CN102595942A - 生物可降解的香烟过滤器丝束及其制造方法 - Google Patents
生物可降解的香烟过滤器丝束及其制造方法 Download PDFInfo
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Abstract
本发明涉及包含纤维素和醋酸纤维素复合丝的生物可降解的香烟过滤器丝束,和制备这类过滤器丝束的方法,所述方法包括在离子型液体或N-甲基吗啉-N-氧化物(NMMO)中提供包含纤维素和醋酸纤维素混合物的溶液粘稠物,并将所述混合物纺入或铸入质子性溶剂中以产生纤维或薄膜,以及将所述纤维或薄膜转化成香烟过滤器丝束。本发明还涉及由这类过滤器丝束制成的香烟过滤器和香烟。
Description
本发明涉及尤其适用于香烟过滤器丝束中的生物可降解的复合材料。
于20世纪20年代开发出第一种香烟过滤器,其由皱纹纸构成,有时还含有纤维素填料。随后对吸烟与健康之间有害联系的关注导致对能够产生较低焦油水平的过滤器的强烈需求。开发出一种在纸鞘内含有醋酸纤维素纤维的双层过滤器,其允许添加其它功能性成分如活性炭。
随着对健康的进一步关注,对减少焦油、尼古丁和一氧化碳水平的法规和市场压力的增加需要持续开发过滤器技术。当今,香烟国际市场每年突破5.8万亿根,其中的97%现在含有过滤器。在带过滤器香烟中,80.4%由标准醋酸纤维素纤维制成(4.5万亿根),16.6%被归入‘专用’过滤器,且3%由聚丙烯制成。
通常,香烟过滤器包含“过滤器丝束”,“过滤器丝束”通常为包在水松纸内的卷曲的醋酸纤维素纤维。本发明涉及过滤器丝束成分。
制造香烟和香烟过滤器最迫切的问题之一是过滤器的生物降解速率。根据环境条件,醋酸纤维素过滤器将花费一个月至三年来进行生物降解,这不能快到足以避免垃圾问题。丢弃的香烟过滤器在几乎所有沿海清洁调查中占据榜首。垃圾问题不仅仅是视觉问题,由用过的香烟过滤器吸附的毒素已被发现泄漏于环境中,并且具有潜在的生物危害。
已经提出一系列用于制备可生物降解过滤器丝束的方法,包括使用醋酸纤维素与其它可生物降解聚合物的复合物、用于提高醋酸纤维素降解速率的添加剂、具有用于提高生物降解性的低取代度(DS)的醋酸纤维素以及生物可降解的聚合物,如PHB/PVB和淀粉,作为过滤器丝束原材料。
然而,到目前为止,还没有找到能够制造出消费者可接受的过滤器的令人满意的商业方案,这种过滤器能够足够快速地被降解从而克服垃圾问题。上述方法的一个主要限制是在过滤器材料可达到的生物降解速率和所产生的吸收谱/口味特征之间实现了可接受的折中。
本发明力图解决这些问题。
本发明提供了生物可降解的香烟过滤器丝束,其包含纤维素和醋酸纤维素复合丝。
纤维素和醋酸纤维素通常以纤维或薄膜的形式铸制。每一种铸制形式都适用于制备本发明的生物可降解的香烟过滤器丝束。当以薄膜形式铸制时,那么必要的是将所产生的薄膜撕碎以产生适用于香烟过滤器丝束的材料。本发明优选的过滤器丝束包含从纤维素和醋酸纤维素凝固溶液纺制出的纤维。
本文所指的纤维素/醋酸纤维素复合丝应被理解为表示从包含纤维素和醋酸纤维素的粘稠物纺制的纤维或从相似组成的粘稠物铸制的碎膜。
我们发现,纤维素/醋酸纤维素复合丝的生物降解性显著大于仅包含纤维素或醋酸纤维素的等同丝。不希望受到任何这类理论的束缚,我们认为,复合物中醋酸盐的存在可以破坏纤维素的结晶度,导致该复合物能够比纤维素本身更快地得到降解。
