Defective ZrO2-x supported Ru nanoparticles as a Mott-Schottky photocatalyst for efficient ammonia synthesis under ambient conditions

GREEN CHEMISTRY(2023)

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摘要
Well-crafted semiconductors exhibiting favorable band structures and strong electron-donating properties can provide a viable pathway for solar-driven nitrogen activation under ambient conditions. In this study, we demonstrate that the nitrogen photo-fixation process can be enhanced by introducing oxygen vacancies and a Ru co-catalyst. The Ru-loaded ZrO2-x photocatalyst achieved an impressive NH3 production rate of 3256 mu g g(-1) h(-1) under visible light irradiation (at 400 nm). Defective ZrO2-x with its enhanced reducing ability and narrow band gap possesses a low work function and excellent electron-donating capability, resulting in remarkable photocatalytic performance for ammonia synthesis under visible light. The supported Ru co-catalyst induces upward band bending in defective ZrO2-x, forming an interfacial Schottky barrier that facilitates the separation of photogenerated charge carriers and provides energetic electrons for nitrogen activation. Mott-Schottky photocatalysts with enhanced back donation ability establish a one-way channel for the transmission of photoexcited electrons, thereby further improving the photocatalytic performance of ammonia synthesis at room temperature.
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