CN116135920A - 一种用于加速高分子材料的厌氧生物降解的添加剂及其制备与使用方法 - Google Patents
一种用于加速高分子材料的厌氧生物降解的添加剂及其制备与使用方法 Download PDFInfo
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Abstract
本发明提供了一种用于主体聚合物材料的厌氧性生物降解促进剂(ABA)、结合厌氧性生物降解促进剂的聚合物材料及其生产和应用方法。厌氧性生物降解促进剂包括载体基质、至少一种生物组分、保护层、生物多样性促进剂、表面活性剂、增容剂、抗氧化剂、增塑剂和性能调节剂。厌氧性生物降解促进剂显著提高了聚合物材料在厌氧环境中的生物降解速率,并且不会显著影响原始聚合物材料的机械性能和其他性能(包括当应用于食品接触安全产品时的食品接触安全性)。
Description
相关申请的交叉引用
本申请要求2021年11月18日提交的美国临时专利申请号63/280,625的优先权,及要求2022年11月16日提交的美国专利申请号17/987,879的优先权,其公开内容以引用的方式并入本文中。
技术领域
本发明涉及一种适用于在各种条件下的生物降解促进剂,特别是在厌氧条件下,可以在存有生物材料的情况下加速主体聚合物材料的生物降解。本发明还涉及厌氧性生物降解促进剂的制备方法及其使用方法。
背景技术
降低塑料的使用是减少塑料废物的一种方法,但目前针对塑料废物的问题,最妥善的解决方法之一似乎仍然是通过有效的塑料降解来减少塑料废物,为了实现这一目的,最常见的塑料降解方法之一是于聚合物材料中添加氧化降解添加剂。然而,越来越多的国家或地区,如法国、西班牙和新西兰,开始质疑氧化降解添加剂的生物可降解性,且其产生的微碎片/微塑料可能对环境更加有害,并将禁止使用氧化降解添加剂。因此,最近有一些研究侧重于寻找可提高传统塑料生物降解性的可能替代品。
美国专利申请公开号US2013/0109781A1公开了一种化学添加剂,它使用呋喃酮化合物作为化学引诱剂,并且指出透过混合该添加剂材料与聚合物材料,可产生至少部分可生物降解的产品。然而,其中没有提供关于这些化学引诱剂如何与微生物在极端环境中(例如,在低温或基本无氧和高温环境中)相互作用以促进生物降解的记载,也没有提供如何通过改性普通塑料来缩短生物降解时间或提高生物降解效率;此外,也指出透过群体感应(quorum sensing)的应用,可以将细菌吸引到聚合物上,以提高聚合物的生物降解性,但此方法并不会改变处理地点的种群动态,相反地,为了试图改变种群动态,必须在化学添加剂中加入额外的微生物,然而,添加的微生物可能与原生微生物不兼容,而在短时间内消失。
此外,现有技术也未充分考虑最终产品的食品接触安全方面和其他实际用途。因此,本领域仍需要一种配方/方法来加速聚合物材料(包括传统塑料和普通可生物降解塑料)的生物降解,且考虑到长期的生物降解,在配方中進一步加入生物多样性促进剂,以改变原生微生物种群,从而促进生物降解。
发明内容
因此,在第一方面,本发明提供了一种用于主体聚合物材料的厌氧性生物降解促进剂(anaerobic biodegradation accelerator,ABA),其中该厌氧性生物降解促进剂包括:
载体基质,用于在促进剂中聚集所有其他成分,并协助将其分散到该主体聚合物材料中;
至少一种生物组分,用于启动主体聚合物材料的生物降解;
保护层,用于保护该生物组分,并延长该厌氧性生物降解促进剂的保质期;
生物多样性促进剂,用于促进和稳定该至少一种生物组分的生长;
表面活性剂,用于促进该至少一种生物组分与该主体聚合物材料的相互作用;
增容剂,用于增加该促进剂与该主体聚合物材料之间的兼容性;
抗氧化剂,用于抑制该促进剂在制造、保存和使用过程中的氧化反应;
增塑剂,以及;
性能调节剂。
在一个实施例中,载体基质包括但不限于可生物降解和/或非生物降解材料,其选自聚乙烯(PE)、聚丙烯(PP)、聚醋酸乙烯酯(EVA)、聚苯乙烯(PS)、聚甲醛(POM)、聚对苯二甲酸乙二醇酯(PETG)、聚酰胺(PA)、聚碳酸酯(PC)、聚氨酯(PU)、热塑性弹性体(TPE)、醋酸纤维素(CA)、聚氯乙烯(PVC)、丙烯腈-丁二烯-苯乙烯(ABS)、聚乙烯醇(PVA)、聚乳酸(PLA)、多羟基脂肪酸酯(PHA)、聚丁二酸丁二醇酯(PBS)、聚己内酯(PCL)、聚己二酸丁二酯(PBAT)、聚乙醇酸(PGA)和聚乳酸-羟基乙酸(PLGA),或其任何组合。
载体基质可占厌氧性生物降解促进剂总重量的30%至90%。
在一个实施例中,该至少一种生物组分是选自细菌、真菌和酶中的一个或多个,或其任意组合,其在好氧和厌氧条件下具有生物活性和/或酶活性。
该细菌可包括但不限于:热梭菌、黄体微球菌、红球菌、栗褐链霉菌、不动杆菌属、产碱菌属、拟无枝酸菌属、节杆菌属、芽孢杆菌属、柠檬酸杆菌属、棒状杆菌属、肠杆菌属、微小杆菌属、赖氨酸芽孢杆菌属、巨型芽孢杆菌、枯草杆菌、微杆菌属、微球菌属、诺卡氏菌属、巴氏杆菌属、假单胞菌属、红球菌属、施莱格尔菌(Schlegelella)属、鞘氨醇杆菌属和葡萄球菌属。
该真菌包括但不限于:酵母、黑曲霉、阿克霉属、曲霉属、金担子菌属、枝孢菌属、镰刀菌属、黏帚菌属、毛霉属、青霉属、拟盘多毛孢属、原毛平革菌属、链霉菌属、栓菌属和木霉菌属。
