涉及从螺杆挤出机的前部(即进料区和过渡区)到后部(即计量区和模具区)逐渐增加的温度分布,但在组合物中以20∶80至80∶20的摩尔比使用一种较短寿命的引发剂(诸如过氧化苯甲酰)和一种较长寿命的引发剂(诸如过氧化二异丙苯)的混合体系可在整个聚合物熔融配混过程中保持高的引发效率和接枝率。
基于有机过氧化物的引发剂包括广泛的分解半衰期和溶解性。以下是以分解半衰期升序排列的基于过氧化物的引发剂的一般类别的列表:过酸酯、过氧化二碳酸酯、烷基过氧化碳酸酯、二酰基过氧化物、过缩酮、酮过氧化物、过酸、二烷基过氧化物、氢过氧化物和甲硅烷基过氧化物。
在优选的实施方案中,乙烯基单体是通过带有至少一个电子供体取代基而具有高电子密度双键和疏水分子的电子供体,诸如苯乙烯、α-甲基苯乙烯、乙烯基萘、异丁烯、乙烯基降冰片烯、丁基乙烯基醚和2-氯乙基乙烯基醚。当制备改性热塑性树脂组合物时,乙烯基单体倾向于与酸酐、电子受体和亲水分子共聚成交替或无规的多嵌段共聚物,该多嵌段共聚物赋予强烈的两亲性。
改性热塑性树脂组合物中的所形成的共聚物被锚定为热塑性树脂主链上的导致毛状或梳状结构的多个短分支,因此它们具有表面活性,并且在与干燥或潮湿环境接触时将自由地迁移到表面,以在表面处产生污垢释放和自清洁效果。虽然它们共价连接到基材,但这不会导致任何浸出问题。
化学接枝物上具反应性且可水解性的酸酐部分本质上是双官能的。它们一方面可以用来捕获并与带有醇、胺和亲核物质的添加剂化合物化学结合导致一些超支化微观结构,另一方面可以用来改善与其他极性热塑性材料的粘附或相容性,这可导致增韧的合金。这种方法优于商业偶联剂的替代使用,所述商业偶联剂诸如丙烯酸改性聚烯烃、聚烯烃接枝马来酸酐树脂、聚烯烃接枝甲基丙烯酸缩水甘油酯树脂以及苯乙烯、马来酸酐和N-苯基马来酰亚胺的一些无规共聚物,它们以商品名(Nippon Paper Industries)、PolybondTM(ChemPoint)、/>(Clariant)、/>(Eastman Chemicals)、ExxelorTM(ExxonMobil)、/>(Honeywell)、GraftabondTM(Graft Polymer)、/>(Polyscope Polymers)、IP(Denka)、/>(Polyram)、Lustran(Styrolution)、AmplifyTM(Dow)、/>(Arkema)、/>(Arkema)和/>(DuPont)以各种级别获得。尽管后者看起来更简单,但这两种方法产生了不同的聚合物微观结构。对于后者,偶联剂在分散在热塑性树脂的基质中后仅提供酸酐或羧酸基团的固定反应性锚,而不是开放式突出臂,该开放式突出臂能够从本体基质中分离并在短时间尺度内利用疏水/亲水单元或短链段的快速表面重建创建自适应刷状拓扑结构,如本公开中的。虽然接枝长度是不受控制的,并且本质上是多分散的,但具有混合链长度的接枝将通过包括较短链的刷下层阻止小溶质的吸附并抵消较长链的表面密度降低的不利影响而显著增强基材表面的防污性,所述小溶质能够扩散到被栓住的刷的空隙和间隙中。
乙烯基单体(作为供体)和酸酐(作为受体)的接枝共聚的交替趋势与热塑性树脂改性剂组合物的进料比和总单体转化率有关。如果总单体转化率低于15%,则可从含有30至70摩尔%受体的组合物进料中获得交替聚合物。如果总单体转化率高于80%,则通常从等摩尔或接近等摩尔进料比获得严格交替的共聚物。然而,当使用非等摩尔进料时,链对链组成偏差是不可避免的。除了控制热塑性树脂改性剂组合物的乙烯基单体和酸酐之间的进料比之外,三种其他条件可能有利于这种二元体系的交替,并实现更高的接枝效率:(i)两种组分的反应性比率(r1和r2)的乘积落在0和1之间(该r1和r2是非零的并且与不超过60∶1的r1∶r2(r1≥r2)相当接近),更优选接近于零;(ii)它们的根据Alfrey-Price Q-e方案的e系数(其中Q表示单体反应性(共振稳定的度量),并且e表示其极化(极性效应的度量))差异很大并且更优选地在幅度上是大的并且具有相反的符号;和(iii)乙烯基单体或酸酐对热塑性树脂的聚合物大分子基团的反应性优选大于其对应物,诸如其形成稳定大分子基团并且所得自由基容易与其对应物共聚从而产生接枝分子络合物的能力。例如,苯乙烯是乙烯基单体的优选,它能够生成稳定的苯乙烯基大分子基团。据报道,苯乙烯和马来酸酐(具有可比Q系数的典型给体-受体单体对)的反应性比率、Q系数和e系数分别为(0.04,1,-0.8)和(0,0.86,+3.69),并且因此在等摩尔进料比下具有产生交替接枝的强烈倾向。原则上,通过使大于一种类型的乙烯基单体作为共聚单体是可行的,所述乙烯基单体诸如乙酸乙烯酯、丙烯酰胺、N-异丙基丙烯酰胺、N-乙烯基吡咯烷酮、N-羟甲基丙烯酰胺、丙烯酰胺基乙醇酸、丙烯腈、甲基丙烯酸、甲基丙烯酸甲酯、甲基丙烯酸2-羟乙酯、甲基丙烯酸2-氨基乙酯、甲基丙烯酸2-(二甲基氨基)乙酯、3-甲基丙烯酰氧基丙基三甲氧基硅烷、丙烯酸2-羧乙酯、甲基丙烯酸2-氮杂环庚烷乙酯(2-azepane ethyl methacrylate)、甲基丙烯酸缩水甘油酯、2-乙烯基吡啶、4-叔丁氧基苯乙烯以及具有组合物进料中的主要单体和酸酐之间的中间极性的4-乙烯基邻苯二酚缩丙酮。最后两个共聚单体实例可随后用路易斯酸/布朗斯台德酸脱保护,以在接枝上形成苯酚和邻苯二酚部分,并显示出强力的抗氧化和抗菌活性。与酸酐相比,双官能共聚单体,诸如N-羟甲基丙烯酰胺和丙烯酰胺基乙醇酸,是潜在的偶联剂,并且带环氧基的共聚单体诸如甲基丙烯酸缩水甘油酯,是通用的反应性偶联剂。共聚单体混合物中的乙烯基单体中的至少一种优选为具有更负e系数的电子供体,以便进行多组分共聚,从而可能产生受体-给体-受体三元共聚物接枝结构。
在一些实施方案中,热塑性树脂是加成聚合物。加成聚合物是通过单体连接而在没有其他产物共同产生的情况下形成的聚合物,并且是本领域技术人员熟知的。在另一个实施方案中,热塑性树脂是聚烯烃弹性体(POE)。POE是基于聚乙烯骨架的弹性体,并且在本领域技术人员中也是熟知的。在另一个实施方案中,含烯烃的热塑性树脂是橡胶。橡胶可以是天然橡胶或合成橡胶。
