Substrate mediated properties of gold monolayers on SiC

Abstract

In light of their unique physicochemical properties two-dimensional metals are of interest in the development of next-generation sustainable sensing and catalytic applications. Here we showcase results of the investigation of the substrate effect on the formation and the catalytic activity of representative 2D gold layers supported by non-graphenized and graphenized SiC substrates. By performing comprehensive density functional theory (DFT) calculations, we revealed the epitaxial alignment of gold monolayer with the underlying SiC substrate, regardless of the presence of zero-layer graphene or epitaxial graphene. This is explained by a strong binding energy (∼4.7 eV) of 2D Au/SiC and a pronounced charge transfer at the interface, which create preconditions for the penetration of the related electric attraction through graphene layers. We then link the changes in catalytic activity of substrate-supported 2D Au layer in hydrogen evolution reaction to the formation of a charge accumulation region above graphenized layers. Gold intercalation beneath zero-layer graphene followed by its transformation to quasi-free-standing epitaxial graphene is found to be an effective approach to tune the interfacial charge transfer and catalytic activity of 2D Au. The sensing potential of substrate-supported 2D Au was also tested through exploring the adsorption behaviour of NH₃, NO₂ and NO gas molecules. The present results can be helpful for the experimental design of substrate-supported 2D Au layers with targeted catalytic activity and sensing performance.