Abstract
Polyphenol-derived vitrimers offer compelling prospects for sustainable materials owing to their intrinsic recyclability, reprocessability and biodegradability. However, practical development remains constrained by structure degradation under harsh reprocessing conditions and the need for sophisticated modifications of the bio-sourced precursors. Herein, we reported a strategy that integrates commercially available polyphenols and low-molecular-weight PDMS through adaptable iminoboronate chemistry, obviating the need for structural modifications. The N-B coordination lowers the activation barriers for both imine and boronic ester exchange, enabling efficient bond rearrangement. The resulting vitrimers exhibited excellent reprocessability under relatively mild conditions while retaining excellent creep resistance under typical usage conditions. Furthermore, the dynamic chemical framework supports multiple functionalities, including adhesion performance, Fe(3+)-induced photothermal effects, and anthracene-mediated fluorescence response. Notably, replacing PDMS with a polyurethane matrix yields vitrimers with outstanding mechanical performance (ultimate tensile strength ≈21.4 MPa; elongation at break ≈731%) and enables reprocessing at temperatures as low as 80 °C. This work presents a novel strategy for developing robust and multifunctional vitrimers with mild reprocessing properties, making them suitable for a wide range of practical applications.