在一些实施方案中,热塑性树脂包括但不限于:聚乙烯(PE)、聚丙烯(PP)、聚丁烯(PB)、环烯烃共聚物(COC)、聚甲基戊烯(PMP)、聚乙烯醇缩丁醛(PVB)、聚丙烯腈(PAN)、丁腈橡胶(NBR)、乙丙橡胶(EPR)、聚(乙烯-共-1-辛烯)、聚(乙烯-共-1-己烯)、氯丁橡胶、聚异戊二烯(PI)、聚(苯乙烯-乙烯-丁烯-苯乙烯)(SEBS)、聚(苯乙烯-乙烯-丙烯-苯乙烯)(SEPS)、聚(苯乙烯-丁二烯-苯乙烯)(SBS)、苯乙烯-异戊二烯嵌段共聚物(SIS)、甲基丙烯酸甲酯-丁二烯-苯乙烯(MBS)、丙烯腈丁二烯苯乙烯(ABS)、乙烯丙烯酸丁酯共聚物(EBA)、乙烯乙酸乙烯酯(EVA)、乙烯乙烯醇(EVOH)、乙烯丙烯酸(EAA)、乙烯丙烯酸甲酯(EMA)、乙烯丙烯二烯单体(EPDM)、乙烯四氟乙烯(ETFE)、乙烯氯三氟乙烯(ECTFE)、乙烯-氯乙烯(EVCL)、烯烃复分解产物,包括它们的组合。
在优选的实施方案中,热塑性树脂是中至高流动的均聚烯烃、多嵌段共聚物和无规共聚物,以及衍生自两种或更多种单体物质的此类共聚物的共混物,并且表现出由多相体系中的相分离和/或结晶驱动的均匀分散但小尺寸的畴(domain)形态。热塑性树脂的熔体流动指数更优选为5g/10min(190℃/2.16kg)或以上。众所周知,热塑性树脂的冲击和高光泽性能取决于结晶度。结晶度随着立构规整性的降低而降低,并且材料显示出更高的弹性但更小的雾度。已知许多用于控制相分离和结晶的方法,诸如通过引入立构缺陷、通过短链支化、通过引入共聚单体以及通过添加成核剂加速结晶和增加核形成的数量。热塑性树脂优选为无定形或低结晶等级的热塑性弹性体和聚α-烯烃。这些市售树脂中的大多数主要包括乙烯和/或丙烯重复单元,实例有诸如Vistamaxx、Exact、Optema、EMAC、EBAC、Notio、Tafmer、Vestoplast、Lutene、Lumicene、L-Modu、Versify、Engage、Elvax、Lotryl、Evatane、Elvaloy AC、Clyrell、Tafthren、Tefabloc、Kraton G等。
乙烯基单体、可共聚酸酐、热自由基聚合引发剂和其他添加剂可能不彼此良好溶解。这可以通过将它们以相对于可共聚酸酐约1∶3至1∶2的重量比混合在有机溶剂或溶剂混合物中,然后在熔融处理之前与热塑性树脂配混来协助。可通过向引发剂添加一种或多种具有不同极性和惰性的溶剂来调节溶解性。溶剂的实例包括四氯化碳、异丙醇、四氢呋喃、乙酸乙酯、苯、甲苯、甲基乙基酮、邻二氯苯、二甲基甲酰胺、N,N-二甲基乙酰胺、N,N-二甲基苯胺、4,N,N-三甲基苯胺、二甲基亚砜、亚磷酸三苯酯、亚磷酸三(壬基苯基)酯、己内酰胺、液体石蜡、无臭溶剂油、异十二烷、异丙基苯、1,3-二异丙基苯、环己基苯和一些高度支化的异十六烷。所选择的溶剂种类在一定程度上可以调节乙烯基单体和可共聚酸酐在热塑性树脂的聚合物骨架上的聚合与接枝,这取决于它们的极性、极化性、挥发性、给电子/吸电子能力和链转移常数。含有氮、磷或硫原子且衍生自诸如酰胺、内酰胺、氨基甲酸酯、胺氧化物、亚磷酸酯、磷酸酯、膦酸酯、磷酰胺、氧化膦、一硫化物、亚砜、芳基二硫化物和噻唑基二硫化物的溶剂可充当亲电单体或酸酐的电子供体以及交联(凝胶化)、降解和均聚的抑制剂,但接枝共聚的促进剂。这种效果可以通过小剂量的自由基/二氧清除剂、活性链转移剂或助催化剂与初级自由基、单体自由基和大分子基团相互作用来促进,其剂量范围为约十分之一至十分之二重量份的热自由基聚合引发剂,所述自由基/二氧清除剂、活性链转移剂或助催化剂诸如对苯醌、二苯甲酮、苯基-2,4,6-三甲基苯甲酰基亚膦酸锂、苯并三唑、羟基苯基三嗪、醌甲基化物、4-羟基-2,2,6,6-四甲基哌啶-1-氧基、2-氰基-2-丙基苯并二硫、丁基化羟基甲苯、四硫化双五亚甲基秋兰姆、三(2,4-二叔丁基苯基)亚磷酸酯、辛基硫醇锡、辛基羧酸锡、邻苯二甲酸二丁酯、硬脂酰胺、抗坏血酸、硫代巴比妥酸、N-乙酰氧基-邻苯二甲酰亚胺、锌盐、碘鎓盐、锍盐和衍生自硫醇的化合物、硫醚、硫代碳酸酯、硫酯、硫代氨基甲酸酯、黄原酸酯、磺脲、烷氧基胺、咪唑基硝酮、多不饱和脂肪酸、受阻酚、受阻胺、有机硅氢化物、有机硼烷、烷基铝、过硫酸盐、内鎓盐、金属内鎓盐络合物和过渡金属(诸如Sn(II)、Sb(III)、Pb(II)、Bi(III)、Fe(II)、Ti(II)、Ti(III)、Mn(II)、Mn(III)或Ge(II))络合物。
除臭剂的含量可在0.5%(w/w)至1%(w/w)之间,用于吸收或中和由于在熔融处理期间未反应/蒸发的酸酐或酸、挥发性杂质的排气以及涉及胺和硫组分(诸如硫化氢、硫醇和硫醚)的官能团的其他反应而产生的刺鼻气味的痕迹。除臭剂的合适实例包括膨润土、活性炭、金属交换的沸石、钾明矾、硅胶、滑石粉、碱性吸附剂、云母、硅藻土和市场上可获得的一些其他商业产品,诸如含有蓖麻醇酸锌的含有环氧乙烷反应性基团的以及/>RP 17。
热塑性树脂改性剂组合物可通过将热塑性聚合物树脂(可以是颗粒或粉末形式)、乙烯基单体(可以是液体或糊状形式)、可共聚酸酐和热自由基聚合引发剂以以下量来组合而制备:
·热塑性树脂:约90%(w/w)至约98%(w/w)
·乙烯基单体:约0.5%(w/w)至约4%(w/w)
·可共聚酸酐:约0.5%(w/w)至约4%(w/w)
·热自由基聚合引发剂:约0.05%(w/w)至约2%(w/w)。
然后,所得混合物可在封闭室中经受振荡摇动或机械搅拌。在混合、涂覆和尺寸减小设备的帮助下,可以更均匀地进行千克生产规模的混合,所述设备有诸如叶片混合器、螺带混合器、3维转筒混合器、班布里混合器、分散捏合机、固体盘式涂布机、流化床粉末涂布机、雾化器、喷粉涂布机、低温或非低温塑料粉碎机或球磨机,其优选配备有温度控制和惰性气体供给以最小化剪切加热效应。
