Computation-Aided Design of Single-Atom Catalysts for One-Pot CO₂ Capture, Activation, and Conversion

Lowering the concentration of CO2 in atmosphere is a global concern but yet remains one of the most challenging processes in chemistry. Herein, we report a rational design of single-atom catalyst (SAC), namely, vanadium atom supported on newly synthesized β12 boron monolayer (V1/β12-BM), for one-pot CO2 capture, activation, and efficient conversion into methanol. Our first-principles computations reveal that strong interaction ensures V1/β12-BM can capture CO2 at ambient and elevated temperatures. Substantial charge transfer between V1/β12-BM and CO2 triggers the activation of CO2 into anionic CO2–, which can be efficiently hydrogenated into CH3OH with an ultralow limiting potential of 0.54 V and a rather low rate-determining barrier of 1.04 eV. Moreover, the adsorption of H2O molecules can make the reaction intermediates closer to the hydrogen source by the steric hindrance, which plays a key role in lowering the reaction barrier. Our findings present the first SAC for one-pot CO2 capture, activation, and conversion, which may open a new avenue for recycling CO2.