College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, PR China.
Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE. College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, PR China.
J Colloid Interface Sci. 2023 Jul 15;642:669-679. doi: 10.1016/j.jcis.2023.03.199. Epub 2023 Apr 3.
Artificial manipulation of charge separation and transfer are central issues dominating hydrogen evolution reaction triggered via photocatalysis. Herein, through elaborate designing on the architecture, band alignment, and interface bonding mode, a sulfur vacancy-rich ZnInS-based (Vs-ZIS) multivariate heterostructure ZnInS/MoSe/InSe (Vs-ZIS/MoSe/InSe) with specific Janus Z-scheme charge transfer mechanism is constructed through a two-step hydrothermal process. Steering by the Janus Z-scheme charge transfer mechanism, photogenerated electrons in the conduction band of MoSe transfer synchronously to the valence band of Vs-ZIS and InSe, resulting in abundant highly-active photogenerated electrons reserved in the conduction band of Vs-ZIS and InSe, therefore significantly enhancing the photocatalytic activity of hydrogen evolution. Under visible light irradiation, the optimized Vs-ZIS/MoSe/InSe with the mass ratio of MoSe and InSe to ZnInS at 3 % and 30 %, respectively, performs a high hydrogen evolution rate of 124.42 mmol·g·h, about 43.5-folds of the original ZIS photocatalyst. Besides, an apparent quantum efficiency (AQE) of 22.5 % at 420 nm and favorable durability are also achieved over Vs-ZIS/MoSe/InSe photocatalyst. This work represents an important development in efficient photocatalysts and donates a sound foundation for the design of regulating charge transfer pathways.
人工操纵电荷分离和转移是通过光催化触发的析氢反应的核心问题。在此,通过精心设计结构、能带排列和界面键合方式,通过两步水热法构建了具有特定的单原子层范德瓦尔斯肖特基结电荷转移机制的富硫空位的 ZnInS 基(Vs-ZIS)多元异质结 ZnInS/MoSe/InSe(Vs-ZIS/MoSe/InSe)。在单原子层范德瓦尔斯肖特基结电荷转移机制的引导下,MoSe 导带中的光生电子同步转移到 Vs-ZIS 和 InSe 的价带,导致大量高活性的光生电子保留在 Vs-ZIS 和 InSe 的导带中,从而显著提高了析氢的光催化活性。在可见光照射下,优化后的 MoSe 和 InSe 与 ZnInS 的质量比分别为 3%和 30%的 Vs-ZIS/MoSe/InSe 表现出 124.42 mmol·g·h 的高析氢速率,约为原始 ZIS 光催化剂的 43.5 倍。此外,在 Vs-ZIS/MoSe/InSe 光催化剂上还实现了 420nm 时 22.5%的明显量子效率(AQE)和良好的耐久性。这项工作代表了高效光催化剂的重要发展,为调节电荷转移途径的设计提供了坚实的基础。