T. Stach, A. Seif, A. Ambrosetti, P. L. Silvestrelli, U. Burghaus
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Enhancing the reactivity of clean, defect-free epitaxial graphene by the substrate—Experiment and theory
Experimental and theoretical evidence is presented that a sulfur compound dissociates on clean, defect-free epitaxial graphene (Gr) in ultrahigh vacuum (UHV). Together with density functional theory calculations (DFT), experimental kinetics and spectroscopic data suggest an auto-(/self)catalytic process. The results could open a pathway to a carbocatalyst. While adsorbing H2S in UHV at low temperatures on single-layer graphene/ruthenium (Gr/Ru), H2 desorbs and sulfur remains on the surface. Vacancy and grain boundary defects, respectively, can be excluded as active sites. DFT results indicate the importance of the Ru(0001) support in facilitating a reaction pathway with small activation energy for H2S dissociation. Gr becomes reactive due to a complex interplay of structural and electronic effects, including the corrugation of the graphene layer and the hybridization of ruthenium's d orbital with antibonding states of H2S.
期刊介绍:
Journal of Vacuum Science & Technology A publishes reports of original research, letters, and review articles that focus on fundamental scientific understanding of interfaces, surfaces, plasmas and thin films and on using this understanding to advance the state-of-the-art in various technological applications.