Abstract：
The rationally designing and constructing atomic-level heterointerface of two-dimensional (2D) chalcogenides is highly desirable to overcome the sluggish H2O-activation process toward efficient solar-driven hydrogen evolution. Herein, a novel in-plane 2D/2D molybdenum disulfide-rhenium disulfide (ReS2-MoS2) heterostructure is well-designed to induce the charge self-regulation of active site by forming electron-enriched Re(4-δ)+ and electron-deficient S(2-δ)- sites, thus collectively facilitating the activation of adsorbed H2O molecules and its subsequent H2 evolution. Furthermore, the obtained in-plane heterogenous ReS2-MoS2 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 ReS2-MoS2/TiO2 photocatalyst achieves an outperformed H2-generation rate of 6878.3 μmol h-1 g-1 with visualizing H2 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：
非常需要合理地设计和构建二维（2D）硫属化物的原子级异质界面，以克服缓慢的H2O活化过程，以实现有效的太阳能驱动的氢析出。在这里，一种新型的平面内2D/2D二硫化钼-二硫化铼（ReS2-MoS2）异质结构经过精心设计，可通过形成富含电子的Re（4-δ）和电子-缺陷的S（2-δ）位点来诱导活性位点的电荷自我调节。从而共同促进吸附的H2O分子的活化及其随后的H2析出。此外，通过先进的开尔文探针测量（KPFM）观察到，获得的平面内异质ReS2-MoS2纳米片可以有力地转移光激发电子以抑制光载流子复合，原位X射线光电子能谱（XPS）和飞秒瞬态吸收光谱（fs-TAS）。不出所料,获得的ReS2-MoS2/TiO2光催化剂在碱性/中性条件下可视化H2气泡时，H2的产生速率优于6878.3μmolh-1g-1。这项关于具有强自由电子相互作用的平面内2D/2D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有希望的策略。
