Entropy-driven toughening and closed-loop recycling of polymers via divergent metal-pyrazole interactions

Lei Huang, Jiujie Xia, Zeyuan Jin, Xinman Hu, Xiping Chen, Ning Zhao (), Changyou Gao () and Wenxing Liu ()
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Lei Huang: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering
Jiujie Xia: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering
Zeyuan Jin: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering
Xinman Hu: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering
Xiping Chen: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering
Ning Zhao: University of Chinese Academy of Sciences, Laboratory of Polymer Physics and Chemistry, Institute of Chemistry, Chinese Academy of Sciences
Changyou Gao: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering
Wenxing Liu: Zhejiang University, MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Developing dynamic polymeric materials that possess closed-loop recyclability under mild conditions and outstanding mechanical properties is a highly desirable but challenging pursuit. This study presents a entropy-driven toughening strategy through divergent metal-pyrazole (DiMP) coordinations, achieving a mechanically robust and recyclable polyurethane (PU) elastomer. DiMP interactions feature multiple discrete complexes (i.e., CuL2, Cu2L2, and CuL3, where L = dipyrazole ligand) to minimize the entropy-gain mediated compensatory effect during bond dissociation and accordingly increase energy dissipation upon polymer deformation. The DiMP-crosslinked PUs (DiMPUs) exhibit an unprecedented 11-fold improvement in toughness (310.8 MJ m−3), a tensile strength of 59.0 MPa, and exceptional elastic recovery (94%), attributed to gradient energy dissipation mechanisms involving dynamic DiMP coordinations and synergistically hierarchical hydrogen bonds. Crucially, the selective acidolysis of pyrazole-urea bonds, together with the inherently weak protonation affinity of pyrazole relative to amine, allows monomers to be efficiently recovered and reengineered into virgin materials, manifesting the closed-loop recyclability. This work provides a sustainable blueprint for dynamic polymers balancing mechanical robustness and environmental circularity.

Date: 2025
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DOI: 10.1038/s41467-025-65700-4

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