Abstract

Defect sites on oxide semiconductors play a crucial role in promoting photocatalytiperformance and modulating the bandgap structure of photocatalysts. However, the role of interfacial coordinatively unsaturated defect sites between metal and oxide in photocatalysis is still under debate. So, we designed an experiment to probe the role of interfacial coordinatively unsaturated defect sites. In this work, a series of Ti/TiO2 photocatalysts with varying concentrations of interfacial Ti3+ sites were prepared through an epitaxial growth method under hydrothermal conditions. Through experimental and computational investigations, the roles of interfacial defect sites were discussed in detail. On the one hand, the interfacial coordinatively unsaturated Ti3+ sites could act as visible-light-responsive sites in photocatalytic reactions due to the overlap and hybridization of multiple electronic orbitals. On the other hand, the Ti/TiO2 interface exhibited a certain degree of metallic character near the Fermi level because of the partial delocalization and redistribution of electrons, facilitating the charge migration and separation across the metal-oxide interface. Consequently, the obtained Ti/TiO2 catalysts showed notably enhanced charge transfer efficiency and visible light photocatalytic activity compared to their pristine counterparts. This work may provide a new perspective to interfacial defect engineering in classic metal/oxide heterojunction photocatalysts and figure a more precise direction to synthesize higher effective photocatalysts for environmental governance.

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