Aerobic Oxidative Carboxylation of Styrene Over Cobalt Catalysts: Integrated CO 2 Capture and Conversion.

The direct synthesis of cyclic carbonates through oxidative carboxylation of alkenes using CO 2 and O 2 offers a sustainable and carbon-neutral method for CO 2 utilization, which is, however, still a largely unexplored field. Here we develop a single-atom catalyst (SAC) Co-N/O-C as the earth-abundant metal catalyst for the oxidative carboxylation of styrene with CO 2 and O 2 . Remarkably, even using the flue gas as an impure CO 2 and O 2 source, desired cyclic carbonate could be obtained with moderate productivity, which shows the potential for integrated CO 2 capture and conversion, leveraging the high CO 2 adsorption capacity of Co-N/O-C. In addition, the catalyst can be reused five times without an obvious decline in activity. Detailed characterizations and theoretical calculations elucidate the crucial role of single Co atoms in activating O 2 and CO 2 , as well as controlling selectivity.