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

The alternating copolymerization of CO 2 /epoxides to polycarbonates (CO 2 –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 CO 2 -based polycarbonates greatly limit the scope of the application in practice. With an aim to develop smart materials with high added-value, herein, the CO 2 -based thermoplastic elastomers (CO 2 -TPEs) were first reported. The CO 2 -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 CO 2 -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 CO 2 -TPEs via addition of a small amount of boronic ester as dynamic cross-linker. The mechanical properties including the Young’s modulus, maximal strength, and extensibility of the CO 2 -TPE materials can be nearly completely recovered without any extra stimulus at room temperature.