Thermoset Architecture Fusion Enabled by Catalyst-Free C═C/C═N Metathesis Chemistry

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Thermoset Architecture Fusion Enabled by Catalyst-Free C═C/C═N Metathesis Chemistry
Title:
Thermoset Architecture Fusion Enabled by Catalyst-Free C═C/C═N Metathesis Chemistry
Journal Title:
Journal of the American Chemical Society
Keywords:
Publication Date:
05 September 2025
Citation:
Zheng, J., Rusli, W., Tang, K. Y., Goh, W. P., Ding, N., Chien, S. W., Hadjichristidis, N., & Li, Z. (2025). Thermoset Architecture Fusion Enabled by Catalyst-Free C═C/C═N Metathesis Chemistry. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.5c12217
Abstract:
Thermosets with permanent crosslinked structures provide excellent durability but pose significant challenges for reprocessing and recycling, raising engineering and environmental concerns as their usage expands. The advent of covalent adaptable networks (CANs) with dynamic covalent linkages has improved thermoset recyclability and enabled the fusion of identical polymer networks (A-A type fusion). However, fusing different thermosets (A-B type fusion) remains challenging due to their distinct dynamic behaviors and variable activation energies for bond exchange. This study introduces catalyst-free solid-state C=C/C=N metathesis chemistry to achieve A-B type fusion between two distinct thermosets. Furthermore, by simply adjusting the mixing ratio of the parent thermosets, the thermal behavior, mechanical properties, activation energy (Ea), and topology freezing transition temperature (Tv) of the fused networks can be precisely tailored. This approach offers enhanced control over thermal and mechanical characteristics, rendering them suitable for diverse high-performance applications. Our findings represent a significant step forward in developing recyclable thermosets with improved engineering performance, contributing to advancing a more sustainable circular economy.
License type:
Publisher Copyright
Funding Info:
This research / project is supported by the Agency for Science, Technology and Research - RIE2025 Manufacturing, Trade and Connectivity - Developing a toolbox for nex-gen circular plastic materials
Grant Reference no. : M22K9b0049

This research / project is supported by the Agency for Science, Technology and Research - Manufacturing, Trade and Connectivity - Developing Liquid Wood Resin for Sustainable Specialty Polymers
Grant Reference no. : M25O2b0016
Description:
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see 10.1021/jacs.5c12217.
ISSN:
0002-7863
1520-5126
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