Block Poly(carbonate-ester) Ionomers as High-Performance and Recyclable Thermoplastic Elastomers.

Thermoplastic elastomers based on polyesters/carbonates have the potential to maximize recyclability, degradability and renewable resource use. However, they often underperform and suffer from the familiar trade-off between strength and extensibility. Herein, we report well-defined reprocessable poly(ester-b-carbonate-b-ester) elastomers with impressive tensile strengths (60 MPa), elasticity (>800 %) and recovery (95 %). Plus, the ester/carbonate linkages are fully degradable and enable chemical recycling. The superior performances are attributed to three features: (1) Highly entangled soft segments; (2) Fully reversible strain-induced crystallization and (3) Precisely placed Zn -carboxylates dynamically crosslinking the hard domains. The one-pot synthesis couples controlled cyclic monomer ring-opening polymerization and alternating epoxide/anhydride ring-opening copolymerization. Efficient convresion to ionomers is achieved by reacting vinyl-epoxides to install Zn -carboxylates.