Theoretical calculation of single-atom supported BN catalyzing CO2 hydrogenation to formic acid: A first principles study

Abstract

Exploring suitable catalysts for CO₂ hydrogenation is crucial to alleviate greenhouse effect and produce useful chemicals. In this work, the potential of a single transition metal atom embedded in a boron nitride monolayer (TM-BN) as a catalyst for CO₂ hydrogenation to formic acid was evaluated using first-principles calculations. The TM-BN systems (TM = Sc, Ti, V, Cr and Mn) exhibit significant stability due to the strongly interaction between the TM-3d orbitals and the 2p orbitals of the three surrounding N atoms. While, only V-BN system shows the strongest adsorption energies of CO₂ and H₂ than others. Four mechanisms were proposed for CO₂ hydrogenation to formic acid, where the process including CO₂ absorbed on V-BN monolayer in side-on type as initial state has the lowest energy barriers of 0.44 eV. This work not only provides a new way for CO₂ hydrogenation but also further broadens the range of applications for BN-based materials.