按照常规,纤维素是从纤维胶铸制或纺制成的,并且从同一混合物难以或不可能铸制或纺制出醋酸纤维素,因为醋酸纤维素在这些条件下有水解的可能。相反,按照常规,醋酸纤维素是从丙酮铸制或纺制成的,并且从同一混合物难以或不可能铸制或纺制出纤维素,因为纤维素在丙酮中的溶解度受限。
然而,我们发现通过从离子型液体(IL)或从N-甲基吗啉-N-氧化物(NMMO)铸制或纺制纤维素和醋酸纤维素,可能形成包含这些材料的复合混合物的纺成纤维和铸型薄膜。这类复合物的提高的生物降解性及其在香烟过滤器丝束制造中的适用性在之前是没有意识到的。
因此,本发明的香烟过滤器丝束优选由从离子型液体(IL)或从N-甲基吗啉-N-氧化物(NMMO)纺制或铸制出的作为混合物的纤维素和醋酸纤维素纤维或薄膜制成。
IL和NMMO用于溶解纤维素和其它聚合物的用途已被充分证明,例如在阿拉巴马大学的US20050288484和US 20070006774、北卡罗来纳州立大学的US20080188636以及Holbrey等的WO2005098546中。大量的离子型液体,包括前述出版物中公开的那些,适于溶解纤维素和醋酸纤维素,并适于从其铸制成作为混合物的纤维或薄膜。合适的IL的一般类型包括基于咪唑、吡咯、噻唑或吡唑阳离子与卤素、磷酸盐、羧酸盐或金属氯化物阴离子的结合的那些IL。特别优选的IL包括1-丁基-3-甲基咪唑氯化物(BMIM-Cl)、1-丁基-3-甲基咪唑醋酸盐(BMIM-Ac)和1-乙基-3-甲基咪唑醋酸盐(EMIM-Ac)。
从其纺制纤维或铸制薄膜的纤维素和醋酸纤维素溶液在本文称为粘稠物。粘稠物还可以包含非质子性溶剂如DMSO、DMF、THF或二噁烷,从而促进纤维素和/或醋酸纤维素的溶解。一种特别优选的非质子性溶剂是DMSO。
粘稠物中醋酸纤维素和纤维素的混合物还可以包含一种或多种其它热塑性材料,例如聚羟基脂肪酸酯如PHB和/或PHVB,这些材料可以为本发明的香烟过滤器丝束添加其它功能如防水功能。其它功能性添加剂可以包括用于功能目的的醋精、聚丙烯腈(PAN)、聚-2-羟乙基丙烯酸甲酯(PHEMA)、聚乙烯醇(PVA)、聚苯胺和聚乙二醇,所述功能目的例如吸收和/或口味谱的改善、降解增强(例如通过水溶性材料)以及成型性能改善,例如与湿强度相关(醋精可以改善口味谱,以及可以充当增塑剂)。
粘稠物中以及因此本发明的香烟过滤器丝束中纤维素与醋酸纤维素的重量比为10∶90至90∶10,例如20∶80至80∶20或30∶70至70∶30。
通常,粘稠物包含高达约50%w/w,优选高达约40%w/w,更优选高达约30%w/w且最优选高达约20%w/w的固体含量。
本发明的过滤器丝束还可以包含一种或多种增塑剂如醋精,其可以促进复合丝卷曲。在本发明的香烟过滤器丝束中,纤维素/醋酸纤维素的复合丝优选被卷曲,以提供烟屏障接触点。增塑剂可以包含在粘稠物中,或可以在纺制或铸制之后添加,例如通过在卷曲之前或之中喷射到过滤器丝束表面。
本发明的过滤器丝束还可以包含促进过滤器丝束氧化降解的催化剂。合适的催化剂包括铁和铜的氧化物以及氯化物,可以通过将复合丝浸入水溶性铁盐或铜盐如硫酸盐或氯化物中,并用氢氧化钠或其它合适的沉淀剂处理使氧化物(优选为纳米形式)沉淀于细丝上或细丝中,来将催化剂引入丝束中。
