First principles studies on the redox ability of (Ga1−xZnx)N1−xOx solid solutions and thermal reactions for H2 and O2 production on their surfaces
Literature Information
Yaojun A. Du, Yun-Wen Chen, Jer-Lai Kuo
The (Ga1−xZnx)N1−xOx solid solution has been emerging as an effective photocatalyst for water splitting utilizing the visible solar spectrum, regarded as a host GaN bulk doped with ZnO impurities. H2 and O2 production occur simultaneously and stoichiometrically on the surface of (Ga1−xZnx)N1−xOx particles. In this work, we characterize the redox ability of (Ga1−xZnx)N1−xOx and find that a solid solution with a ZnO concentration of 0.125 < x < 0.250 is optimal for water splitting. This is consistent with the experimental finding that the maximum photocatalytic activity of (Ga1−xZnx)N1−xOx is achieved at x = 0.13. The thermal reactions of water splitting are modeled on both the GaN and an idealized (Ga1−xZnx)N1−xOx (100) surface. The computed activation barriers allow us to gain some clues on the efficiency of water splitting on a specific photocatalyst surface. Our results suggest that the non-polar (100) and polar (0001) surfaces may play different roles in water splitting, i.e., the (100) surface is responsible for O2 production, while hydroxyl groups could dissociate on the (0001) surface.
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