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

Abstract

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 Co_3.6%–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 ^cCo_3.6%–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.