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

Abstract

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.