所述丝束还可以包含一种或多种润滑剂以降低静电荷。优选的润滑剂包括矿物油。例如,可以在纺制纤维或铸制薄膜的过程中将具有乳化剂的1%w/w的矿物油施加到复合丝中。
优选地,本发明的过滤器丝束包含以每根细丝1、5或9旦尼尔(细丝厚度(每根细丝的旦尼尔数)定义为9000m单根非卷曲细丝的质量(克))制造出的纤维素/醋酸纤维素复合丝。
总丝束质量(总旦尼尔)(定义为9000m非卷曲过滤器丝束的总质量,通常包含数千根,例如11,000根单根纤维)将随纤维纺制所用的方法和丝束中单根纤维的数量而显著变化。一根典型的丝束的质量为35,000g。
优选地,本发明的过滤器丝束包含具有三叶形细丝横截面的纤维(任选地,用三叶形喷丝孔形成),从而优化表面积。
本发明的过滤器丝束优选包含卷曲的纤维,卷曲结构由卷曲指数定义,卷曲指数是拉伸的(加载25kg)过滤器丝束与非拉伸的(加载0.25kg)过滤器丝束的比值。卷曲指数将随确切的制造方法而显著变化。
本发明的香烟过滤器丝束含水量优选为至少约2%w/w,更优选至少约5%w/w,更优选至少约10%w/w。已发现含水量对防止静电荷至关重要,但优选不要过高(例如,不高于50%w/w),因为丝束具有很高的含水量将难以保持弯曲。
本发明的过滤器丝束优选包含缠绕的细丝。
本发明还提供了包含在接装纸(tipping wrapper)中包装的上文所描述的香烟过滤器丝束的香烟过滤器。
优选地,接装纸本身是生物可降解的物质,并且例如可以包含纸或可选的生物可降解的基质如纤维素、PLA、羟基烷酸酯、淀粉基聚合物或其它形式的生物聚合物。
当接装纸包含生物聚合物时,其优选包含在量上不超过约25%重量比的软化剂,以实现尤其与伸长和管弯曲相关的适宜的性质。
生物聚合物接装纸中的软化剂可以选自任何合适的材料,但优选选自丙三醇、丙烷-1,2-二醇以及选自German Tobacco Ordnance(TVO)名录下的任何其它合适的软化剂。
本发明还提供了包含可抽吸的物质和上文所述的香烟过滤器的香烟。
本发明还提供了制造香烟过滤器丝束的方法,其包括在离子型液体或NMMO中提供包含纤维素和醋酸纤维素混合物的溶液,并将所述混合物纺入或铸入质子性溶剂以产生纤维或薄膜,以及将所述纤维或薄膜转化成香烟过滤器丝束。
水是用于混合物再生铸制的优选质子性溶剂。
在本发明的方法中,可以通过在水和/或其它质子性溶剂中再生溶液来产生任何比值的复合纤维素/醋酸纤维素材料。水中的凝固速率已被发现依赖于粘稠物中醋酸纤维素的含量,其中提高的醋酸纤维素水平降低凝固速率。
下面结合实施例并参照附图对本发明进行更详细的描述。
图1展示了显示i)醋酸纤维素纤维;ii)纤维素纤维;以及iii)本发明的纤维素和醋酸纤维素混合物纤维的三个载玻片。
图2展示了图1的载玻片在厌氧条件下生物降解2周后。
图3展示了图1的载玻片在厌氧条件下生物降解4周后。
图4展示了图1的载玻片在厌氧条件下生物降解6周后。
实施例1
与等同的纤维素湿纺纤维和等同的醋酸纤维素湿纺纤维相比来评价混合纤维素/醋酸纤维素湿纺纤维的生物降解性。
利用标准的湿纺设备,从EMIM-Ac∶DMSO(20∶80)中i)纤维素(DP~800)和ii)1∶1纤维素∶醋酸纤维素(Eastman,CA-398-30)固体为10%的溶液纺制纤维。使用孔径为70μm的40-孔喷丝头,其浸入含有纯净水的室温凝固池中。湿纤维被卷起,在卷轴上充分洗涤,然后在50℃干燥。
