Ultrafine Co-MoS2 monolayer catalyst derived from oil-soluble single-molecule polyoxometalates for slurry phase hydrocracking

Herein, a novel single-molecule confinement-sulfurization strategy was proposed to construct ultrafine Co-MoS2 monolayer catalysts by using oil-soluble single-molecule polyoxometalates (POMs), (DODA)(6)Co2Mo10, as precursors. Well-defined Co2Mo10 -POM, acting as molecular pre-assembling platform, is introduced for the atomically precise construction of bimetallic sites. Highly efficient conversion of VR under severe condition is realized with (DODA)(6)Co2Mo10. The origin of prominent catalytic performance can be attributed to the in-situ formation of ultrafine single-layered Mo-based nanosheets with abundant exposed CoMoS active sites. By combining synchrotron radiation-based X-ray absorption spectroscopy and density functional theory calculations, we further discover that there is clearly intimate interaction between Mo and Co atoms and the dissociation of molecular hydrogen at CoMoS phases is energetically preferred, leading to remarkable hydrogenation and coke suppression activity. This work highlights an idea on the rational design and targeted synthesis of ultrafine bimetallic catalysts for slurry phase HCK with dramatically synergistic catalysis.