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用于高效光催化产氢的面内二维/二维异质共催化剂的电荷自调节

Charge self-regulation over in-plane two-dimensional/two-dimensional hetero-cocatalyst for robust photocatalytic hydrogen generation.

作者信息

Xu Jiachao, Zhang Xidong, Wang Xuefei, Wu Xinhe, Yu Huogen

机构信息

State Key Laboratory of Silicate Materials for Architectures and School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, PR China.

Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, 68 Jincheng Street, Wuhan, 430078, PR China.

出版信息

J Colloid Interface Sci. 2024 Dec;675:592-601. doi: 10.1016/j.jcis.2024.07.034. Epub 2024 Jul 6.

Abstract

The rationally designing and constructing atomic-level heterointerface of two-dimensional (2D) chalcogenides is highly desirable to overcome the sluggish HO-activation process toward efficient solar-driven hydrogen evolution. Herein, a novel in-plane 2D/2D molybdenum disulfide-rhenium disulfide (ReS-MoS) heterostructure is well-designed to induce the charge self-regulation of active site by forming electron-enriched Re and electron-deficient S sites, thus collectively facilitating the activation of adsorbed HO molecules and its subsequent H evolution. Furthermore, the obtained in-plane heterogenous ReS-MoS nanosheet can powerfully transfer photoexcited electrons to inhibit photocarrier recombination as observed by advanced Kelvin probe measurement (KPFM), in-situ X-ray photoelectron spectroscopy (XPS) and femtosecond transient absorption spectroscopy (fs-TAS). As expected, the obtained ReS-MoS/TiO photocatalyst achieves an outperformed H-generation rate of 6878.3 μmol h g with visualizing H bubbles in alkaline/neutral conditions. This work about in-plane 2D/2D heterostructure with strong free-electron interaction provides a promising strategy for designing novel and efficient catalysts for various applications.

摘要

合理设计和构建二维(2D)硫族化物的原子级异质界面对于克服缓慢的氢氧根(HO)活化过程以实现高效的太阳能驱动析氢非常必要。在此,一种新型的面内二维/二维二硫化钼-二硫化铼(ReS-MoS)异质结构被精心设计,通过形成富电子的铼(Re)和缺电子的硫(S)位点来诱导活性位点的电荷自调节,从而共同促进吸附的HO分子的活化及其随后的析氢反应。此外,通过先进的开尔文探针测量(KPFM)、原位X射线光电子能谱(XPS)和飞秒瞬态吸收光谱(fs-TAS)观察到,所获得的面内异质ReS-MoS纳米片能够有效地转移光激发电子以抑制光载流子复合。正如预期的那样,所获得的ReS-MoS/TiO光催化剂在碱性/中性条件下可视化氢气泡时,实现了6878.3 μmol h g的优异析氢速率。这项关于具有强自由电子相互作用的面内二维/二维异质结构的工作为设计用于各种应用的新型高效催化剂提供了一种有前景的策略。

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