Multiscale design of two-dimensional MoS3 materials and their electrocatalytic performance for CO2 reduction

Abstract

Leveraging the CBD-GM platform developed by our group, this study presents the first theoretical prediction of a novel two-dimensional layered MoS₃ structure. Its thermodynamic, mechanical, and dynamic stabilities are confirmed through cohesive energy, elastic constant, phonon dispersion calculations and ab initio molecular dynamics simulations. Strain engineering reveals a semiconductor-to-metal phase transition under 9.5% tensile strain, significantly enhancing the electrical conductivity. MoS₃ also exhibits high hole mobility (409 cm² V⁻¹ s⁻¹), indicating its potential in highly efficient charge transport for electrocatalysis. Furthermore, systematic evaluation of transition metal single-atom doping identifies Mn_α, Co_α, Ni_α@MoS₃, and Zn_β@MoS₃ as efficient CO₂RR catalysts with strong CO₂ binding and favorable selectivity. This work offers an integrated theoretical framework bridging structure prediction, electronic tuning, and catalytic design.