参照图1至4,这些复合材料的惊人特性是在厌氧环境下的生物降解速率超过相同条件下的纤维素,并远远超过醋酸纤维素(参见附录1)。认为(尽管该理论绝对不应被认为是束缚)两种成分形成了最终的混合复合物,以及提高的降解速率来自纤维素结晶度的降低。复合物纤维素成分的降解被认为导致醋酸纤维素成分以分子尺度沉淀。我们还发现,本发明的香烟过滤器丝束在有氧条件下的生物降解速率同样被提高。
这些复合材料在制造纤维中的应用提供了获得具有以下特性的产品的途径:同时具有利用单独的醋酸纤维素所获得的期望的吸收谱/口味特征,和显著提高的生物降解速率。
实施例2
利用干纺法来制造本发明的过滤器丝束。首先将二醋酸纤维素和纤维素(1∶1混合)以10%的固体溶解于EMIM-Ac∶DMSO(20∶80)中来制备粘稠物。添加TiO2以产生增白的外观。然后过滤粘稠物,并在纺制进小室,使得细丝固化并逐渐变细。从一系列纺丝仓纺制出多于10,000根细丝,它们结合形成一股。填塞箱用来模压具有卷曲结构的过滤器丝束,将得到的过滤器丝束在水松纸包装以形成香烟过滤器。
发现所得到的香烟过滤器保留了实施例1所示的有利的生物降解性并且具有令人满意的口味特征。
Claims (14)
1.生物可降解的香烟过滤器丝束,其包含纤维素和醋酸纤维素复合丝。
2.如权利要求1所述的过滤器丝束,其还包含一种或多种其它热塑性材料。
3.如权利要求2所述的过滤器丝束,其中所述其它热塑性材料选自以下的一种或多种:PHB、PHVB、聚丙烯腈(PAN)、聚-2-羟乙基丙烯酸甲酯(PHEMA)、聚乙烯醇(PVA)、聚苯胺和聚乙二醇。
4.如权利要求1至3中任一项所述的过滤器丝束,其中纤维素与醋酸纤维素的重量比为10∶90至90∶10。
5.如权利要求4所述的过滤器丝束,其中纤维素与醋酸纤维素的所述比值为20∶80至80∶20。
6.如权利要求5所述的过滤器丝束,其中纤维素与醋酸纤维素的所述比值为30∶70至70∶30。
7.如权利要求1至6中任一项所述的过滤器丝束,其还包含一种或多种增塑剂。
8.如权利要求1至7中任一项所述的过滤器丝束,其还包含促进所述过滤器丝束氧化降解的催化剂。
9.如权利要求1至8中任一项所述的过滤器丝束,其还包含一种或多种润滑剂以降低所述丝束上的静电荷。
10.香烟过滤器,其包含在接装纸中包装的权利要求1至9中任一项所述的香烟过滤器丝束。
11.香烟,其包含可抽吸的物质和权利要求10所述的香烟过滤器。
12.制造权利要求1至9中任一项所述的香烟过滤器丝束的方法,包括在离子型液体或N-甲基吗啉-N-氧化物(NMMO)中提供包含纤维素和醋酸纤维素混合物的溶液粘稠物,并将所述混合物纺入或铸入质子性溶剂中以产生纤维或薄膜,以及将所述纤维或薄膜转化成香烟过滤器丝束。
13.如权利要求12所述的方法,其中所述粘稠物还包含非质子性溶剂,以促进所述纤维素和/或醋酸纤维素的溶解。
14.如权利要求13所述的方法,其中所述非质子性溶剂包含DMSO、DMF、THF或二噁烷中的一种或多种。
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