Exploring enzymatic degradation, reinforcement, recycling, and upcycling of poly(ester)s-poly(urethane) with movable crosslinks

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem Pub Date : 2024-10-29 DOI:10.1016/j.chempr.2024.09.026

Jiaxiong Liu, Ryohei Ikura, Kenji Yamaoka, Akihide Sugawara, Yuya Takahashi, Bunsho Kure, Naomi Takenaka, Junsu Park, Hiroshi Uyama, Yoshinori Takashima

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Abstract

Enzymes are highly efficient, chemoselective, and sustainable biocatalysts, standing out as eco-friendly tools to advance the circular plastics economy. Herein, we explored enzymatic reactions of poly(ε-caprolactone)-poly(urethane) (PCL-PUs) in organic solvent under different reaction conditions using Novozym 435 (immobilized lipase) as the enzyme. PCL-PUs with triacetylated γ-cyclodextrin (TAcγCD)-based movable crosslinks (PCL-γCD-PU) not only exhibited excellent mechanical properties due to effective energy dissipation, but also efficient enzymatic degradation that was optimized for increases in TAcγCD content. Under reaction time control, molecular weight and mechanical properties of PCL-γCD-PU were enhanced by a novel enzymatic reinforcement strategy. Without sorting, the degraded products are versatile resources that can be enzymatically closed-loop recycled by switching reaction concentration or enzymatically upcycled into value-added polymers by mixing with selective substrates. The facile polymer structure design combined with enzymatic reactions is expected to provide a broad approach for toughening various polymeric materials and advancing their development as sustainable resources.

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探索具有可移动交联的聚（酯）-聚（氨基甲酸乙酯）的酶降解、加固、回收和再循环

酶是一种高效、化学选择性和可持续的生物催化剂，是推动循环塑料经济的环保工具。在此，我们以 Novozym 435（固定化脂肪酶）为酶，探索了在不同反应条件下有机溶剂中聚（ε-己内酯）-聚（氨基甲酸乙酯）（PCL-PUs）的酶促反应。具有基于三乙酰化γ-环糊精（TAcγCD）的可移动交联的 PCL-PU（PCL-γCD-PU）不仅由于有效的能量耗散而表现出优异的机械性能，而且随着 TAcγCD 含量的增加，酶降解效果也得到了优化。在反应时间控制下，新型酶强化策略提高了 PCL-γCD-PU 的分子量和机械性能。降解产物无需分拣，是一种多功能资源，可通过转换反应浓度进行酶法闭环循环，或通过与选择性基质混合进行酶法升级循环，转化为高附加值聚合物。简便的聚合物结构设计与酶促反应相结合，有望为各种聚合物材料的增韧提供广泛的方法，并推动其作为可持续资源的发展。

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来源期刊

Chem Environmental Science-Environmental Chemistry

CiteScore

32.40

自引率

1.30%

发文量

281

期刊介绍： Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.