Advancing Recyclable Thermosets through C═C/C═N Dynamic Covalent Metathesis Chemistry

• DOI: 10.1021/jacs.4c05346
• Publication Date: 2024-07-24T17:25:27Z
• Authors: Jie Zheng; Hongzhi Feng; Xinglong Zhang; Jianwei Zheng; Jeffrey Kang Wai Ng; Sheng Wang; Nikos Hadjichrist...; Zibiao Li
• Keywords: Dynamic Covalent Chemistry; Thermosetting polymer

Thermoset polymers have become integral to our daily lives due their exceptional durability, making them feasible for a myriad of applications; however, this ubiquity also raises serious environmental concerns. Covalent adaptable networks (CANs) with dynamic covalent linkages that impart efficient reprocessability and recyclability thermosets garnered increasing attention. While various exchange reactions been explored in CANs, many rely on the stimuli active nucleophilic groups and/or catalysts, introducing performance instability escalating initial investment. Herein, we propose new direct catalyst-free C═C/C═N metathesis reaction between α-cyanocinnamate aldimine as novel motif constructing recyclable thermosets. This chemistry offers mild conditions (room temperature catalyst-free), ensuring high yields simple isolation procedures. By incorporating into covalently cross-linked polymer networks, obtained exhibit both malleability reconfigurability. The resulting tunable properties, coupled thermal stability linkage-based enrich toolbox chemistry.