Binding sites of water molecules on GaN (100) surface: DFT calculations

Recently, preliminary experimental results of solar-to-hydrogen generation by wafer level InGaN nanowires were reported [Z. Mi et al. Nano Lett., 2011, 11 (6), pp 2353-2357]. In the present paper we report a theoretical investigation on the dissociation process of water molecules on wurtzite GaN (100) surface (M-Plane) using the density functional theory (DFT). We calculated the structure and energetic of the water adsorption, reaction barrier energies and pathway for water dissociation. The results suggest that the absorption of H2O is more favorable near Gallium atoms than near Nitrogen atoms and we determined the likely binding sites of water molecules on GaN (100) surface. We also analyzed a model for hydrogen evolution reaction on GaN (100) that involves three steps, where a water molecule first dissociates into a hydrogen atom plus the OH group, followed by the dissociation of the hydroxyl group, and finally the two hydrogen atoms recombine to form molecular hydrogen. For these reactions, the atomic positions and the reaction barriers were determined.

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