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arXiv · 1811.10379

Influence of surface restructuring on the activity of SrTiO3 photoelectrodes for photocatalytic hydrogen reduction

Yihuang Xiong·Ismaila Dabo
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Abstract

Perovskite photoelectrodes are being extensively studied in search for photocatalytic materials that can produce hydrogen through water splitting. The solar-to-hydrogen efficiency of these materials is critically dependent on the electrochemical state of their surface. Here, we develop an embedded quantum-mechanical approach using the self-consistent continuum solvation (SCCS) model to predict the relation between band alignment, electrochemical stability, and photocatalytic activity taking into account the long-range polarization of the semiconductor electrode under electrical bias. Using this comprehensive model, we calculate the charge-voltage response of various reconstructions of a solvated SrTiO3 surface, revealing that interfacial charge trapping exerts primary control on the electrical response and surface stability of the photoelectrode. Our results provide a detailed molecular-level interpretation of the enhanced photocatalytic activity of SrTiO3 upon voltage-induced restructuring of the semiconductor-solution interface.

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Yihuang Xiong, Ismaila Dabo. 2018-10-16. Influence of surface restructuring on the activity of SrTiO3 photoelectrodes for photocatalytic hydrogen reduction. https://doi.org/10.1103/physrevmaterials.3.065801

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