该酶包括但不限于:α-淀粉酶、过氧化氢酶、纤维素酶、角质酶、解聚酶、酯酶、葡萄糖苷酶、水解酶、漆酶、脂肪酶、锰过氧化物酶、脲酶和蛋白酶,如木瓜蛋白酶、菠萝蛋白酶。
该生物组分的占比约为厌氧性生物降解促进剂总重量的大于0%至20%。
在一个实施例中,该保护层包括阿拉伯胶、海藻酸钠、明胶、壳聚糖、纤维素、聚乙烯醇、聚(乳酸-羟基乙酸)、聚乙二醇或其任何组合的一种或多种保护层材料,并进一步包括表面活性剂。
该一种或多种保护层材料的占比约为厌氧性生物降解促进剂总重量的大于0%至30%。
在一个实施方案中,该生物多样性促进剂包括但不限于:醣类化合物、含氮化合物、磷化合物或其任何衍生物以及微量营养素;其中该醣类化合物包括环糊精、纤维素、淀粉、蔗糖和葡萄糖;该含氮化合物包括蛋白质、肉类提取物、自溶物、硝酸盐和尿素;该磷化合物包括五氧化二磷、磷酸氢、磷酸二氢根和有机磷酸盐;该衍生物包括果胶、木聚糖、羧酸、氨基酸;该微量营养素包括维生素、矿物质、钾、钙、镁、铁、锰、锌、硼、铜和钼;或其任意组合。
该生物多样性促进剂的占比约为厌氧性生物降解促进剂总重量的大于0%至20%。
在各种实施例中,该表面活性剂是一种或多种非离子或离子表面活性剂,其中非离子表面活性剂包括聚山梨酸酯、山梨醇酯和烷基酚乙氧基化物;离子表面活性剂包括阳离子表面活性剂、阴离子表面活性剂,两性离子表面活性剂和生物表面活性剂。其中,阴离子表面活性剂包括含有阴离子官能团的化合物,包括硫酸盐、磺酸盐、磷酸盐、羧酸衍生物、烷基硫酸盐、琥珀酸磺酸二辛酯钠、全氟辛烷磺酸、全氟丁烷磺酸、烷基芳醚磷酸盐、烷基醚磷酸盐、烷基醚磷酸酯十二烷基苯磺酸钠、十二烷基硫酸纳、硬脂酸钠、硬脂酸钙,其中,该烷基硫酸盐包括十二烷基硫酸铵,十二烷基硫酸钠和相关的烷基醚硫酸盐月桂酸钠和聚醚硫酸钠;该阳离子表面活性剂包括盐酸辛烯胺、溴化十六烷基铵、氯化十六烷基吡啶、氯化苯扎氯铵、氯化苯乙氧铵、氯化二甲基十八烷基铵和二十八烷基二甲基铵;两性离子表面活性剂包括十二烷基二甲胺氧化物和肉豆蔻胺氧化物;生物表面活性剂包括糖脂、磷脂、脂肽、中性脂质、脂肪酸和脂多糖;或其任意组合。
不同实施例中的表面活性剂的占比约为厌氧性生物降解促进剂总重量的大于0%到10%。
在一个实施例中,增容剂包括但不限于扩链剂和偶联剂,其中扩链剂包括改性苯乙烯-丙烯酸聚合物、乳酸、乙二醇和1,4-丁二醇;偶联剂包括马来酸酐、桐油酸酐、环氧化大豆油、亚甲基二苯基二异氰酸酯、丙烯酸和柠檬酸;或其任意组合。
该增容剂的占比约为厌氧性生物降解促进剂总重量的大于0%至10%。
在一个实施例中,增塑剂包括但不限于:水、尿素、甘油、乙二醇、聚乙二醇、桐油酸酐、环氧大豆油、柠檬酸三乙酯和柠檬酸乙酰三乙酯或其任意组合。
该增塑剂的占比约为厌氧性生物降解促进剂总重量的大于0%至10%。
在一个实施例中,性能调节剂包括但不限于碳酸钙、二氧化钛、滑石粉、有机蒙脱土、膨润土、纳米填料、天然纤维、色母粒、气味母粒或其任意组合。
该性能调节剂的占比可以大于厌氧性生物降解促进剂总重量的大于0%至10%。
在一个实施例中,该抗氧化剂包括但不限于:抗坏血酸、生育酚、谷胱甘肽、四价[亚甲基(3,5-二叔丁基-4-羟基氢肉桂酸)]甲烷、三(2,4-二叔丁基苯基)亚磷酸酯、硫辛酸和尿酸,或其任意组合。
该抗氧化剂的占比约为厌氧性生物降解促进剂总重量的大于0%至10%。
一个实施例中,该主体聚合物材料包括但不限于:聚乙烯(PE)、聚丙烯(PP)、聚醋酸乙烯酯(EVA)、聚苯乙烯(PS)、聚甲醛(POM)、聚对苯二甲酸乙二醇酯(PETG)、聚酰胺(PA)、聚碳酸酯(PC)、聚氨酯(PU)、热塑性弹性体(TPE)、醋酸纤维素(CA)、聚氯乙烯(PVC)、丙烯腈-丁二烯-苯乙烯(ABS)、聚乙烯醇(PVA)、聚乳酸(PLA)、多羟基脂肪酸(PHA)、聚丁二酸丁二醇酯(PBS)、聚己内酯(PCL)、聚己二酸丁二酯(PBAT)、聚乙醇酸(PGA)和聚乳酸-羟基乙酸(PLGA)或其任意组合,其中,该主体聚合物材料是常规塑料或通过普通塑料加工技术的任何塑料,普通塑料加工技术过程包括但不限于挤出、树脂制造、发泡、片材生产、热成型、注塑、吹膜、吹塑、纤维/织物和长丝制造。
在第二方面中,本发明提供一种将第一方面的厌氧性生物降解促进剂制备为母粒的制备方法,其中该方法包括:
将保护层材料引入到至少一种生物组分,以形成围绕该至少一种生物组分的保护层;在第一高温下,将具有保护层的该至少一种生物组分和厌氧性生物降解促进剂中的其余组分和/或材料均质化,以获得混合物;以及
在第二高温下挤压该混合物,直到获得母粒。
该第一高温的温度范围为室温至80℃。
该第二高温的温度范围为50℃至250℃。
具有保护层的该至少一种生物组分以及其余组分和/或材料的均质化可在40至1000rpm的混合速度下进行。
在第三方面中,提供了一种含有厌氧性生物降解促进剂(ABA)的聚合物材料的制备方法,其中包含上述的厌氧性生物降解促进剂,且该厌氧性生物降解促进剂以母粒的形式与该聚合物材料结合,其中该方法包括:
将厌氧生物降解促进剂母粒与主体聚合物材料均质化,形成混合物;以及
在第三高温下挤压该混合物,以获得含有厌氧性生物降解促进剂的聚合物材料。
在一个实施例中,该含有厌氧性生物降解促进剂的聚合物材料中的厌氧性生物降解促进剂的重量比大约占总重量的大于0%到30%。