然后可以通过熔融处理热塑性树脂改性剂组合物来制备改性热塑性树脂组合物。熔融处理可涉及加热(熔化)和冷却(凝固)的一个完整循环,其中该方法包括四个主要模块:(a)进料单元;(b)熔化/输送单元;(c)定型/冷却单元;和(d)卷绕/造粒/成形单元。颗粒或丸粒形式的固体树脂可以研磨成细粉末,以增强与其他起始材料混合的均匀性。如果机器配备有自动液体进料机、计量泵或可包括用于连续生产的任何高精度计量单元(其可以是体积的、光学的和重量的),则固体和液体形式的起始材料可以分别进料到熔化/输送单元,例如螺旋型挤出机。在大量液体试剂的情况下,当固液混合物在进料单元中随时间沉淀时,树脂上的干混合将导致液体滴落。由于大多数乙烯基单体可溶于非极性有机溶剂,因此可以使用多孔的有机改性无机产品(诸如粘土、滑石、沸石、二氧化硅、气凝胶、飞灰等)或可热降解的聚烯烃烃超吸收剂(所谓的“petrogel”),该超吸收剂在释放液体试剂的同时,在其重量上表现出快速且高的吸油能力,或者甚至在高温下加热时破裂用于爆裂释放。该超吸收剂可以是含有一种或多种短链脂族烃(比如说乙烯、1-己烯、1-辛烯、1-癸烯等)、苯乙烯和二乙烯基苯单元的精细聚丙烯纤维或轻度交联聚烯烃共聚物。除了挤出机之外,可以考虑使用微波辐射作为成形和焊接的手段以及使用微波接收添加剂(诸如滑石、氧化锌、炭黑、碳纤维、碳纳米管、聚乙二醇等)作为提高普通塑料对微波处理的敏感性的方式进行热塑性树脂的高度局部化的快速熔化。
在一些实施方案中,冷却单元是用于冷却和固化来自螺旋型挤出机的熔融挤出物的循环水浴。如果需要,该液体浴可以转化为试剂的化学浴和/或配备有表面改性和pH/温度/氧化还原电位控制单元,诸如液中等离子体发生器、碱性电解槽、富氢水发生器、活性氧和氮物质(ROS/RNS)发生器、超声波处理器的喇叭等。ROS/RNS的实例包括超氧化物(O2·-)、羟基(·OH)、过氧基(RO2·)和烷氧基(RO-),以及次氯酸(HOCl)、臭氧(O3)、单线态氧(1O2)和过氧化氢(H2O2),它们是非自由基。这些非自由基要么是氧化剂,要么很容易转化为自由基。含氮氧化剂包括一氧化氮(NO·)、过氧亚硝酸基(ONOO·)和二氧化氮(NO2)。这种额外的工艺不仅能够去除游离的残余化合物,而且还调节所生产的热塑性树脂的润湿性(所述热塑性树脂相对疏水),从而极性添加剂可以被捕获/沉积并更均匀地分散在固体基质内。一个实例是超声液体浴,该超声液体浴以分别用作前体、共溶剂和封端剂的无机金属盐(例如羧酸盐、卤化物、硝酸盐、硫化物等)、醇(例如乙醇)和脂肪酸/铵/聚合化合物(例如乙醇胺、六亚甲基四胺、油酸、聚乙烯醇、聚乙二醇、聚乙烯吡咯烷酮等)以0.1-1M的盐浓度配制,并通过超声波化学法在树脂表面上形成金属氧化物纳米结构层。通过添加氢氧化钠、氨、乙酸或天然碱化矿物石,可以将浴pH调整至5至8。
在另一个实施方案中,改性热塑性树脂组合物可以通过较低处理温度下的溶剂辅助固相聚合而不是熔融处理来生产,特别是对于软质和橡胶状热塑性塑料、温度敏感或剪切敏感的粘性材料、所有粉末混合物、湿糊剂、乳液,或先进加工设备(诸如水下造粒机、共振声学混合器、超声均化器、离心混合器、搅拌机、球形造粒机(marumerizer)、高剪切造粒机、桶式造粒机、双圆顶挤出机、行星辊挤出机和一些专门的双螺杆挤出机(包括分配/分散元件和螺杆型线/相互啮合设计配置的组合))可能不可用的制造设施。
将热塑性树脂放置在多孔套管中,该多孔套管安装在索氏萃取器上,并允许在惰性气体环境中用接收瓶中优选挥发性的溶剂(诸如四氯化碳、己烷、石油醚、乙醚和甲苯)的加热浴进行纯化,直到树脂颗粒膨胀并接近用溶剂饱和而没有明显的重量变化。未反应的单体、可溶性低分子量馏分和有机杂质可在洗涤过程中去除。接下来,在连续氮气流(10-30ml s-1)和23至30℃(±1℃)的温度下,将溶胀的颗粒浸泡在乙醚溶液中,以将乙烯基单体、可共聚酸酐和热自由基聚合引发剂从预先以上述三种成分的所需重量组成制备的溶液中吸收。引发剂优选表现出在60和80℃之间的在约1小时的分解半衰期下的较高的自加速分解温度。与此类性质匹配的引发剂实例包括AIBN、过氧化二月桂酰和过氧化二(十六烷基)二碳酸酯。在浸泡过程期间允许乙醚溶剂排出,直到其大部分蒸发。随后将浸渍有乙烯基单体、可共聚酸酐和热自由基聚合引发剂的颗粒加热至1小时半衰期温度并反应1至1.5小时,然后在冰浴中冷却至室温。收集改性颗粒并通过索氏萃取用乙醚进行至少8小时的纯化,以在惰性气体环境中除去未反应的组分和自聚合的副产物。
通过将改性热塑性树脂组合物与一种或多种添加剂组合以形成混合物,并使该混合物经受熔融处理,可以使用改性热塑性树脂组合物来制备功能性树脂组合物。在一个实施方案中,一种或多种添加剂可以是通常包含在母料中的添加剂。合适的添加剂包括但不限于:催化剂、颜料、光泽增强剂、抗氧化剂、光稳定剂、抗冲击改性剂、增塑剂、柔软剂、交联剂、相容剂、填料、抗静电剂、光滑剂、防结块剂、防灰雾剂、表面活性剂、阻燃剂、光学澄清剂(optical clarifier)、流变改性剂和香料以及其他加工助剂、偶联剂以及对构成塑料制品的芯材的物理性质至关重要的试剂。改性热塑性树脂组合物可以用商业喷涂、刷涂或内洗耐久防水产品或表面修整产品(诸如Nikwax、Gear Aid、Ultratech International、Shi-Etsu、Huntsman、TexchemUK、Rust-Oleum NeverWet、Cytonix、Wuxi Shunye Technology等出售的)进行表面预处理,以赋予防水/防油和防污/防尘性能。一种或多种添加剂可包括一种或多种具有抗菌、抗病毒或防污性质的化合物。抗菌、抗病毒或防污性质可通过如上所述的乙烯基单体和/或通过在功能性树脂组合物中包含一种或多种具有抗菌、抗毒或防污性质的化合物而赋予给塑料制品。
虽然可以通过在用于制备改性热塑性树脂组合物的组分的混合物中包括一种或多种添加剂而在单个步骤中制备功能性树脂组合物,但将该过程分为两个步骤避免了添加剂(诸如基于环氧烷或它们的醇、多不饱和脂肪酸、酸酯等的加合物的化合物)在高温下的自由基引起的降解,其导致功能性树脂组合物中的自氧化、变色和气味。
用于生产塑料制品的方法
图1总结了用于制备根据本公开的塑料制品的方法。在一个实施方案中,通过将改性热塑性树脂组合物100与一种或多种添加剂组合而将其转化为功能性树脂101。然后通过成形(例如通过模塑)将功能性树脂101直接转化为塑料制品。
