Dynamic supramolecular hydrogels mediated by chemical reactions

Supramolecular self-assembly in a biological system is usually dominated by sophisticated metabolic processes (chemical reactions) such as catalysis of enzymes and consumption of high energy chemicals, leading to groups of biomolecules with unique dynamics and functions in an aqueous environment. In recent years, increasing efforts have been made to couple chemical reactions to molecular self-assembly, with the aim of creating supramolecular materials with lifelike properties and functions. In this feature article, after summarising the work of chemical reaction mediated supramolecular hydrogels, we first focus on a typical example where dynamic self-assembly of molecular hydrogels is activated by in situ formation of a hydrazone bond in water. We discuss how the formation of the hydrazone-based supramolecular hydrogels can be controlled in time and space. After that, we describe transient assembly of supramolecular hydrogels powered by out-of-equilibrium chemical reaction networks regulated by chemical fuels, which show unique properties such as finite lifetime, dynamic structures, and regenerative capabilities. Finally, we provide a perspective on the future investigations that need to be done urgently, which range from fundamental research to real-life applications of dynamic supramolecular hydrogels.