更优选地,该厌氧性生物降解促进剂的量约为该含有厌氧性生物降解促进剂的聚合物材料重量的1%至5%,以利于降低对原始聚合物材料的机械性能和其他性能(包括当应用于食品接触安全产品时的食品接触安全性)的影响。
该第三高温的温度范围为50℃至300℃。
厌氧性生物降解促进剂母粒与主体聚合物材料的均质化可在40至1000rpm的混合速度下进行。
本发明的该含有厌氧性生物降解促进剂的聚合物材料具有与主体聚合物材料相当的可回收性。
该含有厌氧性生物降解促进剂的聚合物材料具有优于主体聚合物材料的生物降解性。
该主体聚合物材料包括但不限于聚乙烯(PE)、聚甲醛(POM)、聚苯乙烯(PS)、膨胀聚苯乙烯(EPS)、聚丙烯(PP)或聚对苯二甲酸乙二醇酯(PET)。
附图说明
以下参考附图更详细地描述本发明的实施例,其中:
图1显示厌氧性生物降解促进剂的概念图;
图2显示厌氧性生物降解促进剂如何加速聚合物材料在厌氧环境中的生物降解;
图3显示制备厌氧性生物降解促进剂母粒的方法;
图4显示制备含有厌氧性生物降解促进剂的聚合物材料的方法,并说明其相关应用;
图5A至5C显示根据本发明的一个实施例所制备的含有厌氧性生物降解促进剂的低密度聚乙烯(LDPE):图5A显示通过挤出吹膜工艺制备的含厌氧性生物降解促进剂的低密度聚乙烯膜;图5B分别显示低密度聚乙烯薄膜卷的外观(左)和含有5wt.%厌氧性生物降解促进剂的低密度聚乙烯薄膜卷的外观(右);图5C显示以含有5wt.%厌氧性生物降解促进剂的低密度聚乙烯的薄膜卷制成的塑料袋;
图6显示根据本发明的一个实施例,由含有5wt.%ABA的不同主体聚合物所制成的不同产品的外观;
图7显示含有厌氧性生物降解促进剂的叉子的食品接触安全测试报告;
图8显示添加和无添加厌氧性生物降解促进剂的LDPE在480天观察期间的生物降解速度的差异;以及
图9显示添加和无添加厌氧性生物降解促进剂的POM在450天观察期间的生物降解速度的差异。
具体实施方式
在以下描述中,将用于制备和使用该配方、组合物和方法等列为优选实例。在不脱离本发明的范围和精神的情况下所进行的修改,包括添加和/或替换,对于本领域技术人员来说是显而易见。可省略具体细节避免模糊本发明;然而,编写本文是为了使本领域技术人员能够实践本发明的方案而无需过度实验。
如本文所用,术语“大于0%”是指任何高于0%的百分比,举例来说,包括0.0001%、0.001%、0.01%、0.1%和1%。
参考附图,图1显示本发明的厌氧性生物降解促进剂(ABA)的组成,包括载体基质、在该载体基质中的生物多样性促进剂、受保护层保护的生物组分、表面活性剂、增容剂、增塑剂、抗氧化剂和性能调节剂。
本发明中的载体基质用于聚集厌氧性生物降解促进剂中的所有其他成分,并帮助将其分散到含有厌氧性生物降解促进剂的聚合物材料中,其中载体基质包括但不限于一种或多种的生物可降解和/或非生物可降解材料,其选自聚乙烯(PE)、聚丙烯(PP)、聚乙烯(PP)和/或聚乙烯(PET)中的,聚醋酸乙烯酯(EVA)、聚苯乙烯(PS)、聚甲醛(POM)、聚对苯二甲酸乙二醇酯(PETG)、聚酰胺(PA)、聚碳酸酯(PC)、聚氨酯(PU)、热塑性弹性体(TPE)、醋酸纤维素(CA)、聚氯乙烯(PVC)、丙烯腈-丁二烯-苯乙烯(ABS)、聚乙烯醇(PVA)、聚乳酸(PLA)、聚羟基脂肪酸(PHA)、聚琥珀酸丁烯酯(PBS)、聚己内酯(PCL)、聚己二酸丁二醇酯(PBAT)、聚乙醇酸(PGA)和聚乳酸-羟基乙酸共聚物(PLGA)或其任意组合。在一些实施例中,厌氧性生物降解促进剂中的载体基质占厌氧性生物降解促进剂总重量的约30%到小于100%,较优选地,大约占厌氧性生物降解促进剂总重量的30%到90%。在一优选实施例中,载体基质由可生物降解材料组成,以增强微生物的初始生物降解性和生长,以利于后续的生物降解。
在部分实施例中,该生物组分可选自严格厌氧菌或兼性厌氧菌的细菌,例如,热梭菌(Clostridium thermocell)、黄微球菌(Micrococcus luteus)、红红球菌(Rhodoccusrhodochrous)、栗褐链霉菌(Streptomyces badius)、不动杆菌属(Acinetobacter spp.)、产碱菌属(Alcaligenes spp.)、拟无枝酸菌属(Amycolatopsisspp.)、节杆菌属(Arthrobacter spp.)、芽孢杆菌属(Bacillus spp.)、柠檬酸杆菌属(Citrobacter spp.)、棒状杆菌属(Corynebacteriumspp.)、肠杆菌属(Enterobacterspp.)、微小杆菌属(Exigobacterium spp.)、赖氨酸芽孢杆菌属(Lysinibillus spp.)、巨型芽孢杆菌(Bacillus megaterium)、枯草杆菌(Bacills subtilis)、微杆菌属(Microbacterium spp.)、微球菌属(Micrococcus spp.)、诺卡氏菌属(Nocardia spp.)、巴氏杆菌属(Paenibillus spp.)、假单胞菌属(Pseudomonas spp.)、红球菌属(Rhodococcusspp.)、施莱格尔菌属(Schlegelella spp.)