Programmable liquid crystal elastomers with dynamic covalent siloxane bonds based on a dual self-catalytic strategy

The exchange reaction of preparing the siloxane-based liquid crystal elastomers (Si-LCEs) always require the acid or base catalysts, which will increase the complexity of the operation and reduces the stability of the Si-LCE materials. In this paper, a novel and simple dual self-catalytic strategy for producing Si-LCEs with dynamic covalent siloxane bonds was proposed. A readily available compound-1,3-bis (aminopropyl) tetramethyldisiloxane (BATS) acts as chain extender and crosslinker for elastomers and provides dynamic covalent bonds (DCBs) as well. More importantly, amino groups of BATS play the role of dual self-catalyst, not only accelerating the thiol Michael addition reaction and aza Michael addition reaction simultaneously during producing Si-LCEs, but also promoting dynamic covalent siloxane bonds exchange reaction at an elevated temperature after the formation of the cross-linked network. With this ingenious design, the obtained fully cured polydomain Si-LCEs possess excellent self-healing and processing abilities enabled by DCBs and outstanding mechanical properties facilitated by hydrogen bond, which can be easily aligned, programmed and recycled. By exploiting these dynamic features, a series of multi-functional soft actuators were realized by simple welding, showing a local fast response and precise control by light and heat. Furthermore, soft robots fabricated with a bilayer structure of Si-LCEs can perform crawling and coiling actuation controlled by near-infrared (NIR) light facilely. These results manifest that the self-catalytic dynamic covalent siloxane bonds strategy is a facile and effective approach for preparing Si-LCEs and provides a new solution for the exploitation of multi-functional liquid crystal elastomers with fast response to various stimulus.