Multiscale Design of Two-Dimensional MoS 3 Materials and Their Electrocatalytic Performance for CO 2 Reduction

Abstract

Leveraging the self-developed CBD-GM platform, this study presents the first theoretical prediction of a novel two-dimensional layered MoS 3 structure. Its thermodynamic, mechanical, and dynamic stability is confirmed through cohesive energy, elastic constants, phonon dispersion, and ab initio molecular dynamics simulations. Strain engineering reveals a semiconductor-to-metal phase transition under 9.5% tensile strain, significantly enhancing electrical conductivity. MoS 3 also exhibits strong visible-light absorption and high hole mobility (409 cm²•V⁻¹•s⁻¹), indicating its potential in next-generation flexible optoelectronic devices. Furthermore, systematic evaluation of transition metal single-atom doping identifies Mn S1 , Co S1 , Ni S1 @MoS 3 , and Zn S2 @MoS 3 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.