在替代实施方案中,通过按比例增加其成分含量,将改性热塑性树脂组合物100转化成作为母料(102)的功能性树脂。然后,将功能性树脂母料102与适当的芯材树脂103(其反映将由其生产塑料制品的芯/基本塑料)组合,并熔融处理以形成塑料制品。通过利用该方法,功能性树脂母料102能够在熔融处理以形成制品之前与芯材树脂103干混。结果,可以使用较低熔化温度的芯材树脂(诸如聚烯烃弹性体)作为功能性树脂母料102中添加剂的本体载体,以便尽可能减少它们的化学分解和副产物形成。在一些实施方案中,芯材树脂103∶功能性树脂母料102的比率为约80至95份∶5至20份。
在另一实施方案中,改性热塑性树脂组合物100与母料104和芯材树脂103组合,并使用熔融处理直接转化成塑料制品。在一些实施方案中,芯材树脂103∶母料104∶改性热塑性树脂组合物100的比率为约75至85份∶5至15份∶5份至15份。
芯材树脂可以是任何期望由其生产制品的塑料材料。在一些实施方案中,芯材树脂是上述热塑性树脂中的一种或多种。
本发明人已经发现,通过改变乙烯基单体上的表面能、接枝长度、空间大小和侧基电荷,以及树脂改性剂组合物的硬度和将构成塑料制品的芯材中存在的树脂改性剂组合物的量,该制品的性能可以被精细地调节,以区别地控制微生物、病毒的杀灭和/或驱除以及来自周围介质的残余生物材料(诸如血渍、孢子、花粉、蛋白质、酶、核酸、胞外聚合物质、代谢产物和致病剂(例如内毒素和真菌毒素)的积聚。已经发现,杀灭和/或驱除效果不仅发生在制品的平坦和光滑的表面上,而且也发生在制品的无光泽、弯曲、微孔和泡沫表面上。此外,杀灭和/或驱除效果在很大程度上不受环境压力(诸如伽马射线/紫外线照射和反复的高压灭菌和清洗循环)的影响,从而使制品不仅适合于一次性使用,而且适合于可重复使用的包装、医疗器械和塑料实验室器皿应用。这些制品还是生物相容性的,并且与食品接触是安全的。有利地,该制品不需要表面涂层,并且因此不易于分层。
制品的性能是可调的,因为制品可以是如下防污、抗菌和/或抗病毒的:
·驱除微生物但不杀死它们;
·杀死微生物但不驱除它们;
·协同地杀死和驱除微生物;
·驱除病毒和生物材料;
·将传染性病毒灭活。
在可由与热塑性树脂组合物不同类型的材料制成的散装制品预成型件(bulkarticle preform)的情况下,可使用嵌件模塑、包覆成型、多重模塑、热熔层压或双组分共挤出工艺用功能性树脂组合物装饰基材的周围或目标表面,从而形成芯鞘或双层型材。
发明人发现,在需要蛋白质抗性的情况下,醇乙氧基化物或环氧烷衍生的化合物(包括乙二醇的低聚物/聚合物)可以包含在功能性树脂组合物中。制备的所得塑料制品表现出高度有效的蛋白结合抗性。
几种机制正在运作,以赋予塑料制品的蛋白结合抗性,诸如通过施加大的排除体积效应以及归因于高构象迁移率(conformational mobility)、高水合水平和低界面自由能的通过其与运输介质接触的下表面引起的熵斥力和渗透斥力。为此,一种有效的方式是通过掺入亲水添加剂并且优选超吸收性聚合物来增加塑料基材的亲水性,从而它将通过在最上表面上形成耐久和快速作用的水合层来施加隐形效应,所述最上表面表现出与血浆蛋白的有限或微弱的相互作用,并且在添加剂对基材进行共价功能化后,也表现出低的非特异性细胞摄取。上述添加剂(其应易于水合/溶胀,并且优选是水溶性且对pH和带电物质不太敏感)可以是非离子物质或带电物质。乙二醇的低聚物/聚合物(其中至少一端是羟基或甲氧基封端的,并且另一端是酸酐反应性的)是非离子亲水添加剂的优选选择。其他合适的实例包括聚乙烯醇、聚缩水甘油、聚(N-异丙基丙烯酰胺)、聚(甲基丙烯酸2-羟乙酯)、聚(N-[三(羟甲基)甲基]丙烯酰胺)、聚(2-甲基-2-噁唑啉)、聚(2-乙基-2-噁唑啉)、聚磷酸酯和衍生物。具有所需蛋白结合抗性的带电荷的亲水添加剂的合适实例是甜菜碱型两性离子,其带有具有膦酸根(PO3 -)、磺酸根(SO3 -)和羧酸根(COO–)和末端氨基酸(–OOC-C-NH3 +)的磷酸胆碱、磺基甜菜碱、磷酸甜菜碱和羧基甜菜碱中的一个或多个侧基(其在α-碳原子上同时具有带正电荷的氨基和带负电荷的羧基);或混合电荷的两性离子,其在不同的单体单元中含有平衡的带正电荷部分和带负电荷部分,或键合至同一载体或固体载体(诸如作为固有的双电荷填料的锂皂石粘土和在边缘上带正电荷并且表面上带负电荷的盘状颗粒),或通过包含聚阴离子和聚阳离子的带相反电荷的聚电解质的静电组装层。聚阴离子的非限制性实例包括聚丙烯酸盐(或卡波姆)、聚苯乙烯磺酸盐、聚(乙烯氧基-4-丁酸)、聚(偏磷酸)、透明质酸、聚谷氨酸盐、聚天冬氨酸盐、聚藻朊酸盐、酪朊酸盐、黄原胶、阿拉伯胶、羧甲基魔芋葡甘露聚糖、k-角叉菜胶、果胶、羧甲纤维素、葡聚糖硫酸盐、软骨素硫酸盐、角蛋白硫酸盐、岩藻多糖和L/S/FS系列(Evonik Industries)。聚阳离子的非限制性实例包括聚乙烯亚胺、聚(烯丙胺盐酸盐)、聚乙烯吡啶、聚赖氨酸、聚精氨酸、壳聚糖、明胶、聚乙烯胺、聚(叔胺)和/>E/RL/RS系列(Evonik Industries)。带电荷化合物通常比非离子化合物热稳定性差。对于更长的处理时间和超过100℃的处理温度,非离子化合物是优选的。
本发明人还发现,调整添加剂的亲水-亲油平衡(HLB)或1-辛醇-水分配系数的对数(log P)可以使塑料制品对接近的细菌或病毒施加驱除或杀死/去活化或两者的作用。这可以通过掺入的添加剂的HLB或log P值来控制。
添加剂可以是两亲物,其典型地是含有由一些间隔单元以不同长度和饱和度分隔的极性头部和非极性尾部的线性分子,优选地是通过水溶液在低能疏水表面上的快速扩散而执行的超扩散/超润湿剂,例如T形三硅氧烷聚氧乙烯醚,更优选双子表面活性剂,其是磷脂双层细胞膜成分的仿生物,诸如Gemsurf Alpha 142,其是由Chukyo-Yushi提供的商业产品。具有类似双子结构的其他商业品牌包括Evonik Industries的和/>添加剂的HLB值越高(或更负的log P值),掺入后塑料制品的亲水性和蛋白结合抗性越大。HLB值高于7(或log P值低于4)的添加剂,并且优选渗透促进剂,诸如脂肪酸单甘油酯、脂肪酸烷基酯、二取代酰胺、N-烷基取代的内酰胺、甘油/脱水山梨糖醇酯、二醇酯和糖酯(其碳链长度在约10-18个碳的范围内),可以在接触时与蛋白质或细胞相互作用。商业级渗透促进剂的实例包括MontaneTM、/>AtmerTM、/>和/>
