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Nat Commun. 2019 Mar 11;10(1):1164. doi: 10.1038/s41467-019-09130-z.

Thermodynamically stable whilst kinetically labile coordination bonds lead to strong and tough self-healing polymers.

Author information

1
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, People's Republic of China.
2
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, People's Republic of China. chli@nju.edu.cn.
3
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing National Laboratory of Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, People's Republic of China. zuojl@nju.edu.cn.
4
Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA. zbao@stanford.edu.

Abstract

There is often a trade-off between mechanical properties (modulus and toughness) and dynamic self-healing. Here we report the design and synthesis of a polymer containing thermodynamically stable whilst kinetically labile coordination complex to address this conundrum. The Zn-Hbimcp (Hbimcp = 2,6-bis((imino)methyl)-4-chlorophenol) coordination bond used in this work has a relatively large association constant (2.2 × 1011) but also undergoes fast and reversible intra- and inter-molecular ligand exchange processes. The as-prepared Zn(Hbimcp)2-PDMS polymer is highly stretchable (up to 2400% strain) with a high toughness of 29.3 MJ m-3, and can autonomously self-heal at room temperature. Control experiments showed that the optimal combination of its bond strength and bond dynamics is responsible for the material's mechanical toughness and self-healing property. This molecular design concept points out a promising direction for the preparation of self-healing polymers with excellent mechanical properties. We further show this type of polymer can be potentially used as energy absorbing material.

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