、鞘氨醇杆菌(Sphingobacterium spp.)、和葡萄球菌(Staphylococcus spp.)等;真菌,例如,酵母、黑曲霉(Aspergillus niger)、阿克霉属(Acremonium spp.)、曲霉属(Aspercillus spp.)、金担子菌属(Aureobasidium spp.)、枝孢菌属(Cladosporium spp.)、镰刀菌属(Fusarium spp.)、黏帚菌属(Glioclodiumspp.)、毛霉属(Mucor spp.)、青霉属(Penicillium spp.)、拟盘多毛孢属(Pestalotiopsisspp.)、原毛平革菌属(Phanerochaete spp.)、链霉菌属(Streptomyces spp.)、栓菌属(Trametes spp.)和木霉菌属(Trichoderma spp.)等;该生物组分也可以是酶,例如,α-淀粉酶、过氧化氢酶、纤维素酶、角质酶、解聚酶、酯酶、葡萄糖苷酶、水解酶、漆酶、脂肪酶、锰过氧化物酶、蛋白酶(例如,木瓜蛋白酶、菠萝蛋白酶)、脲酶等,在部分实施方案中,厌氧性生物降解促进剂中的生物组分重量占比为厌氧性生物降解促进剂总重量的大于0%至小于70%,优选地为介于大于0%至20%的重量比。
在部分实施方案中,参见图2,表面活性剂用于促进微生物(或生物组分)与塑料(例如,疏水性塑料)的相互作用,以加速微生物附着至聚合物材料的过程与生物膜的形成,其中含有本发明的厌氧性生物降解促进剂的塑料可吸引微生物(步骤1),比不含厌氧性生物降解促进剂的原始塑料能更有效地形成生物膜(步骤2),然后加速塑料的生物降解(步骤3)。本发明的表面活性剂可包括但不限于以下材料:非离子表面活性剂,例如聚山梨酸酯(例如Tween-20、Tween-40、Tween-60、Tween-80等)、山梨醇酯(例如Span-20、Span-40、Span-60、Span-80等)、烷基酚乙氧基化物(例如Triton X-100);离子表面活性剂、阴离子表面活性剂(例如,在其顶部含有阴离子官能团的表面活性剂、硫酸盐、磺酸盐和磷酸盐、羧酸盐衍生物、烷基硫酸盐、琥珀酸磺酸二辛酯钠(dioctyl sodium sulfosuccinate)、全氟辛烷磺酸(perfluorooctanesulfonate)、全氟丁烷磺酸(perfluorobutanesulfonate)、烷基芳醚磷酸盐(alkyl-aryl ether phosphates)、烷基醚磷酸盐(alkyl-aryl etherphosphates)、烷基醚磷酸酯十二烷基苯磺酸钠(alkyl ether phosphates sodiumdodecylbenzenesulfonate)、十二烷基硫酸纳(sodium dodecyl sulfate)、硬脂酸钠(sodium stearate)、硬脂酸钙(calcium stearate)等,其中,该烷基硫酸盐包括十二烷基硫酸铵(ammonium lauryl sulfate)、十二烷基硫酸钠(sodium lauryl sulfate)和相关的烷基醚硫酸盐月桂酸钠(alkyl-ether sulfates sodium laureth sulfate)和聚醚硫酸钠(sodium myreth sulfate));阳离子表面活性剂(例如,盐酸辛烯胺(octenidinedihydrochloride)、溴化十六烷基铵(cetrimonium bromide)、氯化十六烷基吡啶(cetylpyridinium chloride)、氯化苯扎氯铵(benzalkonium chloride)、氯化苯乙氧铵(benzethonium chloride,)、氯化二甲基十八烷基铵(dimethyldioctadecylammoniumchloride)和溴化二十八烷基二甲基铵(dioctadecyldimethylammonium bromide)等);两性离子表面活性剂(例如月桂基二甲胺氧化物(lauryldimethylamine oxide)和肉豆蔻胺氧化物(myristamine oxide)等);生物表面活性剂(例如,糖脂、磷脂、脂肽、中性脂质、脂肪酸和脂多糖等)。在部分实施方案中,厌氧性生物降解促进剂中的表面活性剂含量约占厌氧性生物降解促进剂总重量的大于0%至10%。
在部分实施例中,增容剂可增加厌氧性生物降解促进剂中不相溶组分之间的相溶性,并增加促进剂与聚合物材料之间的兼容性,以达到将厌氧性生物降解促进剂高度分散于聚合物材料中的效果。本发明的增容剂可包括但不限于以下材料:扩链剂(例如改性苯乙烯-丙烯酸聚合物(modified styrene acrylic polymers)、乳酸、乙二醇、1,4-丁二醇)与偶联剂(例如马来酸酐(maleic anhydride)、桐油酸酐(Tung oil anhydride)、环氧化大豆油(epoxidized soybean oil)、亚甲基二苯基二异氰酸酯(methylene-diphenyldiisocyanate)、丙烯酸、柠檬酸等)。
