Aerobic Oxidative Carboxylation of Styrene Over Cobalt Catalysts: Integrated CO₂ Capture and Conversion

The direct synthesis of cyclic carbonates through oxidative carboxylation of alkenes using CO₂ and O₂ offers a sustainable and carbon-neutral method for CO₂ 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 CO₂ and O₂. Remarkably, even using the flue gas as an impure CO₂ and O₂ source, desired cyclic carbonate could be obtained with moderate productivity, which shows the potential for integrated CO₂ capture and conversion, leveraging the high CO₂ 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 O₂ and CO₂, as well as controlling selectivity.