附着到改性热塑性树脂组合物的聚合物上的添加剂能够渗透到细菌的细胞膜或藻类/真菌的细胞壁中,因此由于通过添加超过阈值浓度的添加剂引起的机械应力和弯曲以及随后破坏细胞膜/壁的渗透性而导致微生物死亡。在HLB值介于10和16之间的情况下,添加剂可以同时起到防污剂和杀生物剂的作用,从而协同发挥杀灭/去活化和驱除作用。在接近20的较高HLB值的情况下,塑料制品变成完全驱除性的,并且表现得类似于亲水添加剂。常见种类的非离子表面活性剂包括但不限于醇乙氧基化物、烷基酚乙氧基化物、烷基芳基烷氧基化物、烷基胺乙氧基化物、乙氧基化脂肪酸烷醇酰胺、乙氧基化脂肪胺、烷基烷氧基化磷酸酯、芳基烷氧基化磷酸酯、环氧乙烷(EO)-环氧丙烷(PO)嵌段共聚物、泊洛沙姆(Pluronics)、EO/PO烷氧基化物、脂肪醇乙氧基化物、脂肪酸乙氧基化物、乙氧基化甘油三酯、脱水山梨糖醇/甘油酯乙氧基化物、烷基葡糖苷、聚二甲基硅氧烷共聚多元醇、聚醚改性聚硅氧烷、醚连接的含氟表面活性剂、或其组合。两性表面活性剂的实例包括但不限于烷基胺氧化物、烷基甜菜碱和烷基酰胺丙基甜菜碱。两亲添加剂优选是非离子或无盐的两性表面活性剂,而不是正电荷或负电荷的离子洗涤剂诸如十二烷基硫酸钠、十二烷基苯磺酸钠、胆酸钠、脱氧胆酸钠、苯扎氯铵、烷基醚硫酸盐、烷基硫酸盐、烷基苯磺酸盐、α烯烃磺酸盐、磷酸酯、全氟化羧酸、烷基胺、烷基咪唑啉、烷氧基化胺以及其他基于季铵和氨基酸的化合物。蛋白质与表面活性剂分子相互作用的性质是静电的和疏水的。当离子洗涤剂用作添加剂时,分子的极性头部如果悬空,则可以静电结合到蛋白质上带相反电荷的残余上。因此,非离子和两性表面活性剂比离子洗涤剂更温和,更不易发生蛋白质变性,离子洗涤剂有时不期望用于作为蛋白质储存容器的某些应用。商业级别的非离子表面活性剂主要是乙氧基化化合物,诸如TritonTM-X、 MontanoxTM、DynolTM、/>Chemguard、/>和/>少数非烷氧基化(无EO/PO)实例来自ArlacelTM、/>和SimulsolTM系列。具有低毒性水平和高生物可再生碳指数的表面活性剂是优选的。具有超过4个EO单元(亲水含量)和小于3的log P值的乙氧基化表面活性剂通常不太利于生物累积。
上文第[00157]至[00161]段中所述的任何一种或多种化合物可根据需要作为母料或功能性树脂中的添加剂。
在另一个实施方案中,可以包括抗生物膜、抗病毒剂、群体感应、作为添加剂,以提供塑料制品的二级保护,防止在其表面处的微生物生长和/或病毒活性。此类试剂主要来源于生物质、天然衍生的或生物合成的化合物,包括单硝酸异山梨酯、S-亚硝基硫醇(其是一氧化氮供体并可诱导生物膜分散)、伊佛霉素、核苷类似物、木醋酸、一些植物化学提取物(诸如肉桂醛、大蒜素、iberin、大蒜烯、芳樟醇、香茅醇、香叶醇、丁香酚、姜黄素、香豆素、百里酚、香芹酚、白藜芦醇、表没食子儿茶素没食子酸酯、槲皮素、咖啡因、薄荷醇、香草醛酸、绿原酸、水杨酸、flavagline、鞣花单宁),和一些生物表面活性剂(诸如脂肽、鼠李糖脂、槐糖脂和微生物/藻类胞外多糖)。在另一个实施方案中,可以包括抗生物膜、抗病毒剂、群体感应、c-二-GMP/c-二-AMP或质子泵抑制剂作为添加剂,以提供塑料制品的二级保护,防止在其表面处的微生物生长和/或病毒活性。此类试剂主要来源于生物质、天然衍生的或生物合成的化合物,包括单硝酸异山梨酯、S-亚硝基硫醇(其是一氧化氮供体并可诱导生物膜分散)、伊佛霉素、核苷类似物、木醋酸、一些植物化学提取物(诸如肉桂醛、大蒜素、iberin、大蒜烯、芳樟醇、香茅醇、香叶醇、丁香酚、姜黄素、香豆素、百里酚、香芹酚、白藜芦醇、表没食子儿茶素没食子酸酯、槲皮素、咖啡因、薄荷醇、香草醛酸、绿原酸、水杨酸、flavagline、鞣花单宁、苯并咪唑衍生物、糖基化三萜皂苷),和一些生物表面活性剂(诸如脂肽、鼠李糖脂、槐糖脂和微生物/藻类胞外多糖)。
在一些实施方案中,催化剂与添加剂一起包含在母料或功能性树脂组合物中,以对改性热塑性树脂组合物进行后改性。催化剂可以是碱,实例有诸如三乙胺、咪唑、1,4-二氮杂双环[2.2.2]辛烷、1,8-二氮杂双环(5.4.0)十一碳-7-烯、1,5,7-三氮杂双环[4.4.0]癸-5-烯和N-杂环卡宾化合物;或酸,实例有诸如硬脂酸、磷酸二苯酯、甲磺酸、对甲苯磺酸、三氟甲磺酸、二月桂酸二丁基锡、2-乙基己酸锡(II)、乙酸锌(II)和丁醇钛(IV)。加热时在熔体中分解的脲用作氨源,用于在改性热塑性树脂组合物中的聚合物的酮或醛部分上形成亚胺,或酸酐或羧酸部分的酰胺化。甲硅烷基化试剂,诸如六甲基二硅氮烷(HMDS)、1,3-双(三甲基甲硅烷基)脲(BSU)和三甲基硅基氯化物(TMSCl),用作助剂,以将聚合物的一部分醇和羧酸部分封端和疏水化,并使它们对催化剂活性的竞争影响最小化。可以包括扩链剂以提高聚合物对添加剂的特定种类官能团的化学选择性,所述扩链剂有诸如二醇、二胺,并且更优选杂双官能物质,诸如乙醇胺、异山梨醇单(碳酸甲酯)、对马来酰亚胺基苯基异氰酸酯、3-氨基丙基三乙氧基硅烷和聚乙二醇单甲基丙烯酸酯,其带有醇、胺、卤化物、酰基卤化物、硫醇、硫辛酸、羧酸、碳酸酯、醛、环氧树脂、异氰酸酯、丙烯酸酯、琥珀酰亚胺酯、马来酰亚胺、噁唑啉、碳二亚胺、硅烷和二肽中任一的两个不同端基。扩链剂的柔性程度可以通过间隔单元的长度和脂族/芳香族结构来控制。相容剂(其优选为缩合物塑料(condensationplastics))可掺入所述组合物中,以改善芯材树脂与包含亲水和疏水成分的改性热塑性树脂组合物的混溶性,并可产生增韧效果。合适的实例包括聚酰胺、聚酯、聚碳酸酯、聚氨酯、聚(氨基酸)、聚(酯酰胺)、聚(酰胺胺)、聚(醚-嵌段-酰胺)、聚氨酯脲、聚酰亚胺、聚异氰脲酸酯、聚碳二亚胺、硅酮树脂、酚醛树脂、脲醛树脂、环氧树脂,更优选生物塑料或生物可降解聚合物,诸如聚己二酸对苯二甲酸丁二酯、聚琥珀酸丁二醇酯、聚乳酸、聚(乳酸-共-乙醇酸)、聚己内酯、聚赖氨酸、聚羟基链烷酸酯,最典型地聚羟基丁酸酯和聚(3-羟基丁酸酯-共-3-羟基戊酸酯),以及归功于它们的生物相容性的一些其他碳水化合物和蛋白质衍生的热塑性塑料。
