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Thermosets Based on Covalent Bond Exchange: Mechanisms, Properties, and Reprocessing
Xiaojuan Shi1,2, Daotong Zhuang1
1Shanghai Institute of Applied Mathematics and Mechanics, Shanghai Key Laboratory of Mechanics in Energy Engineering, School of Mechanics and Engineering Science, Shanghai University, Shanghai 200072, China.
Abstract:
Thermosets are widely used in engineering applications due to their high mechanical strength, thermal stability, and chemical resistance; however, their permanently crosslinked networks also limit repair, reshaping, and recycling. Dynamic covalent chemistry offers a route to addressing these limitations through the incorporation of reversible bond exchange into thermoset networks. A range of dynamic thermosets has been developed based on transesterification, Diels-Alder reactions, imine exchange, disulfide metathesis, boronic ester exchange, and siloxane equilibration, enabling self-healing, reprocessing, welding, and closed-loop recycling. This review examines representative dynamic thermosets in terms of exchange mechanisms, network topology evolution, and macroscopic response. By correlating molecular exchange processes with network-level mechanics and macroscopic performance, this review identifies design principles for dynamic thermosets with improved sustainability and processing compatibility.
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