Simultaneously Tuning the Defects and Surface Properties of Ta₃N₅ Nanoparticles by Mg-Zr Codoping for Significantly...

The simultaneous control of the defect species and surface properties of semiconducting materials is a crucial aspect of improving photocatalytic performance, yet it remains challenging. Here, we synthesized Mg-Zr-codoped single-crystalline Ta₃N₅ (Ta₃N₅:Mg+Zr) nanoparticles by a brief NH₃ nitridation process, exhibiting photocatalytic water reduction activity 45 times greater than that of pristine Ta₃N₅ under visible light. A coherent picture of the relations between the defect species (comprising reduced Ta, nitrogen vacancies and oxygen impurities), surface properties (associated with dispersion of the Pt cocatalyst), charge carrier dynamics, and photocatalytic activities was drawn. The tuning of defects and simultaneous optimization of surface properties resulting from the codoping evidently resulted in the generation of high concentrations of long-lived electrons in this material as well as the efficient migration of these electrons to evenly distributed surface Pt sites. These effects greatly enhanced the photocatalytic activity. This work highlights the importance and feasibility of improving multiple properties of a catalytic material via a one-step strategy.