Predicting the Structure of MoS ₃ and Designing Transition-Metal-Doped Catalysts for Efficient CO ₂ Electroreduction

The development of efficient and highly selective catalysts for the electrochemical CO2 reduction reaction (CO2RR) is crucial for achieving carbon neutrality and sustainable energy cycles. In this study, the stable structure of the MoS3 monolayer was determined using the crystal structure prediction software CBD-GM. Owing to its distinct sulfur coordination environments and large dipole moment, MoS3 serves as an ideal support for single-atom catalysts. By doping transition metals at specific sulfur sites (S1–S3), we systematically screened a series of single-atom configurations for CO2 activation. The results demonstrate that CO2 molecules are effectively activated when Sc, Mn, Fe, Co, and Ni single atoms are doped at the S2 site. Remarkably, CoS2@MoS3 and NiS2@MoS3 are demonstrated as highly effective catalysts for selective CO2-to-CH4 conversion, with low limiting potentials of −0.17 and −0.49 V, respectively. This study provides theoretical insights into the rational design of MoS3-based single-atom systems for efficient and selective CO2 electroreduction.