Computing Surface Reaction Rates by Adaptive Multilevel Splitting Combined with Machine Learning and Molecular Dynamics.

Computing accurate rate constants for catalytic events occurring at the surface of a given material represents a challenging task with multiple potential applications in chemistry. To address this question, we propose an approach based on a combination of the rare event sampling method called adaptive multilevel splitting (AMS) and molecular dynamics. The AMS method requires a one-dimensional reaction coordinate to index the progress of the transition.

MUSIC Speciation of γ-AlO at the Solid Liquid Interface: How DFT Calculations Can Help with Amorphous and Poorly Crystalline Materials.

Transition aluminum oxides, such as γ-AlO or alumina, are widely used in many different technical applications that rely on the surface reactivity of this material at the solid liquid interface. The speciation of surface sites of this material confronts several obstacles. On the one hand, alumina is a poorly crystalline oxide, thus allowing for a limited amount of empirical structural information for an important number of surface sites with different trends in reactivity and, on the other hand, it is a metastable material.

Influence of the hydroxylation of gamma-Al2O3 surfaces on the stability and diffusion of single Pd atoms: a DFT study.

Using recent well-defined models of gamma-Al2O3 surfaces, we study the interaction of single Pd atoms with gamma-Al2O3 surfaces corresponding to realistic pretreatment conditions by means of density functional theory periodic calculations. For relevant hydroxylation states of the surface, we determine potential energy surfaces (PES) that depict the relationship between structure and interaction at the metal-oxide interface. This approach enables the determination of the low-energy diffusion paths of the adsorbed Pd species.