Unveiling the Effects of Cu Doping on the H2 Activation by Ceo2 Surface Frustrated Lewis Pairs

Abstract

Recently, the solid-state frustrated Lewis pairs (FLPs) based on CeO2 have been demonstrated to effectively catalyze the hydrogenation of unsaturated substrates. Here, the effects of Cu doping on the intrinsic FLPs properties for different facets of CeO2 is investigated by using DFT calculations. The results demonstrate that introducing O vacancies creates FLPs with the ability to efficiently cleavage hydrogen molecules, and to reduce the formation energy of O vacancies. Importantly, Cu exert an influence not only on the intrinsic properties of FLPs but also on the formation of new Ce-O and Cu-O FLPs. Considering the H2 activation, the doping of Cu results in an enhancement for the thermodynamics by decreasing the reaction energies, while a hinderance for the kinetics by increasing the energy barriers. Overall, with these theoretical investigations, we propose certain hints for further studies concerning the Cu doped CeO2 catalysts for H2 activation and hydrogenation reactions.

Keywords: frustrated lewis pairs, CeO2, Density functional theory, h2 activation