Dynamic reaction-induced phase separation in tunable, adaptive covalent networks

Herbert, Katie M.; Getty, Patrick T.; Dolinski, Neil D.; Hertzog, Jerald E.; de Jong, Derek; Lettow, James H.; Romulus, Joy; Onorato, Jonathan W.; Foster, Elizabeth M.; Rowan, Stuart J.

doi:10.1039/d0sc00605j

DOE OSTI · 1772914

Dynamic reaction-induced phase separation in tunable, adaptive covalent networks

Herbert, Katie M.·Getty, Patrick T.·Dolinski, Neil D.·Hertzog, Jerald E.·de Jong, Derek·Lettow, James H.·Romulus, Joy·Onorato, Jonathan W.·Foster, Elizabeth M.·Rowan, Stuart J.

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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.

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Herbert, Katie M., Getty, Patrick T., Dolinski, Neil D., Hertzog, Jerald E., de Jong, Derek, Lettow, James H., Romulus, Joy, Onorato, Jonathan W., Foster, Elizabeth M., Rowan, Stuart J.. 2020-05-01. Dynamic reaction-induced phase separation in tunable, adaptive covalent networks. https://doi.org/10.1039/d0sc00605j

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