Phase Engineering of Metastable Transition Metal Dichalcogenides via Ionic Liquid Assisted Synthesis

摘要

Metallic group VIB transition metal dichalcogenides (1T-TMDs) have attracted great interest because of their outstanding performance in electrocatalysis, supercapacitors, batteries, and so on, whereas the strict fabrication conditions and thermodynamical metastability of 1T-TMDs greatly restrict their extensive applications. Therefore, it is significant to obtain stable and high-concentration 1T-TMDs in a simple and large-scale strategy. Herein, we report a facile and large-scale synthesis of high-concentration 1T-TMDs via an ionic liquid (IL) assisted hydrothermal strategy, including 1T-MoS2 (the obtained MoS2 sample was denoted as MoS2-IL), 1T-WS2, 1T-MoSe2, and 1T-WSe2. More importantly, we found that IL can adsorb on the surface of 1T-MoS2, where the steric hindrance, π–π stacking, and hydrogen bonds of ionic liquid collectively induce the formation of the 1T-MoS2. In addition, DFT calculation reveals that electrons are transferred from [BMIM]­SCN (1-butyl-3-methylimidazolium thiocyanate) to 1T-MoS2 layers by hydrogen bonds, which enhances the stability of 1T-MoS2, so the MoS2-IL performs with high stability for 180 days at room temperature without obvious change. Furthermore, the MoS2-IL exhibits excellent HER performance with an overpotential of 196 mV at 10 mA cm–2 in acid conditions.