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Selective Bond Cleavage Strategies for Chemical Recycling of Thermosets and Their Composites
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DOI：10.1016/j.progpolymsci.2025.102069.png)
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Abstract
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Thermosetting polymers and their fiber-reinforced composites are widely used in engineering structures due to their superior thermal and mechanical properties, chemical resistance, and high specific strength and stiffness. However, their densely covalent crosslinked networks present trade-offs between degradation efficiency, selectivity, and scalability for end-of-life recycling, which hinder the retention and reuse of material value. As production and in-service stock continue to grow, end-of-life waste streams are rapidly expanding, exacerbating environmental burdens and the loss of high-value resources. Recycling of thermosets and their composites has therefore become a pressing challenge. This review focuses on the concept of selective bond cleavage strategies and examines two complementary pathways: end-based recycling, which targets the selective deconstruction of existing thermosets and composites, and source-based recycling, which involves designing new resin systems with built-in recyclability. It discusses hydrolysis, alcoholysis, aminolysis, ammonolysis, hydrazinolysis and acidolysis of ester, urea and imide linkages, as well as degradation mediated by strong bases, Lewis and Brønsted acids, and transition metals that cleave C-O, C-N and C-C bonds. The design principles of cleavable or dynamic motifs, together with reversible polymerization and on-demand depolymerization in recyclable thermosets are also summarized. Through a comparative literature analysis, we highlight the trade-off between degradation efficiency and selectivity in end-based recycling and the balance among service performance, processability and deconstruction efficiency in source-based recycling. An application-oriented framework centered on selective deconstruction and efficient reconstruction is proposed, emphasizing the critical roles of mass/heat transfer, solvent and phase behavior, separation and reutilization, process intensification and scale-up, and system-level techno-economic analysis and life cycle assessment. Finally, we outline the key challenges and future directions for bridging laboratory-scale research with engineering practice and industrial implementation.
Keywords:
Thermosetting polymers and composites
Selective bond cleavage
Chemical recycling
Closed-loop recycling
Upcycling
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