实施例
以下通过参考以下非限制性实施例进一步描述本公开。
实施例1–生产改性热塑性树脂组合物(100)
将在使用前研磨成粉末的马来酸酐(MA)和过氧化二异丙苯(DCP)在苯乙烯中搅拌,直到固体部分地溶解。随后将所得的液体分散体添加到烯烃热塑性树脂的颗粒上,并将所得混合物在环境温度下在转筒中摇动,直到液体悬浮液均匀地分散在颗粒上。然后在同向旋转双螺杆挤出机中熔融配混树脂混合物。温度分布设定在160℃至180℃之间,这是烯烃热塑性树脂的常见处理窗口。将从模具挤出的长丝拉伸并在水中冷却后从熔体固化,然后切割成丸粒,以得到改性热塑性树脂组合物(100)。
实施例2–将改性热塑性树脂组合物(100)转化成功能性树脂(101)
将改性热塑性树脂组合物(100)与包含B 225和醇乙氧基化物(AEO-n)即RO(CH2CH2O)nH(R=C12-14烷基且n=3-23,跨越7和18之间的HLB值的全范围)的其他添加剂的液体混合物在与上述实施例1相同的温度分布下,在第二遍挤出中熔融配混以提供丸粒形式的功能性树脂(101)。
实施例3-基于功能性树脂(101)、或改性热塑性树脂组合物(100)、母料(104)和芯材树脂(103)的混合物的塑料制品的注射模塑
在与上述实施例1相同的温度分布下通过挤出生产携带所需添加剂的母料(104)。将功能性树脂(101)或通过干式共混或熔融共混制备的改性热塑性树脂组合物(100)、母料(104)和芯材树脂(103)的混合物送入注射模塑机,它们可以从模腔成形为各种类型的塑料制品。
在下表1中给出了塑料制品的详情:
表1
表1中的缩写如下:
AEO-5–醇乙氧基化物(AEO-n),即RO(CH2CH2O)nH,其中R=C12-14烷基,n=5,报告的HLB值为10-11,并且羟基值为130-140mg KOH/g(供应商:Shandong Usolf)
DCP–过氧化二异丙苯
HMDS–六甲基二硅氮烷
MA–马来酸酐
PPH–聚丙烯均聚物(SKYLUXTM H530,DragonChem)
PPR-a–聚丙烯无规共聚物(Clyrell RC5056,LyondellBasell)
PPR-b–聚丙烯无规共聚物(Moplen RP6068,HMC Polymers)
PPO–基于丙烯的烯烃弹性体(VistamaxxTM 6202,ExxonMobil)
SA–硬脂酸
关于表1中的脚注4-6的描述参见下面的表3
实施例4-基于功能性树脂(101)或改性热塑性树脂组合物(100)、母料(104)和芯材树脂(103)的混合物的塑料制品的蛋白结合特性
根据实施例3通过注射模塑制备1.5mL标准离心管。将试管的低保留性能与商业基准在蛋白质损失或回收方面并将“空白”试管作为对照(即在研究中未接种蛋白质溶液)而进行比较。图2和表2中总结了分别在相对短和长的接触时间尺度内进行的实验的结果。可以清楚地作出结论:一个组合物实施例,即组合物实施例2,在表现出低蛋白结合特性方面胜过或至少类似于商业基准。
图2的实验如下进行:将牛血清白蛋白(BSA)用作测试蛋白。首先,通过将BSA(薄片)溶解在1x PBS缓冲溶液(pH 7.2-7.4)中来新鲜制备浓缩的10mg/mL BSA溶液。用移液器将200微升BSA溶液转移到5个离心管样品中,加盖并在不搅拌的情况下保持直立静置。在室温下孵育10分钟后,用移液器从每个样品中缓慢取出BSA溶液,直到没有溶液残余物的迹象。然后,用移液器将200微升浅绿色的商业二辛可宁酸(BCA)测定试剂添加到每个样品和对照品中,并适度摇动。通过与蛋白质剩余物的浓度成比例的从绿色到紫色的样品溶液的颜色变化来确定测定筛选。在商业基准的情况下,颜色变为深紫色,而在由组合物实施例2制成的离心管的情况下颜色为浅紫色。“空白”试管中的颜色保持在BCA测定试剂的初始颜色。
表2的实验如下进行:将用PBS缓冲液稀释并然后分散到总计12个样品管(每个样品1毫升,每个样品类型和储存条件3个样品)的人混合血清(BF-ho-45,BangfeiBiological,120微升)用作蛋白质测试对象。分别在4℃下储存48小时和7天的经过时间后,从样品管中收集血清溶液,然后用Bradford测定试剂盒定量,以根据在575nm和615nm之间的给定波长下测量的净吸光度与连续稀释的血清浓度的标准曲线计算从样品管回收的蛋白质的量。
表2
实施例5-基于功能性树脂(101)或改性热塑性树脂组合物(100)、母料(104)和芯材树脂(103)的混合物的塑料制品的抗菌和抗病毒性能
表3总结了基于功能性树脂(101)、或改性热塑性树脂组合物(100)、母料(104)和芯材树脂(103)的混合物的一批组合物实施例的模塑测试样品的抗菌和抗病毒性能。这些实施例清楚地显示了有希望的观察结果。特别地,组合物实施例2协同地发挥优异的杀灭/去活化和驱除作用,同时还被证明是生物相容的,并且对食物接触是安全的。
表3
1杀菌功效。参照ISO 22196:2011/JIS Z 2801:2010由认可的实验室进行测试。
2驱菌功效。参照T/GDPIA 1-2019/ASTM WK66122由认可的实验室进行测试。
3杀病毒活性。参照ISO 21702:2019由认可的实验室进行测试。
4证实了实施例2根据美国US FDA 21CFR 177.1520(d)(1)、(d)(3)(ii)&(d)(4)(ii)以及EU No10/2011在三种模拟物:3%(w/v)乙酸水溶液、10%(v/v)乙醇水溶液和经精馏的橄榄油中(所有均在70℃下、2h)的总体迁移以及重金属在3%(w/v)乙酸水溶液中在相同条件下的特定迁移方面通过了食品接触安全性测试。样品(实施例3)还通过了参照GB/T16886.11-2011的急性全身毒性测试和参照GB/T 16886.4-2003的体外溶血测试。所有测试均由认可的实验室进行。
5实施例4(组合物中不含AEO-n)能够证明对革兰氏阳性菌(金黄色葡萄球菌)和革兰氏阴性菌(大肠杆菌)的驱除选择性。
6改性热塑性树脂组合物(100)能够使缩合物塑料(诸如聚酰胺)功能化,在一定程度上具有抗菌性质。