在部分实施方案中,抗氧化剂可用于抑制氧化反应,以在热加工(例如挤压过程)期间保护厌氧性生物降解促进剂,并在储存和使用期间延长厌氧性生物降解促进剂的保质期。本发明的抗氧化剂可包括但不限于以下材料:抗坏血酸、生育酚、谷胱甘肽、四[亚甲基(3,5-二叔丁基-4-羟基肉桂酸酯)]甲烷(tetrakis[methylene(3,5-di-t-butyl-4-hydroxyhydrocinnamate)]methane)、三(2,4-二叔丁基苯基)亚磷酸酯(tris(2,4-di-tert-butylphenyl)phosphite)、硫辛酸、尿酸等。在部分实施例中,厌氧性生物降解促进剂中的抗氧化剂含量约占厌氧性生物降解促进剂总重量的大于0%至10%。
在部分实施例中,本发明的增塑剂可提高促进剂的可塑性,以利于制备。增塑剂可包括但不限于以下材料:水、尿素、甘油、乙二醇、聚乙二醇、桐油酸酐、环氧化大豆油、柠檬酸三乙酯、柠檬酸乙酰三乙酯等。
在部分实施方案中,本发明的性能调节剂可改善厌氧性生物降解促进剂的特定性质(例如机械性质)和/或将特定性质(如颜色和气味)引入聚合物材料,增强厌氧性生物降解性。在部分实施例中,所述性能调节剂可包括但不限于以下材料:碳酸钙、二氧化钛、滑石粉、有机蒙脱石、膨润土、纳米填料、天然纤维、色母粒、气味母粒等。
在部分实施例中,本发明的保护层可在厌氧性生物降解促进剂的制备过程中保护其生物组分,并可降低其生物组分在应用至食品接触安全产品(如餐具)时产生转移,同时增加厌氧性生物降解促进剂在储存和使用方面的保质期。在部分实施例中,保护层由一种或多种优选可生物降解的材料制成,以增强微生物的初始生物降解性和生长,用于进一步生物降解。本发明的保护层材料可包括但不限于以下材料:阿拉伯胶、海藻酸钠、明胶、壳聚糖、纤维素、聚乙烯醇、聚(乳酸-乙醇)、聚乙二醇。保护层还包含一种或多种本发明的表面活性剂。在一些实施例中,ABA中的保护层材料以ABA重量的大于0%至30%、优选约大于ABA重量%至10%的量存在。
此外,参见图3,本发明的厌氧性生物降解促进剂可以母料的形式制备。如图3中所示,先将保护层材料和生物组分透过各种技术(如喷雾干燥、挤出法、乳液、喷雾冷却、凝聚、共结晶、脂质体形成等)引入至均化器(301)中,随后将厌氧性生物降解促进剂的其他组分加入均化器中,并充分混合(302),再将其送至挤出机进行挤出(303),其中,于均化器中混合厌氧性生物降解促进剂的组分时,均化器的混合速度范围约为40至1000rpm,且均化器操作温度范围为室温至约80℃,并且充分混合的厌氧性生物降解促进剂组分在挤出机中是以50℃至约250℃的操作温度挤出,挤出后,将其进行冷却(304),再造粒(305),以形成厌氧性生物降解促进剂母料(306)。应当理解,生产方法的任何合理修改、变化和优化,或本领域技术人员已知的任何其他可用方法,也可用于生产本厌氧性生物降解促进剂母料,且生成的厌氧性生物降解促进剂母料在并入聚合物材料后,可满足所预期的聚合物材料生物降解性。
图4显示如何将根据本发明的部分实施例的厌氧性生物降解促进剂(例如根据图3所示的方法生产的厌氧性生物降解促进剂母料)结合到聚合物材料中,以生产含有厌氧性生物降解促进剂的聚合物材料。在图4中,厌氧性生物降解促进剂组分或厌氧性生物降解促进剂母料和聚合材料在混合器中均化(401),然后经过挤出机进行挤出(402),挤出后,将挤出的厌氧性生物降解促进剂/聚合物材料的共混物冷却并造粒(403),以获得含有厌氧性生物降解促进剂的聚合物材料(405),含有厌氧性生物降解促进剂的聚合物材料可以制成不同形式的产品,例如薄膜、瓶子、片材等(407),且也可以直接经过现有的一般塑料加工生产线进行挤出后的厌氧性生物降解促进剂/聚合物材料共混物的加工(404),获得不同形式的产品,例如含有厌氧性生物降解促进剂的聚合物材料的薄膜、瓶子、片材等(406)。
示例
实施例1.含有厌氧性生物降解促进剂的聚合物低密度聚乙烯(LDPE)
如图5A-5C所示,将厌氧性生物降解促进剂(重量百分比5wt.%)与低密度聚乙烯(LDPE)树脂混合,然后直接在160-190℃的操作温度下进行挤出吹膜处理。如图5A所示,在挤出吹膜过程中,相比于普通低密度聚乙烯膜,含有厌氧性生物降解促进剂(5%重量比)的低密度聚乙烯膜显示出具有相似厚度的良好延展性,此外,含有厌氧性生物降解促进剂的低密度聚乙烯薄膜也易于储存;如图5B所示,含有厌氧性生物降解促进剂的低密度聚乙烯膜与普通低密度聚乙烯膜一样,都可以卷状的形式保存,换句话说,厌氧性生物降解促进剂的加入不会影响低密度聚乙烯的基本力学性能;此外,如图5C所示,以含有厌氧性生物降解促进剂的低密度聚乙烯卷所制成的塑料袋,具有透明的外观,表示厌氧性生物降解促进剂的加入不会改变低密度聚乙烯的透明度。综合以上结果,厌氧性生物降解促进剂的加入不会影响或改变低密度聚乙烯的适用性。
实施例2.含有厌氧性生物降解促进剂的聚合物材料的产品示例
