Theoretical Insights on the Synergistic Effect of Dual Metal Sites Supported on MgO(100) Promoting the Hydrogenation Reaction

Abstract

Designing heterogeneous catalysts with dual-functional sites for hydrogenation reactions holds significant potential for improving activity and selectivity. We present catalysts that incorporate two distinct metal sites onto a MgO support, serving as adsorption sites for reactant and H₂, respectively. From screening 16 candidates using density functional theory calculations, we identified Pt₁Al₁/MgO as a promising catalyst for nitroaromatic hydrogenation. The Al–Mg moiety adsorbs 3-nitrostyrene via its nitro group, while the neighboring Pt–O facilitates H₂ dissociation through transient frustrated Lewis pairs. The synergistic effect of the Al–O–Pt moiety enhances reaction activity, driven by the appropriate adsorption/desorption of *H at the Pt site and a low diffusion barrier. This study offers valuable insights into the design of transient frustrated Lewis pair catalysts and is pivotal for the development of heterogeneous catalysts with dual-sites for hydrogenation reactions.