本文对任何参考文献的引用都不应解释为承认此类参考文献可用作本发明的现有技术。进一步地,本说明书中提及的任何现有出版物(或来自现有出版物的信息)或任何已知事物均不视为或不应视为对现有出版物(或来自现有出版物的信息)或已知事物构成本说明书所涉及事业领域的公识常识的一部分的承认或许可或任何形式的建议。
本领域技术人员将理解,本文所描述的公开内容易受除具体描述的那些之外的变化和修改的影响。应当理解,本公开包括所有这种变化和修改。本公开还包括本说明书中单独或共同地提及或指出的所有步骤、特征、组合物和化合物,以及两个或更多个所述步骤、特征、组合物和化合物的任何和所有组合。
Claims (74)
1.一种热塑性树脂改性剂组合物,其包含:
(i)乙烯基单体;
(ii)可共聚酸酐;
(iii)热自由基聚合引发剂;和
(iv)热塑性树脂。
2.根据权利要求1所述的热塑性树脂改性剂组合物,其中所述乙烯基单体包含一个或多个具有抗菌、抗病毒或防污性质的部分。
3.根据权利要求2所述的热塑性树脂改性剂组合物,其中所述一个或多个具有抗菌、抗病毒或防污性质的部分是羟基、氨基或羧基。
4.根据权利要求2所述的热塑性树脂改性剂组合物,其中所述一个或多个具有抗菌、抗病毒或防污性质的部分是:天然肽、N-取代酰胺、角鲨烯、单宁、皂苷、类黄酮、生物碱、类固醇、内酯、凝集素、内酰胺、抑菌毛剂、抑卷毛剂、烷基糖苷、氨基糖苷、含糖聚合物、糖脂类、糖酯、季铵化合物、萜烯、萜类化合物、脂肪酸、脂肪酸酯、烷基胺、烷基胺氧化物、醇烷氧基化物、硝基氧、卤胺、二芳基醚、氧杂蒽酮、醌、香豆素、聚乙炔、胍、卤素、磷酸基衍生物、磺酸基衍生物、酚衍生物、苯甲酸衍生物、有机金属、吡啶鎓衍生物、哌嗪衍生物、吡咯烷酮衍生物、苯胺衍生物、双胍和相关化合物、肟和相关化合物、异噻唑啉酮和相关化合物、吲哚衍生物、杂唑衍生物、杂吡咯啉衍生物、酰肼-腙衍生物、吡喃和相关化合物、呋喃和相关化合物、大环内酯、四环素、噁唑烷酮、喹诺酮、氨肟、酰胺胺和聚丙烯亚胺。
5.根据权利要求1所述的热塑性树脂改性剂组合物,其中所述乙烯基单体是短链烯烃、苯乙烯、丙烯酸烷基酯、烷基丙烯酸酯、乙酸乙烯酯、乙烯醇、乙烯基苯酚、乙烯基烷基醚、乙烯基卤化物、乙烯基乙酸、丙烯腈、丙烯酰胺、乙烯基硅烷、不饱和脂肪酸或不饱和脂肪酸酯。
6.根据权利要求1所述的热塑性树脂改性剂组合物,其中所述乙烯基单体是苯乙烯、α-甲基苯乙烯、乙烯基萘、异丁烯、乙烯基降冰片烯、丁基乙烯基醚或2-氯乙基乙烯基醚。
7.根据权利要求1至6中任一项所述的热塑性树脂改性剂组合物,其包含多个乙烯基单体。
8.根据权利要求7所述的热塑性树脂改性剂组合物,其中所述多个乙烯基单体选自:乙酸乙烯酯、丙烯酰胺、N-异丙基丙烯酰胺、N-乙烯基吡咯烷酮、N-羟甲基丙烯酰胺、丙烯酰胺基乙醇酸、丙烯腈、甲基丙烯酸、甲基丙烯酸甲酯、甲基丙烯酸2-羟乙酯、甲基丙烯酸2-氨基乙酯、甲基丙烯酸2-(二甲基氨基)乙酯、3-甲基丙烯酰氧基丙基三甲氧基硅烷、丙烯酸2-羧乙酯、甲基丙烯酸2-氮杂环庚烷乙酯、甲基丙烯酸缩水甘油酯、2-乙烯基吡啶、4-叔丁氧基苯乙烯和4-乙烯基邻苯二酚缩丙酮。
9.根据权利要求1至8中任一项所述的热塑性树脂改性剂组合物,其中所述可共聚酸酐是有机酸酐。
10.根据权利要求9所述的热塑性树脂改性剂组合物,其中所述有机酸酐是马来酸酐。
11.根据权利要求1至10中任一项所述的热塑性树脂改性剂组合物,其中所述热自由基聚合引发剂是过氧化物或偶氮化合物。
12.根据权利要求11所述的热塑性树脂改性剂组合物,其中所述自由基聚合引发剂是过氧化苯甲酰和过氧化二异丙苯的混合物。
13.根据权利要求12所述的热塑性树脂改性剂组合物,其中所述过氧化苯甲酰和所述过氧化二异丙苯以约20∶80和约80∶20之间的摩尔比存在。
14.根据权利要求1至13中任一项所述的热塑性树脂改性剂组合物,其中所述热塑性树脂是中至高流动均聚烯烃、多嵌段共聚物、无规共聚物或其混合物。
15.根据权利要求1至13中任一项所述的热塑性树脂改性剂组合物,其中所述热塑性树脂是加成聚合物、聚烯烃弹性体、热塑性烯烃或橡胶。
16.根据权利要求1至13中任一项所述的热塑性树脂改性剂组合物,其中所述热塑性树脂是PE、PP、PB、COC、PMP、PVB、PAN、NBR、EPR、PI、SEBS、SEPS、SBS、SIS、MBS、ABS、EBA、EVA、EVOH、EAA、EMA、EPDM、ETFE、ECTFE、EVCL、聚(乙烯-共-1-辛烯)、聚(乙烯-共-1-己烯)、氯丁橡胶、烯烃复分解产物或其任何组合。
17.根据权利要求1至16中任一项所述的热塑性树脂改性剂组合物,进一步包含有机溶剂。
18.根据权利要求1至17中任一项所述的热塑性树脂改性剂组合物,进一步包含除臭剂。
19.一种制备改性热塑性树脂组合物的方法,所述方法包括:将
(i)乙烯基单体;
(ii)可共聚酸酐;
(iii)热自由基聚合引发剂;和
(iv)热塑性树脂
组合以提供混合物,
并使所述混合物经受熔融处理或溶剂辅助固相聚合。
20.根据权利要求19所述的方法,其中所述乙烯基单体以在约0.5%(w/w)和约4%(w/w)之间的量存在于所述混合物中。
21.根据权利要求19或权利要求20所述的方法,其中所述可共聚酸酐以在约0.5%(w/w)和约4%(w/w)之间的量存在于所述混合物中。
22.根据权利要求19至21中任一项所述的方法,其中所述热塑性树脂以在约90%(w/w)和约98%(w/w)之间的量存在于所述混合物中。
23.根据权利要求19至22中任一项所述的方法,其中熔融处理包括挤出、模塑、吹膜、纺丝、拉伸、挤压、捏合、辊轧或热成型。
24.根据权利要求23所述的方法,其中熔融处理包括挤出。
25.根据权利要求19至24中任一项所述的方法,其中使所述改性热塑性树脂组合物经受表面处理。
26.根据权利要求25所述的方法,其中所述表面处理是将防污、防油和/或防水性质赋予给所述改性热塑性树脂组合物的处理。
27.一种每当通过权利要求19至26中任一项所述的方法制备的改性热塑性树脂组合物。
28.一种制备功能性树脂组合物的方法,包括将权利要求27所述的改性热塑性树脂组合物与一种或多种添加剂组合以形成混合物,并使所述混合物经受熔融处理。
29.根据权利要求28所述的方法,其中所述一种或多种添加剂包括一种或多种具有抗菌、抗病毒或防污性质的化合物。
