Highly efficient hydrodesulfurization driven by an in-situ reconstruction of ammonium/amine intercalated MoS₂...

Hydrodesulfurization (HDS) is a commonly used route for producing clean fuels in modern refinery. Herein, ammonium/amine-intercalated MoS₂ catalysts with various content of 1T phase and S vacancies have been successfully synthesized. Along with the increment of 1T phase and S vacancies of MoS₂, the initial reaction rate of the HDS of dibenzothiophene (DBT) can be improved from 0.09 to 0.55 μmol·g_cat^-1·s^-1, accounting for a remarkable activity compared to the-state-of-the-art catalysts. In a combinatory study via the activity evaluation and catalysts characterization, we found that the intercalation species of MoS₂ played a key role in generating more 1T phase and S vacancies through the 'intercalation-deintercalation' processes, and the hydrogenation and desulfurization of HDS can be significantly promoted by 1T phase and S vacancies on MoS₂, respectively. This study provides a practically meaningful guidance for developing more advanced HDS catalysts by the intercalated MoS₂-derived materials with an in-depth understanding of structure-function relationships.