如图6所示,将含有厌氧性生物降解促进剂的不同聚合物材料加工,制备出不同应用形式的产品。简言之,将厌氧性生物降解促进剂(重量百分比5wt.%)与聚甲醛(POM)树脂混合,并于175-190℃下挤出,然后将其一起造粒,以产出含有厌氧性生物降解促进剂的聚甲醛树脂粒,供进一步使用,例如用于带扣的注射成型;将厌氧性生物降解促进剂(重量百分比5wt.%)与聚苯乙烯(PS)树脂混合,并于185-210℃下挤出,然后将其一起造粒,以产出含有厌氧性生物降解促进剂的聚苯乙烯树脂,供进一步使用,如餐具注射成型、杯盖的片材生产和热成型;将厌氧性生物降解促进剂(重量百分比5wt.%)与聚丙烯(PP)树脂混合,并于185-230℃下挤出,然后将其一起造粒,以产出含有厌氧性生物降解促进剂的聚丙烯树脂,供进一步使用,如餐具注射成型、餐盒的板材生产和热成型;将厌氧性生物降解促进剂(重量百分比5wt.%)与聚对苯二甲酸乙二醇酯(PET)树脂混合,并于250-270℃下挤出,然后将其一起造粒,以产出含有厌氧性生物降解促进剂的聚对苯二甲酸乙二醇酯树脂,供进一步使用,例如瓶子的吹塑成型。其他还有像是含有厌氧性生物降解促进剂(5wt.%)的可发性聚苯乙烯泡沫塑料杯。根据本发明的部分实施例所生产的含有厌氧性生物降解促进剂的聚合物材料与不含厌氧性生物降解促进剂的聚合材料相同,都是可回收的,且还确保了厌氧性生物降解促进剂的加入不会影响聚合物材料的适用性和可用性。
实施例3.含有厌氧性生物降解促进剂的聚合物材料的食品接触安全性试验
在部分实施例中,在含有厌氧性生物降解促进剂的聚合物材料中,所含的厌氧性生物降解促进剂约占总重量的大于0%至30%,较优选地,为占总重量的1%至5%,以最小化回收后厌氧性生物降解促进剂对机械性能的影响或使其机械性能与原聚合物材料相当,并最小化厌氧性生物降解促进剂对原聚合物材料的特性(包括食品接触安全性)的影响,例如当其应用于食品接触安全产品(如餐具、饭盒、杯子和杯盖)。因此,本发明进一步对由含有厌氧性生物降解促进剂(5wt.%)的聚苯乙烯所制成的叉子进行安全性评估,结果如图7所示,含有厌氧性生物降解促进剂(5wt.%)的聚苯乙烯叉子通过了美国FDA 21CFR175.300(树脂和聚合物涂层)-提取物量的测定,表示含有厌氧性生物降解促进剂的聚合物材料所制成的产品可以安全地用作食品接触产品。
实施例4.含有厌氧性生物降解促进剂的聚合物材料的机械性能
进一步评估了含有厌氧性生物降解促进剂的聚合物材料的机械性能。简言之,含有厌氧性生物降解促进剂(5wt.%)的低密度聚乙烯膜具有14MPa的拉伸强度,而不含有厌氧性生物降解促进剂的低密度聚乙烯膜则是具有12MPa的拉伸强度,可见两者具有类似的拉伸强度;在另一个实施例中,含有厌氧性生物降解促进剂(5wt.%)的聚甲醛树脂具有52MPa的拉伸强度,而不含有厌氧性生物降解促进剂的聚甲醛树脂则是具有56MPa的抗拉强度;在另一个实施例中,含有厌氧性生物降解促进剂(5wt.%)的聚苯乙烯树脂具有1868MPa的弯曲模数,而不含有厌氧性生物降解促进剂的聚苯乙烯树脂则是具有1635MPa的弯曲模数;在另一个实施例中,含有厌氧性生物降解促进剂(5wt.%)的聚丙烯树脂具有1940MPa的弯曲模数,而不含有厌氧性生物降解促进剂的聚苯乙烯树脂则是具有1878MPa的弯曲模数。综合以上,可得知厌氧性生物降解促进剂的加入不会影响聚合物材料的机械性能。
实施例5.含有厌氧性生物降解促进剂的聚合物材料的生物降解效果
与不含厌氧性生物降解促进剂的聚合物材料相比,含有本发明厌氧性生物降解促进剂的聚合材料更易于被生物降解。如图8所示,在Intertek进行的ASTM D5511测试中,含有厌氧性生物降解促进剂(5wt.%)的聚乙烯膜在第180天时,显示出25.99%的生物降解性,并在第480天时呈63.07%的生物降解,而不含厌氧性生物降解促进剂的聚乙烯膜在第180天仅具有1.09%的生物降解;如图9所示,在Intertek进行的ASTM D5511测试中,含有厌氧性生物降解促进剂(5wt.%)的聚甲醛树脂在第90天时,显示出29.16%的生物降解性,并在第450天显示出95.75%的生物降解,而不含厌氧性生物降解促进剂的聚甲醛树脂在90天仅显示出1.53%的生物降解。
其他实施例中显示,在Intertek进行的ASTM D5511测试中,含有厌氧性生物降解促进剂(5wt.%)的聚苯乙烯餐具在第90天显示出11.67%的生物降解,在第270天显示出33.13%的生物降解;而不含厌氧性生物降解促进剂的聚苯乙烯餐具在第60天仅显示出0.08%的生物降解;含有厌氧性生物降解促进剂(5wt.%)的聚苯乙烯杯盖在第90天显示10.50%的生物降解,而不含厌氧性生物降解促进剂的聚苯乙烯杯盖在90天仅显示0.78%的生物降解;含有厌氧性生物降解促进剂(5wt.%)的可发性聚苯乙烯泡沫塑料杯在第90天显示13.31%的生物降解,而不含厌氧性生物降解促进剂的可发性聚苯乙烯泡沫塑料杯在90天仅显示0.20%的生物降解;含有厌氧性生物降解促进剂(5wt.%)的聚对苯二甲酸乙二醇酯瓶在第45天显示6.36%的生物降解,而不含厌氧性生物降解促进剂的聚对苯二甲酸乙二醇酯瓶在第15天仅显示0.00%的生物分解;含有厌氧性生物降解促进剂(5wt.%)的聚丙烯杯在第45天显示出7.13%的生物降解,而不含厌氧性生物降解促进剂的聚丙烯杯在第第45天仅显示出0.05%的生物降解;含有厌氧性生物降解促进剂(5wt.%)的聚丙烯餐盒在第45天显示出7.57%的生物降解,而不含厌氧性生物降解促进剂的聚丙烯餐盒在45天仅显示出0.07%的生物分解。
在不背离本发明的精神和目的的情况下,厌氧性生物降解促进剂的组成可以根据不同的应用和以下一个或多个因素/标准而变化:生物降解性、厌氧性生物降解促进剂与聚合物材料的相容性、聚合物材料的疏水性、加工温度的相容性,机械性能的推断,热性质推断、外观推断、气味推断、食品接触安全要求等。
