Silyl Ether as a Robust and Thermally Stable Dynamic Covalent Motif for Malleable Polymer Design

Here we introduce silyl ether linkage as a novel dynamic covalent motif for dynamic material design. Through introduction of a neighboring amino moiety, we show that the silyl ether exchange rate can be accelerated by almost three orders of magnitude. By incorporating such silyl ether linkages into covalently cross-linked polymer networks, we demonstrate dynamic covalent network polymers displaying both malleability and reprocessability. The malleability of the networks is studied by monitoring stress relaxation at varying temperature, and their topology freezing temperatures are determined. The tunable dynamic properties coupled with the high thermal stability and reprocessability of silyl ether-based networks open doors to many potential applications for this family of materials.