Construction of Autonomic Self-Healing CO2-Based Polycarbonates via One-Pot Tandem Synthetic Strategy

The coupling of epoxides and carbon dioxide to polycarbonates (CO 2 –PCs) has been the subject of intense research for nearly half a century. Although tremendous progress has been achieved, their aliphatic characteristics and lack of functionalities of CO 2 –PCs limit the scope of their application in high value-added and functional materials. In this article, the first CO 2 -based polycarbonate with the ability to autonomously self-heal is constructed via a one-pot synthetic strategy. The key to the success of the synthetic strategy is efficient tandem three different catalytic reactions, i.e., hydrolysis of epoxides, immortal copolymerization of CO 2 /epoxides, and thiol–ene click reactions in a one-pot process. Based on the standard tensile testing, these CO 2 -based materials show robust self-healing properties, where the extensibility, maximal strength, and Young’s modulus of the specimens can almost entirely recover to their original value under ambient temperature. Our studies demonstrate that the self-healing capability of these CO 2 -based materials arises both from the homo -hydrogen bonding (between amide groups) and the hetero -hydrogen bonding (between amide group and carbonate group of polycarbonate backbone). The convenient and atom economic synthesis strategy, combined with the impressive self-healing capability for these materials, should expand the library of high value-added CO 2 -based polycarbonates and the scope of their applications.