对于本领域技术人员来说,显而易见的是,上述系统和方法的示例仅用于说明本发明的作业原理,而非旨在穷举或将本发明限制于所公开的精确形式,许多修改和变化对于本领域技术人员将是显而易见。
选择和描述这些实施例是为了最好地解释本发明的原理及其实际应用,从而使本领域的其他技术人员能够理解本发明的各种实施例以及适用于预期特定用途的各种修改。
工业适用性:
本发明提供的厌氧性生物降解促进剂显着提高了聚合物材料在厌氧环境中的生物降解速率,并且不会显着影响原始聚合物材料的机械性能、可回收性和其他性能,例如当将其应用于食品接触安全产品(如餐具、饭盒、杯子和杯盖)时,不会影响其食品接触安全性。
Claims (25)
1.一种用于主体聚合物材料的厌氧性生物降解促进剂,其特征在于,包括:
载体基质,用于在促进剂中聚集所有其他成分,并协助将其分散到主体聚合物材料中;
至少一种生物组分,用于启动所述主体聚合物材料的生物降解;
保护层,用于保护所述至少一种生物组分,并延长所述厌氧性生物降解促进剂的保质期;
生物多样性促进剂,用于促进和稳定所述至少一种生物组分的生长;
表面活性剂,用于促进所述至少一种生物组分与所述主体聚合物材料的相互作用;
增容剂,用于增加所述厌氧性生物降解促进剂与该主体聚合物材料之间的兼容性;
抗氧化剂,用于抑制所述厌氧性生物降解促进剂在制造、保存和使用过程中的氧化反应;
增塑剂,以及;
性能调节剂。
2.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述载体基质占所述厌氧性生物降解促进剂的总重量的30%至90%,其中所述载体基质包括可生物降解和/或非生物降解材料,其选自聚乙烯(PE)、聚丙烯(PP)、聚醋酸乙烯酯(EVA)、聚苯乙烯(PS)、聚甲醛(POM)、聚对苯二甲酸乙二醇酯(PETG)、聚酰胺(PA)、聚碳酸酯(PC)、聚氨酯(PU)、热塑性弹性体(TPE)、醋酸纤维素(CA)、聚氯乙烯(PVC)、丙烯腈-丁二烯-苯乙烯(ABS)、聚乙烯醇(PVA)、聚乳酸(PLA)、多羟基脂肪酸酯(PHA)、聚丁二酸丁二醇酯(PBS)、聚己内酯(PCL)、聚己二酸丁二酯(PBAT)、聚乙醇酸(PGA)和聚乳酸-羟基乙酸(PLGA)中的一种或多种聚合物或其任何组合。
3.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述至少一种生物组分占所述厌氧性生物降解促进剂的总重量的大于0%至20%,其选自细菌、真菌和酶或其任意组合。
4.如权利要求3所述的厌氧性生物降解促进剂,其特征在于,所述细菌选自热梭菌、黄体微球菌、红球菌、栗褐链霉菌、不动杆菌属、产碱菌属、拟无枝酸菌属、节杆菌属、芽孢杆菌属、柠檬酸杆菌属、棒状杆菌属、肠杆菌属、微小杆菌属、赖氨酸芽孢杆菌属、巨型芽孢杆菌、枯草杆菌、微杆菌属、微球菌属、诺卡氏菌属、巴氏杆菌属、假单胞菌属、红球菌属、施莱格尔菌(Schlegelella)属、鞘氨醇杆菌属和葡萄球菌属。
5.如权利要求3所述的厌氧性生物降解促进剂,其特征在于,所述真菌选自酵母、黑曲霉、阿克霉属、曲霉属、金担子菌属、枝孢菌属、镰刀菌属、黏帚菌属、毛霉属、青霉属、拟盘多毛孢属、原毛平革菌属、链霉菌属、栓菌属和木霉菌属。
6.如权利要求3所述的厌氧性生物降解促进剂,其特征在于,所述酶选自α-淀粉酶、过氧化氢酶、纤维素酶、角质酶、解聚酶、酯酶、葡萄糖苷酶、水解酶、漆酶、脂肪酶、锰过氧化物酶、脲酶和蛋白酶,如木瓜蛋白酶、菠萝蛋白酶。
7.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述保护层占所述厌氧性生物降解促进剂的总重量的大于0%至30%,其中所述保护层包括一种或多种保护层材料,其选自阿拉伯胶、海藻酸钠、明胶、壳聚糖、纤维素、聚乙烯醇、聚(乳酸-羟基乙酸)、聚乙二醇或其任何组合。
8.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述生物多样性促进剂占所述厌氧性生物降解促进剂的总重量的大于0%至20%,其中所述生物多样性促进剂包括醣类化合物、含氮化合物、磷化合物或其任何衍生物以及微量营养素;其中所述醣类化合物包括环糊精、纤维素、淀粉、蔗糖和葡萄糖;所述含氮化合物包括蛋白质、肉类提取物、自溶物、硝酸盐和尿素;所述磷化合物包括五氧化二磷、磷酸氢、磷酸二氢根和有机磷酸盐;所述任何衍生物包括果胶、木聚糖、羧酸、氨基酸;所述微量营养素包括维生素、矿物质、钾、钙、镁、铁、锰、锌、硼、铜和钼;或其任意组合。
9.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述表面活性剂占所述厌氧性生物降解促进剂的总重量的大于0%至10%,其中所述表面活性剂是一种或多种非离子或离子表面活性剂,其中所述非离子表面活性剂包括聚山梨酸酯、山梨醇酯和烷基酚乙氧基化物;所述离子表面活性剂包括阳离子表面活性剂、阴离子表面活性剂、两性离子表面活性剂和生物表面活性剂,其中,所述阴离子表面活性剂包括含有阴离子官能团的化合物,包括硫酸盐、磺酸盐、磷酸盐、羧酸衍生物、烷基硫酸盐、琥珀酸磺酸二辛酯钠、全氟辛烷磺酸、全氟丁烷磺酸、烷基芳醚磷酸盐、烷基醚磷酸盐、烷基醚磷酸酯十二烷基苯磺酸钠、十二烷基硫酸纳、硬脂酸钠、硬脂酸钙,其中,所述烷基硫酸盐包括十二烷基硫酸铵,十二烷基硫酸钠和相关的烷基醚硫酸盐月桂酸钠和聚醚硫酸钠;其中所述阳离子表面活性剂包括盐酸辛烯胺、溴化十六烷基铵、氯化十六烷基吡啶、氯化苯扎氯铵、氯化苯乙氧铵、氯化二甲基十八烷基铵和二十八烷基二甲基铵;其中,所述两性离子表面活性剂包括十二烷基二甲胺氧化物和肉豆蔻胺氧化物;其中,所述生物表面活性剂包括糖脂、磷脂、脂肽、中性脂质、脂肪酸和脂多糖;或其任意组合。
