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-carbonateb- 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(II)-carboxylates dynamically crosslinking the hard domains. The one-pot synthesis couples controlled cyclic monomer ring-opening polymerization and alternating epoxide/anhydride ring-opening copolymerization. Easy conversion to ionomers is achieved using vinyl-substituted epoxides with phthalic anhydride