Closed-loop recycling of tough epoxy supramolecular thermosets constructed with hyperbranched topological structure

Junheng Zhang (), Can Jiang, Guoyan Deng, Mi Luo, Bangjiao Ye, Hongjun Zhang (), Menghe Miao, Tingcheng Li and Daohong Zhang ()
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Junheng Zhang: South-Central Minzu University
Can Jiang: South-Central Minzu University
Guoyan Deng: South-Central Minzu University
Mi Luo: University of Science and Technology of China
Bangjiao Ye: University of Science and Technology of China
Hongjun Zhang: University of Science and Technology of China
Menghe Miao: The University of Melbourne
Tingcheng Li: South-Central Minzu University
Daohong Zhang: South-Central Minzu University

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract The regulation of topological structure of covalent adaptable networks (CANs) remains a challenge for epoxy CANs. Here, we report a strategy to develop strong and tough epoxy supramolecular thermosets with rapid reprocessability and room-temperature closed-loop recyclability. These thermosets were constructed from vanillin-based hyperbranched epoxy resin (VanEHBP) through the introduction of intermolecular hydrogen bonds and dual dynamic covalent bonds, as well as the formation of intramolecular and intermolecular cavities. The supramolecular structures confer remarkable energy dissipation capability of thermosets, leading to high toughness and strength. Due to the dynamic imine exchange and reversible noncovalent crosslinks, the thermosets can be rapidly and effectively reprocessed at 120 °C within 30 s. Importantly, the thermosets can be efficiently depolymerized at room temperature, and the recovered materials retain the structural integrity and mechanical properties of the original samples. This strategy may be employed to design tough, closed-loop recyclable epoxy thermosets for practical applications.

Date: 2024
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DOI: 10.1038/s41467-024-49272-3

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