Abstract In the hydrodenitrogenation reaction, metals such as Fe, Co, and Ni are frequently incorporated as promoters into the MoS 2 catalyst. Exploring the reasons for the differences in catalytic activity within multi‐metal catalysts is crucial for designing novel hydrodenitrogenation catalysts. Herein, first‐principles calculations were used to analyze the action mechanism of NiMoS, CoMoS, and FeMoS catalysts in the hydrodenitrogenation of carbazole. The findings demonstrate that the smaller number of outer‐layer electron holes of Ni atoms results in a weaker binding force on S atoms, thereby facilitating the formation of reactive sites. Meanwhile, the NiMoS catalyst exhibits the highest hydrogenation activity for carbazole and intermediates, attributable to the electronic properties of the Ni atom surface, followed by CoMoS, and FeMoS shows the lowest activity. In addition, the S‐edge of all catalysts exhibited higher hydrogenation activity compared to the Mo‐edge. It is noteworthy that the FeMoS catalyst demonstrates the highest CN bond cleavage activity, a consequence of the strong interaction between Fe atoms and H β . Furthermore, as carbazole undergoes hydrogenation to form dodecahydrocarbazole, the increase in steric hindrance substantially impedes the CN bond cleavage, particularly the E2 elimination process.
Wei et al. (Thu,) studied this question.