Density functional theory calculations are performed to investigate the hydrodesulfurization (HDS) mechanisms of different sulfur-containing compounds, such as thiophene, benzothiophene, dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) on the brim and CUS sites. Based on the systematic calculations, the dominant reaction pathway of different molecules are explored, and the structure-activity relationship of brim and CUS sites is mainly discussed under the real reaction conditions (p(H2) = 4 MPa, T = 650 K). According to the DFT calculation results, brim site is more favorable for the HDS reactions of thiophene and benzothiophene. However, both brim and CUS sites are considered to participate in the DBT and 4.6-DMDBT HDS processes. The brim site provides the hydrogenation active sites, and the CUS site promotes the removal of sulfur atoms. The proposed mechanism strongly supports that the brim and CUS sites act in synergistic effect for the HDS reaction of the highly refractory organic sulfides.
|Original language||English (US)|
|Journal||Chemical Engineering Science|
|State||Published - Feb 2021|
Bibliographical noteKAUST Repository Item: Exported on 2021-02-09
Acknowledged KAUST grant number(s): OSR-2019-CPF-4103.2
Acknowledgements: This research was supported by the National Natural Science Foundation of China (No. 21878330, 21676298), the Project of National Key R&D Program of China (2019YFC1907700), the CNPC Key Research Project (2016E-0707), and the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under Award (No. OSR-2019-CPF-4103.2)
This publication acknowledges KAUST support, but has no KAUST affiliated authors.