Solvent-Free Chemical Recycling of Polyesters and Polycarbonates by Magnesium-Based Lewis Acid Catalyst

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Dr. Wuchao Zhao, Zongpeng Guo, Prof. Dr. Jianghua He, Prof. Dr. Yuetao Zhang
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Abstract

Developing a simple and efficient catalyst system for closed-loop recycling of polymers to monomers is an essentially important but challenging task for the recycle of polymer wastes and preventing the downcycle of plastic products. Herein, we employ inexpensive, commercially available Lewis acids (LAs) to achieve closed-loop recycling in bulk through the catalytic depolymerization of aliphatic polyesters and polycarbonates. The scope of LAs is screened by thermogravimetric analysis experiments and distillation experiments. MgCl2 shows the best catalytic performance that can efficiently depolymerize eleven aliphatic polyesters and polycarbonates (i.e. poly(ϵ-caprolactone) and poly(trimethylene carbonate)), into monomers (up to 98 % yield) at temperatures significantly lower than the ceiling temperature. Moreover, this catalyst system exhibits high selectivity and compatibility towards the depolymerization of (co)polyesters as well as the blends of polyesters and polycarbonates in the presence of other commodity plastics, as well as excellent recycle and reuse catalyst performance. Mechanistic studies indicate that the closed-loop recycling of monomers is achieved through the random chain scission and terminal group cyclization.

Abstract Image

镁基路易斯酸催化聚酯和聚碳酸酯的无溶剂化学回收
开发一种简单高效的催化剂体系,实现聚合物到单体的闭环再循环,对于聚合物废弃物的再循环和防止塑料制品的下循环是一项非常重要但具有挑战性的任务。在这里,我们采用廉价的、市售的路易斯酸(LAs),通过催化脂肪族聚酯和聚碳酸酯的解聚来实现大批量的闭环回收。通过热重分析实验和蒸馏实验筛选了LAs的作用范围。MgCl2表现出最好的催化性能,可以在明显低于上限温度的温度下,有效地将11种脂肪族聚酯和聚碳酸酯(即聚(ε‐己内酯)和聚(三亚甲基碳酸酯)解聚成单体(产率高达98%)。此外,该催化剂体系对(co)聚酯的解聚以及聚酯和聚碳酸酯在其他商品塑料存在下的共混物表现出高选择性和相容性,以及优异的回收和再利用催化剂性能。机理研究表明,单体的闭环循环是通过随机链断裂和末端基环化实现的。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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