Lattice-distorted lithiation behavior of a square phase Janus MoSSe monolayer for electrode applications

Janus transition metal dichalcogenides with unique physical properties have recently attracted increasing research interest for their energy and catalytic applications. In this paper, we investigate the lithiation behavior of a square phase Janus MoSSe monolayer (1S-MoSSe) using first-principles calculations. Computational results show that a single Li atom energetically prefers to adsorb on the central site of the octagonal ring (O site) and on the S-layer side of 1S-MoSSe. The predicted energy barriers for Li diffusion are surface dependent and in the range of 0.33 to 0.51 eV, indicating the acceptable Li migration kinetics on 1S-MoSSe in comparison with other 2D TMD materials. Further thermodynamic analysis demonstrates that Li adsorption on 1S-MoSSe is energetically stable up to a Li concentration of x = 1.0, above which the lithiation process becomes unstable with a negative charging potential. Phonon calculations also confirm that Li adsorption (0.25 ≤ x ≤ 0.75) results in the lattice distortion of 1S-MoSSe in order to suppress the structural instability of the lithiated monolayer 1S-LixMoSSe with imaginary phonon frequencies. The less symmetric nature of 1S-MoSSe is believed to destabilize Li adsorption at much smaller x than 1H-MoSSe does, regardless of the higher dipole moment of 1S-MoSSe. This computational study provides a fundamental understanding of the electrochemical performance of 1S-MoSSe, as well as useful insight into the material design of Janus TMD anodes for Li-ion batteries.