High-Efficiency Construction of CO₂-Based Healable Thermoplastic Elastomers via a Tandem Synthetic Strategy

The alternating copolymerization of CO2/epoxides to polycarbonates (CO2–PCs) has been an area of research focus because of the growing concern about energy and the environment. Regardless of the enormous progress that has been made, the lack of functionalities and inert chemical structure of CO2-based polycarbonates greatly limit the scope of the application in practice. With an aim to develop smart materials with high added-value, herein, the CO2-based thermoplastic elastomers (CO2-TPEs) were first reported. The CO2-TPEs are efficiently constructed in a tandem catalysis process, which includes epoxide hydrolysis reaction, immortal alternating polymerization of carbon dioxide and epoxides, and the thiol–ene click chemistry. The CO2-TPEs exhibit characteristic properties of thermoplastic elastomers with a Young’s modulus up to 10.1 MPa. Moreover, robust self-healing ability could be endowed to the CO2-TPEs via addition of a small amount of boronic ester as dynamic cross-linker. The mechanical properties in...