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

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.