光催化
纳米颗粒
氧气
析氧
材料科学
化学工程
氢
纳米技术
光化学
化学
催化作用
物理化学
有机化学
电极
电化学
工程类
作者
Xu Yao,Kaiwei Liu,Jifang Zhang,Boyang Zhang,Jiaming Zhang,Ke Shi,Haifeng Wang,Guijun Ma
标识
DOI:10.1016/j.jechem.2024.02.051
摘要
Oxynitride semiconductors are promising photocatalyst materials for visible light-driven water splitting, while the synthesis of well crystalized oxynitride still remains challenge. In present work, narrow-bandgap TaON nanoparticles are synthesized via heating a vacuum-sealed mixture of KTaO3, Ta and NH4Cl. This method possesses multiple advantages in terms of lower calcination parameter, higher N conversion efficiency and superior photocatalytic activity in comparison with the traditional thermal ammonolysis using NH3 gas as a nitrogen source. Through the analysis of intermediates produced upon the elevation of heating temperature, a gas-solid-phase reaction between TaCl5 and Ta2O5 is demonstrated as the final step, which is conducive to decreasing thermal energy barrier and accelerating nitridation process. Precise control of preparation conditions, including calcination temperature and duration, allows for the regulation of surface O/N ratio of TaON particles to unity, resulting in optimized photocatalytic activity. Photoelectrochemical assessment and intensity modulated photocurrent spectroscopy provide convincing evidence for improved charge transfer efficiency of photoexcited holes at TaON surface. A Z-scheme overall water splitting is accomplished by employing the TaON as an effective oxygen evolution photocatalyst, SrTiO3:Rh as a hydrogen evolution photocatalyst, and reduced graphene oxide (rGO) as a solid-state electron mediator. This work presents a promising strategy for the synthesis of high-quality oxynitride materials in application to photocatalytic water splitting.
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