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Layer-structure adjustable MoS2 catalysts for the slurry-phase hydrogenation of polycyclic aromatic hydrocarbons
Slurry-phase hydrogenation technology is the frontier topic in the efficient conversion of heavy oils into light fractions around the world. Developing highly active dispersed MoS 2 catalysts is the major obstacle to realize the industrial application of upgrading heavy oils. In this work, both top-down ball-milling method and bottom-up hydrothermal method were designed to synthesize MoS 2 catalysts with controllable layer structures. The stacking layers and lateral sizes for micro-scaled MoS 2 catalysts by ball-milling method can be reduced to their limits and stabilize at 6 ∼ 8 layers and lateral size of ca. 30 nm. The more flexible bottom-up hydrothermal method can construct MoS 2 catalysts with much smaller lateral sizes and fewer stacking layers, especially, MoS 2 catalyst fabricated with ammonium tetrathiomolybdate as Mo and S precursor possesses average stacking layers of 2 and lateral size of 5 ∼ 10 nm. Polycyclic aromatic hydrocarbons anthracene, phenanthrene and naphthalene were used as model compounds of heavy oils to investigate the catalytic hydrogenation performance of designed MoS 2 catalysts. The catalytic activities of MoS 2 catalysts can be well correlated with their stacking layers and lateral size. The edges of top and bottom S-Mo-S atomic layers for MoS 2 sheets, named rim sites, are positively correlated with the exposure of active sites for catalytic hydrogenation of PAHs. The highest catalytic activity of MoS 2 catalyst results from its layer structures of 100% rim sites and the smallest lateral size of 5 ∼ 10 nm, which is beneficial to expose maximum active sites for catalytic hydrogenation reactions. This work can guide us to design the highly active hydrogenation catalysts, and promote the industrial application of upgrading heavy oils.