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Chemo‐Enzymatic Depolymerization of Functionalized Low‐Molecular‐Weight Polyethylene
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2024-09-25 , DOI: 10.1002/anie.202415012
Uwe Bornscheuer, Thomas Oiffer, Friedemann Leipold, Philipp Süss, Daniel Breite, Jan Griebel, Muhammad Khurram, Yannick Branson, Erik de Vries, Agnes Schulze, Christiane A. Helm, Ren Wei

Polyethylene (PE) is the most commonly used plastic type in the world, contributing significantly to the plastic waste crisis. Microbial degradation of PE in natural environments is unlikely due to its inert saturated carbon‐carbon backbones, which are difficult to break down by enzymes, challenging the development of a biocatalytic recycling method for PE waste. Here, we demonstrated the depolymerization of low‐molecular‐weight (LMW) PE using an enzyme cascade that included a catalase‐peroxidase, an alcohol dehydrogenase, a Baeyer Villiger monooxygenase, and a lipase after the polymer was chemically pretreated with m‐chloroperoxybenzoic acid (mCPBA) and ultrasonication. In a preparative experiment with gram‐scale pretreated polymers, GC‐MS and weight loss determinations confirmed ~27% polymer conversion including the formation of medium‐size functionalized molecules such as ω‐hydroxy acids and α,ω‐carboxylic acids. Additional polymer property analyses using AFM showed that enzymatic depolymerization reduced the particle sizes of this mCPBA‐ and enzyme‐treated LMWPE. This multi‐enzyme catalytic concept with distinct chemical steps represents a unique starting point for future development of bio‐based recycling methods for polyolefin waste.

中文翻译:


功能化低分子量聚乙烯的化学酶解聚



聚乙烯 (PE) 是世界上最常用的塑料类型,对塑料垃圾危机造成了重大影响。 PE 在自然环境中不太可能被微生物降解,因为它具有惰性饱和碳碳主链,很难被酶分解,这对开发 PE 废物的生物催化回收方法提出了挑战。在这里,我们证明了在用间氯过苯甲酸对聚合物进行化学预处理后,使用包括过氧化氢酶-过氧化物酶、乙醇脱氢酶、Baeyer Villiger 单加氧酶和脂肪酶在内的酶级联来解聚低分子量(LMW)PE (mCPBA) 和超声处理。在克级预处理聚合物的制备实验中,GC-MS 和重量损失测定证实了约 27% 的聚合物转化,包括形成中等尺寸的官能化分子,如 ω-羟基酸和 α,ω-羧酸。使用 AFM 进行的其他聚合物特性分析表明,酶解聚降低了经过 mCPBA 和酶处理的 LMWPE 的粒径。这种具有独特化学步骤的多酶催化概念代表了聚烯烃废物生物基回收方法未来发展的独特起点。
更新日期:2024-09-25
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