Bio‐Based Vitrimeric Silicone Materials with High‐Strength, Reprocessable, Healing, and Transparent Properties

Abstract Developing reprocessable polymeric materials from earth‐abundant elements and renewable biomass is attractive for dealing with fossil resource crisis and achieving sustainable development. Based on the unique reactivity of biomass‐derived gluconolactone, polydimethylsiloxane (PDMS) terminated with glucosamide groups is synthesized and used for preparing a series of silicone boronic ester based vitrimers. The whole preparation process is quite straightforward without any purification required and highly efficient with water as the only byproduct. The mechanical properties of obtained vitrimers can be precisely controlled by adjusting the content of 1,4‐benzenediboronic acid or the molecular weight of PDMS precursor, producing boronic ester based vitrimers ranging from soft elastomers to rigid plastics. The obtained vitrimers exhibit excellent thermal stability, robust reprocessability, and efficient healing capacity. By encapsulating green‐emitting CsPbBr 3 nanocrystals, these materials are fabricated into hydrophobic, transparent, and luminescent coatings, promising for applications in flexible optical devices.