Stable Janus monolayer MoSHx (0.5 ≤ x ≤ 2)

Abstract

MoSH is a representative example of a Janus two-dimensional monolayered system consisting of a molybdenum atomic layer sandwiched between sulfur and hydrogen atomic layers. Extensive experimental and theoretical efforts have suggested the great promise of the MoSH material, but the validity of the MoSH model (with a Mo–S–H ratio of 1:1:1) remains uncertain. While various experiments have established the Mo-to-S ratio to be close to 1:1, the hydrogen content has remained elusive even with the use of state-of-the-art characterization techniques due to its lightweight nature. In this study, we present a theoretical investigation aiming to determine the positions and ratios of the hydrogen atoms on MoSHx (with x ranging from 0 to 3) as well as assess their structural stability. By evaluating the energetic, mechanical, and thermodynamic properties, we confirm the existence of stable MoSHx structures within a critical range of hydrogen atom ratios, specifically 0.5 ≤ x ≤ 2.0. Additionally, as the hydrogen atom ratio increases, we observe a transition in the preferred adsorption sites of hydrogen atoms from the center of the hexagonal ring composed of molybdenum and sulfur atoms to the upper region of the molybdenum atoms. This study offers critical insight into the structural characteristics and stability of Janus monolayer MoSHx, contributing to the advancement and application of Janus MoSHx in various fields.