由动态二缩醛基序实现的可回收、可降解和完全生物基共价适应性聚合物网络,ACS Sustainable Chemistry & Engineering

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由动态二缩醛基序实现的可回收、可降解和完全生物基共价适应性聚合物网络
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-02-08 , DOI: 10.1021/acssuschemeng.2c06870
Wenxiong Zhang ₁ , Fei Gao ₁ , Xuejiao Chen ₁ , Liang Shen ₁ , Yinjun Chen ₂ , Yangju Lin ₃

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共价适应性网络 (CAN) 可以在光刺激或热刺激下按需重新配置，最近被视为传统热固性聚合物的替代品。虽然这些材料表现出出色的可回收性和可再加工性，但迄今为止报告的大多数材料都是基于不可再生资源。同时，材料回收高度依赖收集系统，任何不可避免地从收集系统中逸出的材料最终都会进入环境，挑战大自然分解这些材料的能力。因此，同时具有可回收性和可降解性的CAN材料是非常可取的。在这项工作中，我们寻求同时解决 CAN 材料的可回收性、可再生性和可降解性。Spiro 二缩醛结构单元来源于生物基苯甲醛和赤藓糖醇，然后使用生物基环氧大豆油作为交联剂进行固化过程，得到完全生物基的 CAN 材料。由于缩醛基序的动态和可降解特性，我们的 CAN 材料表现出良好的可回收性和酸降解性，并且降解产物可重复用于制备新的 CAN。此外，通过调整与活性酚位点相邻的空间位阻，我们能够使用不同的生物基苯甲醛（香草醛、乙基香草醛和丁香醛）来控制 CAN 的机械性能。目前的研究成果为可回收和可降解的生物基 CAN 的设计提供了策略，这将扩展 CAN 的发展。

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Recyclable, Degradable, and Fully Bio-Based Covalent Adaptable Polymer Networks Enabled by a Dynamic Diacetal Motif

Covalent adaptable networks (CANs), which can reconfigure on-demand under photo- or thermal stimuli, have recently been pursued as an alternative to the traditional thermosetting polymers. While these materials have demonstrated excellent recyclability and reprocessability, the majority of them reported to date are based on non-renewable resources. Meanwhile, material recycling highly counts on the collection system, and any materials that inevitably escape from the collection system will eventually go to the environment, challenging nature’s ability to break down these materials. Therefore, CAN materials that possess both recyclability and degradability are highly desirable. In this work, we seek to simultaneously address the recyclability, renewability, and degradability of CAN materials. Spiro diacetal building blocks are derived from bio-based benzaldehyde and erythritol and then subjected to the curing process using bio-based epoxy soybean oil as crosslinkers, yielding fully biobased CAN materials. Owing to the dynamic and degradable features of acetal motifs, our CAN materials exhibit both good recyclability and acid degradability, and the degraded products are reusable for preparation of new CANs. In addition, by tuning the steric hindrance adjacent to the reactive phenol site, we are able to control the mechanical properties of CANs using different bio-based benzaldehydes (vanillin, ethyl vanillin, and syringaldehyde). The outcome of the current research provides a strategy for the design of recyclable and degradable bio-based CANs, which will extend the development of CANs.

更新日期：2023-02-08

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