Search

The high electrical conductivity of 1T′-WTe2deserves particular attention and may show a high potential for hydrogen evolution reaction (HER) catalysis. However, the actual activity certainly does not match expectations, and the inferior HER activity is actually still ambiguous at the atomic level. Unraveling the underlying HER behaviors of 1T′-WTe2will give rise to a new family of HER catalysts. Our structural analysis reveals that the inferior activity could result from insufficient charge density around the Te site and blocked adsorption channel at the W site, which cause too weak hydrogen adsorption. Herein, we fabricated a single WTe2sheet-based electrocatalytic microdevice for directly extracting enhanced HER activity of doped electronegative F atoms. The overpotential at –10 mA cm–2reduced to 0.27 V after F doping compared to 0.45 V for the original state. In situ electrochemical measurement and electrical tests on a single sheet indicate that doped F can regulate surface charge and hydrogen adsorption behavior. Furthermore, the theory simulation uncovers that the smaller atomic radius of F contributes to an empty coordination environment; meanwhile, strong electronegativity induces hydrogen adsorption. Thus, the ΔGH*at W sites around the doped F is as low as 0.18 eV. Synergistically modulating the charge properties and opening steric hindrance provides a new pathway to rationally construct electrocatalysts and beyond.

Recent discovery of intrinsic ferromagnetism in Fe3GeTe2(FGT) monolayer [Deng, Y.; Nature2018, 563, 94−99; Fei, Z.; Nat. Mater.2018, 17, 778–782] not only extended the family of two-dimensional (2D) magnetic materials but also stimulated further interest in the possibility to tune their magnetic properties without changing the chemical composition or introducing defects. By means of density functional theory computations, we explore strain effects on the magnetic properties of the FGT monolayer. We demonstrate that the ferromagnetism can be largely enhanced by the tensile strain in the FGT monolayer due to the competitive effects of direct exchange and superexchange interaction. The average magnetic moments of Fe atoms increase monotonically with an increase in biaxial strain from −5 to 5% in FGT monolayer. The intriguing variation of magnetic moments with strain in the FGT monolayer is related to the charge transfer induced by the changes in the bond lengths. Given the successful fabrication of the FGT monolayer, the strain-tunable ferromagnetism in the FGT monolayer can stimulate the experimental effort in this field. This work also suggests an effective route to control the magnetic properties of the FGT monolayer. The pronounced magnetic response toward the biaxial strain can be used to design the magnetomechanical coupling spintronics devices based on FGT.