Hydrogen-bonded Supramolecular Polymeric Materials: From Structure and Performance to Functionality and Application

The huge consumption of polymeric materials in the world has led to a dramatic increase in plastic waste, which has caused pervasive environmental pollution and severe waste of material resources. Crosslinking the polymer segments by noncovalent bonds is an effective method for developing healable, degradable, and recyclable polymeric materials, which could be a fundamental solution to the global plastic waste crisis. However, the noncovalently crosslinked polymeric materials usually exhibit low mechanical robustness, hindering their practical applications. In this feature article, we summarized the recent research progress of our group on hydrogen-bonded supramolecular polymeric materials with high mechanical robustness and various functionalities. Based on the synergistic effect of high-density hydrogen bonds, the cooperation of hydrogen bonds and dynamic covalent bonds, and the regulation of the microstructures of the polymeric materials, we have developed a series of healable, degradable, and recyclable supramolecular polymer materials that simultaneously possess high strength and high toughness. Our results not only break the bottleneck of poor mechanical properties of noncovalently crosslinked polymeric materials, but also reconcile the mutual exclusiveness between the strength and toughness of polymer materials. These studies provide new ideas for the development of the high-performance sustainable alternatives to traditional polymer materials. Moreover, we have developed a series of hydrogen-bonded functional supramolecular polymeric materials, and their applications in flexible electronic devices, solid-state lithium batteries, and underwater adhesives are also introduced in this feature article. [GRAPHICS] .