Dual Co Single Atom Doping and CO In Situ Regulation Cooperatively Stimulate the Basal Plane of Co–MoS2 with Boosted Hydrodesulfurization Activity

Realizing MoS2 basal plane activation is highly desirable and challenging in the field of hydrodesulfurization (HDS). Herein, we have developed a new strategy of dual Co single atom doping (SAD) combined with CO in situ regulation, which can successfully activate the basal plane of Co3.6%–MoS2-0.3 generating high ratios of thermostable 1T-plane (∼70%) and large S vacancies. For the first time, a synergistic effect has been unraveled where the lattice substituted neighboring dual SA Co can efficiently activate in-plane S through extensively reducing its band gap (2.21 → 0.14 eV), which tremendously favors S subtraction and 2H → 1T phase transition assisted by CO. Boosted thiophene HDS activity can be eventually achieved with the reaction rate constant (k) being 8.3 times higher than that of commercial cCo3.6%–MoS2 (0.04 → 0.33 h–1). Generally, the present work paves a new way for next-generation HDS catalyst design with activated basal plane.