Abstract
The superatomic cluster Au102+ is the smallest known replica of the golden pyramid Au20, and its complex analogues, Au9M2+ (M = Sc-Ni), have exhibited stable and intriguing electronic properties. In this study, we employ density-functional theory (DFT) to investigate the interaction between hydrogen molecules and Au9M2+ clusters. Our DFT calculations reveal that the structures of these clusters are influenced by the dissociative adsorption of H2, but not by the molecular adsorption. By conducting a comprehensive analysis, we show that the preferred adsorption configuration is a result of the competition between various factors, including the surface/encapsulated position, relative electronegativity, and coordination number of atoms. Although Au9M2+-2H (M = Sc, Ti, Mn, and Fe) are remarkably more stable than their corresponding Au9M2+-H2 configurations, different activation energies ranging from 0.15 to 0.99 eV are required during the dissociative reaction pathway. The finding results shed light on the mechanisms underlying the preferred adsorption site of hydrogen on the studied species and provide insights into adsorption kinetics that can aid further theoretical and experimental studies of hydrogenation in nanostructured materials.
Published Version
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