Zhao Wuchao, Guo Zongpeng, He Jianghua, Zhang Yuetao
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, Jilin, China, 130012.
Angew Chem Int Ed Engl. 2025 Feb 24;64(9):e202420688. doi: 10.1002/anie.202420688. Epub 2025 Jan 9.
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. MgCl 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.
开发一种简单高效的催化剂体系,用于将聚合物闭环回收为单体,对于聚合物废料的回收利用以及防止塑料制品的降级循环来说,是一项至关重要但具有挑战性的任务。在此,我们采用廉价的、市售的路易斯酸(LAs),通过脂肪族聚酯和聚碳酸酯的催化解聚,在本体中实现闭环回收。通过热重分析实验和蒸馏实验筛选了路易斯酸的范围。MgCl表现出最佳的催化性能,能够在显著低于上限温度的温度下,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))高效解聚为单体(产率高达98%)。此外,该催化剂体系在存在其他通用塑料的情况下,对(共)聚酯以及聚酯与聚碳酸酯共混物的解聚表现出高选择性和兼容性,并且具有出色的催化剂循环和再利用性能。机理研究表明,单体的闭环回收是通过无规断链和端基环化实现的。