30.根据权利要求29所述的方法,其中所述一种或多种具有抗菌、抗病毒或防污性质的化合物是亲水化合物。
31.根据权利要求29所述的方法,其中所述一种或多种具有抗菌、抗病毒或防污性质的化合物是两亲化合物。
32.根据权利要求31所述的方法,其中所述两亲化合物具有大于约7的HLB值。
33.根据权利要求31所述的方法,其中所述两亲化合物具有在约7和约20之间的HLB值。
34.根据权利要求28至33中任一项所述的方法,其中所述一种或多种添加剂包括芯材树脂。
35.根据权利要求28至34中任一项所述的方法,其中所述一种或多种添加剂包括抗氧化剂。
36.根据权利要求28至35中任一项所述的方法,其中熔融处理包括挤出、模塑、吹膜、纺丝、拉伸、挤压、捏合、辊轧或热成型。
37.根据权利要求36所述的方法,其中熔融处理包括挤出。
38.一种每当通过权利要求28至37中任一项所述的方法制备的功能性树脂组合物。
39.一种用于生产塑料制品的方法,包括使权利要求38所述的功能性树脂组合物成形。
40.根据权利要求39所述的方法,其中成形通过模塑实现。
41.根据权利要求40所述的方法,其中所述模塑是注射模塑、旋转模塑、吹塑或压缩模塑。
42.一种制备塑料制品的方法,包括:
(i)将
(a)改性热塑性树脂组合物;
(b)芯材树脂;和
(c)选自醇乙氧基化物、环氧烷和聚乙二醇的化合物
组合以形成混合物;
(ii)使所述混合物经受熔融处理或溶剂辅助固相聚合,以提供功能性树脂组合物;和
(iii)使所述功能性树脂组合物成形以提供所述塑料制品,
并且其中所述改性热塑性树脂组合物通过混合
(d)乙烯基单体;
(e)可共聚酸酐;
(f)热自由基聚合引发剂;和
(g)热塑性树脂,以形成混合物,和
(iv)使所述混合物经受熔融处理而制备。
43.根据权利要求42所述的方法,其中所述芯材树脂是聚丙烯。
44.根据权利要求43所述的方法,其中所述聚丙烯是聚丙烯无规共聚物。
45.根据权利要求42至44中任一项所述的方法,其中在(c)中,所述化合物是醇乙氧基化物。
46.根据权利要求45所述的方法,其中所述醇乙氧基化物具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=3至23。
47.根据权利要求46所述的方法,其中所述醇乙氧基化物具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=3至9。
48.根据权利要求45至47中任一项所述的方法,其中所述醇乙氧基化物具有在约10和11之间的HLB 10值。
49.根据权利要求42至48中任一项所述的方法,其中步骤(ii)和(iv)中的熔融处理包括挤出。
50.根据权利要求42至49中任一项所述的方法,其中步骤(i)中的所述混合物进一步包含抗氧化剂。
51.根据权利要求42至50中任一项所述的方法,其中所述乙烯基单体是苯乙烯。
52.根据权利要求42至51中任一项所述的方法,其中步骤(iii)中的成形通过模塑进行。
53.根据权利要求52所述的方法,其中所述模塑是注射模塑。
54.根据权利要求42至53中任一项所述的方法,其中所述塑料制品是抗蛋白塑料制品。
55.一种生产塑料制品的方法,包括将权利要求27所述的改性热塑性树脂组合物与一种或多种添加剂组合以形成母料,将所述母料与芯材树脂组合以形成混合物,并处理所述混合物以形成所述塑料制品。
56.一种生产塑料制品的方法,包括将权利要求27所述的改性热塑性树脂组合物与母料和芯材树脂组合以形成混合物,并处理所述混合物以形成所述塑料制品。
57.根据权利要求55或56所述的方法,其中所述母料包含一种或多种具有抗菌、抗病毒或防污性质的化合物。
58.根据权利要求57所述的方法,其中所述一种或多种具有抗菌、抗病毒或防污性质的化合物是亲水化合物。
59.根据权利要求58所述的方法,其中所述一种或多种具有抗菌、抗病毒或防污性质的化合物是两亲化合物。
60.根据权利要求59所述的方法,其中所述两亲化合物具有大于约7的HLB值。
61.根据权利要求60所述的方法,其中所述两亲化合物具有在约7和约20之间的HLB值。
62.一种制备塑料制品的方法,包括:
(i)将
(a)改性热塑性树脂组合物;
(b)芯材树脂;和
(c)包含醇乙氧基化物、环氧烷或聚乙二醇的母料
组合以形成混合物;和
(ii)使所述混合物成形以提供所述塑料制品,
其中所述改性热塑性树脂组合物通过混合
(d)乙烯基单体;
(e)可共聚酸酐;
(f)热自由基聚合引发剂;和
(g)热塑性树脂,以形成混合物,和
(iii)使(d)、(e)、(f)和(g)的所述混合物经受熔融处理或溶剂辅助固相聚合而制备。
63.根据权利要求62所述的方法,其中所述芯材树脂是聚丙烯。
64.根据权利要求63所述的方法,其中所述聚丙烯是聚丙烯无规共聚物。
65.根据权利要求62至64中任一项所述的方法,其中所述母料包含醇乙氧基化物。
66.根据权利要求65所述的方法,其中所述醇乙氧基化物具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=3-9。
67.根据权利要求66所述的方法,其中所述醇乙氧基化物具有以下通式:RO(CH2CH2O)nH,其中R是C12-C14烷基并且n=5。
68.根据权利要求65至67中任一项所述的方法,其中所述醇乙氧基化物具有在10和11之间的HLB值。
69.根据权利要求62至68中任一项所述的方法,其中步骤(ii)中的成形通过模塑进行。
70.根据权利要求69所述的方法,其中所述模塑是注射模塑。
71.根据权利要求62至70中任一项所述的方法,其中步骤(iii)中的熔融处理包括挤出。
72.根据权利要求62至71中任一项所述的方法,其中所述乙烯基单体是苯乙烯。
73.根据权利要求62至72中任一项所述的方法,其中(d)、(e)、(f)和(g)的所述混合物不含或基本上不含表面活性剂。
74.一种每当通过权利要求42至73中任一项所述的方法获得的塑料制品。
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