Publication date: 15th May 2025
Molybdenum disulfide (MoS2), a transition metal dichalcogenide (TMD) material, is a popular example of a non-noble metal catalyst with tunable nanoscale properties. MoS2 is unique in that its edges are highly active catalyst sites, but its basal plane is entirely inert, requiring activation to become catalytic. Doping with transition metal atoms, such as cobalt (Co), is one method of enhancing its catalytic properties, particularly by activating the basal plane. However, the location and influence of these dopant atoms on resultant catalyst behavior is poorly understood. To fill this knowledge gap, we systematically studied the influence of dopants in MoS2 on catalytic hydrogenolysis reactions. We approach this problem through a well-controlled, ligand-directed, tunable doping method to create homogeneously doped and size-controlled colloidal MoS2 nanosheets. X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations revealed the non-monotonous relationship between Co dopant concentration, location, and activity in two model reactions, hydrodesulfurization (HDS) and hydrodeoxygenation (HDO). In these reactions, it was determined that mole ratio concentrations of 21% to 25% Co:Mo, respectively, performed the best. This observation stems due to the saturation of active MoS2 edges with Co below this critical concentration, at which point basal plane activation begins. While Co prefers to dope the edges over basal sites, basal Co atoms are demonstrably more catalytically active than edge Co atoms. We also determined that the addition of Zr dopants can boost the catalytic performance of the Co-MoS2 system albeit by imparting strain on the MoS2 lattice and enhancing the edge Co site activity. These findings provide insight into the hydrogenolysis behavior of doped TMDs and can be extended to other TMD materials for future catalyst application development.
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