Liu Xiao-He, He Yi, Li Zhi, Cheng Ai-Hua, Song Zhiqi, Yu Zhi-Xuan, Chai Shouning, Cheng Cheng, He Chi
Department of Environmental Engineering, College of Geology and Environment, Xi'an University of Science and Technology, Xi'an 710054, China; Department of Environmental Science and Engineering, State Key Laboratory of Multiphase Flow in Power Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.
Department of Environmental Engineering, College of Geology and Environment, Xi'an University of Science and Technology, Xi'an 710054, China.
J Colloid Interface Sci. 2023 Dec;651:368-375. doi: 10.1016/j.jcis.2023.08.001. Epub 2023 Aug 2.
Recently, atomically precise metal nanoclusters (NCs) become a new class of photosensitizer for light energy conversion in metal-cluster-sensitized semiconductor (MCSS) system. However, fundamental understanding for the suitable combination of NCs and semiconductor is still unclear. Aside from aspects of light harvesting, energy level alignment and catalytic activity, interfacial interaction behavior at NCs/semiconductor interface is also crucial due to its important influence in charge transportation. In this work, the interface interaction between Au NCs and TiO is examined by precise transformation of Au NCs from Au(SG) to Au(SG), as well as its effect on photocatalytic hydrogen production activity. From the optical, charge transport and solid-states spectroscopy analyses, it is able to display that precisely tuning the number of core atoms from Au(SG) to Au(SG) results in the strong interface interaction between Au NCs and TiO, reflecting in high difference of work function and modified surface band bending of TiO, therefore promoting the injection of electrons from NCs to TiO and reducing interfacial charges recombination. As a result, Au(SG)/TiO shows higher hydrogen generation rate than Au(SG)/TiO under light irradiation. This work would provide new insights into rational combination of metal NCs with semiconductor and highlights the overlooked effect of interfacial interaction behavior on light energy conversion.
最近，原子精确的金属纳米团簇（NCs）成为金属团簇敏化半导体（MCSS）系统中用于光能转换的一类新型光敏剂。然而，对于NCs与半导体的合适组合的基本理解仍不明确。除了光捕获、能级匹配和催化活性等方面外，NCs/半导体界面处的界面相互作用行为因其对电荷传输的重要影响也至关重要。在这项工作中，通过将Au NCs从Au(SG)精确转变为Au(SG)来研究Au NCs与TiO之间的界面相互作用，以及其对光催化产氢活性的影响。通过光学、电荷传输和固态光谱分析，能够表明将核心原子数从Au(SG)精确调整到Au(SG)会导致Au NCs与TiO之间产生强烈的界面相互作用，这体现在功函数的高度差异和TiO改性的表面能带弯曲上，从而促进电子从NCs注入到TiO并减少界面电荷复合。结果，在光照下，Au(SG)/TiO比Au(SG)/TiO表现出更高的产氢速率。这项工作将为金属NCs与半导体的合理组合提供新的见解，并突出界面相互作用行为对光能转换的被忽视的影响。
