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

The direct synthesis of cyclic carbonates through oxidative carboxylation of alkenes using CO and O offers a sustainable and carbon-neutral method for CO 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 and O. Remarkably, even using the flue gas as an impure CO and O source, desired cyclic carbonate could be obtained with moderate productivity, which shows the potential for integrated CO capture and conversion, leveraging the high CO 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 and CO, as well as controlling selectivity.