Dynamic reaction-induced phase separation in tunable, adaptive covalent networks
Katie M. Herbert, Patrick T. Getty, Neil D. Dolinski, Jerald E. Hertzog, Derek de Jong, James H. Lettow, Joy Romulus, Jonathan W. Onorato, Elizabeth M. Foster, Stuart J. Rowan
Abstract
A series of catalyst-free, room temperature dynamic bonds derived from a reversible thia-Michael reaction are utilized to access mechanically robust dynamic covalent network films. The equilibrium of the thiol addition to benzalcyanoacetate-based Michael-acceptors can be directly tuned by controlling the electron-donating/withdrawing nature of the Michael-acceptor. By modulating the composition of different Michael-acceptors in a dynamic covalent network, a wide range of mechanical properties and thermal responses can be realized. Additionally, the reported systems phase-separate in a process, coined dynamic reaction-induced phase separation (DRIPS), that yields reconfigurable phase morphologies and reprogrammable shape-memory behaviour as highlighted by the heat-induced folding of a predetermined structure.