Recyclable thermoplastic silicone elastomers from non-carbon heteroatomic polymer backbones.

Abstract

Silicone materials are indispensable across industrial and consumer domains, yet their robust Si-O-Si backbones resist depolymerization and typically require chemical crosslinking to attain elastomeric properties. Here we report a modular synthesis to access non-carbon heteroatomic backbone polymers (PTeSiO) featuring periodic Si-O-Te-O linkages. This copolymerization merges Si-O and Te-O as building blocks, enabling a one-pot, room-temperature aqueous route to high-molecular-weight, transparent elastomers with precise control over backbone composition and side-chain architecture. Main-chain engineering via redox-labile Te-O motifs enables chemoselective backbone scission under mild reductive conditions, affording on-demand polymerization-depolymerization cycles with efficient monomer recovery. The semi-flexible backbones and chain entanglement impart elasticity, thermoplastic processability, and side-chain-dependent mechanical performance. This work establishes a modular and general chemical strategy for creating non-carbon heteroatomic backbones as a design principle for sustainable and recyclable silicone materials.