10.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述增容剂占所述厌氧性生物降解促进剂的总重量的大于0%至10%,其中所述增容剂包括扩链剂和偶联剂,其中扩链剂包括改性苯乙烯-丙烯酸聚合物、乳酸、乙二醇和1,4-丁二醇;偶联剂包括马来酸酐、桐油酸酐、环氧化大豆油、亚甲基二苯基二异氰酸酯、丙烯酸和柠檬酸;或其任意组合。
11.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述增塑剂占所述厌氧性生物降解促进剂的总重量的大于0%至10%,其中所述增塑剂包括水、尿素、甘油、乙二醇、聚乙二醇、桐油酸酐、环氧大豆油、柠檬酸三乙酯和柠檬酸乙酰三乙酯或其任意组合。
12.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述性能调节剂占所述厌氧性生物降解促进剂的总重量的大于0%至10%,其中所述性能调节剂包括碳酸钙、二氧化钛、滑石粉、有机蒙脱土、膨润土、纳米填料、天然纤维、色母粒、气味母粒或其任意组合。
13.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述抗氧化剂占所述厌氧性生物降解促进剂的总重量的大于0%至10%,其中所述抗氧化剂包括抗坏血酸、生育酚、谷胱甘肽、四价[亚甲基(3,5-二叔丁基-4-羟基氢肉桂酸)]甲烷、三(2,4-二叔丁基苯基)亚磷酸酯、硫辛酸和尿酸,或其任意组合。
14.如权利要求1所述的厌氧性生物降解促进剂,其特征在于,所述主体聚合物材料包括聚乙烯(PE)、聚丙烯(PP)、聚醋酸乙烯酯(EVA)、聚苯乙烯(PS)、聚甲醛(POM)、聚对苯二甲酸乙二醇酯(PETG)、聚酰胺(PA)、聚碳酸酯(PC)、聚氨酯(PU)、热塑性弹性体(TPE)、醋酸纤维素(CA)、聚氯乙烯(PVC)、丙烯腈-丁二烯-苯乙烯(ABS)、聚乙烯醇(PVA)、聚乳酸(PLA)、多羟基脂肪酸(PHA)、聚丁二酸丁二醇酯(PBS)、聚己内酯(PCL)、聚己二酸丁二酯(PBAT)、聚乙醇酸(PGA)和聚乳酸-羟基乙酸(PLGA)或其任意组合,其中,所述主体聚合物材料是常规塑料或通过普通塑料加工技术的任何塑料,所述普通塑料加工技术包括挤出、树脂制造、发泡、片材生产、热成型、注塑、吹膜、吹塑、纤维/织物和长丝制造。
15.一种将如权利要求1所述的厌氧性生物降解促进剂制备为母粒的制备方法,其特征在于,所述方法包括:
将保护层材料引入至少一种生物组分,以在所述至少一种生物组分周围形成环绕的保护层;
在第一高温下,将所述具有环绕保护层的至少一种生物组分和所述厌氧性生物降解促进剂中的其余组分均质化,以获得混合物;以及
在第二高温下挤压所述混合物,直到获得母粒。
16.如权利要求15所述的制备方法,其特征在于,所述第一高温的温度范围为室温至80℃以及所述第二高温的温度范围为50℃至250℃。
17.如权利要求15所述的方法,其特征在于,所述均质化是在40至1000rpm的混合速度下进行。
18.一种制备含有如权利要求1所述的厌氧性生物降解促进剂的聚合物材料的方法,其特征在于,所述方法包括:
将所述厌氧生物降解促进剂与主体聚合物材料均质化,形成混合物;以及
在第三高温下挤压所述混合物,以获得含有厌氧性生物降解促进剂的聚合物材料;
其中,所述厌氧生物降解促进剂以母粒的形式与所述主体聚合物结合。
19.如权利要求18所述的方法,其特征在于,所述厌氧性生物降解促进剂的重量比占所述含有厌氧性生物降解促进剂的聚合物材料的总重量的大于0%到30%。
20.如权利要求18所述的方法,其特征在于,所述厌氧性生物降解促进剂的重量比占所述含有厌氧性生物降解促进剂的聚合物材料的总重量的1%到5%,以降低其对所述主体聚合物的机械性能和其他性能的影响,其中,所述其他性能包括食品接触安全性。
21.如权利要求18所述的方法,其特征在于,所述含有厌氧性生物降解促进剂的聚合物材料具有与所述主体聚合物材料相当的可回收性。
22.如权利要求18所述的方法,其特征在于,所述含有厌氧性生物降解促进剂的聚合物材料具有优于所述主体聚合物材料的生物降解性。
23.如权利要求18所述的方法,其特征在于,所述主体聚合物材料包括聚乙烯(PE)、聚甲醛(POM)、聚苯乙烯(PS)、膨胀聚苯乙烯(EPS)、聚丙烯(PP)或聚对苯二甲酸乙二醇酯(PET)。
24.如权利要求18所述的方法,其特征在于,所述第三高温的温度范围为50℃至300℃。
25.如权利要求18所述的方法,其特征在于,所述均质化是在40至1000rpm的混合速度下进行。
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