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.