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

Lowering the concentration of CO 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 β boron monolayer (V/β-BM), for one-pot CO capture, activation, and efficient conversion into methanol. Our first-principles computations reveal that strong interaction ensures V/β-BM can capture CO at ambient and elevated temperatures. Substantial charge transfer between V/β-BM and CO triggers the activation of CO into anionic CO, which can be efficiently hydrogenated into CHOH with an ultralow limiting potential of 0.54 V and a rather low rate-determining barrier of 1.04 eV. Moreover, the adsorption of HO 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 CO capture, activation, and conversion, which may open a new avenue for recycling CO.