Highly efficient hydrodesulfurization driven by an in-situ reconstruction of ammonium/amine intercalated MoS2 catalysts
Tianlan Yan,
Yingshuai Jia,
Kaige Hou,
Zhuxin Gui,
Wenbiao Zhang,
Ke Du,
Di Pan,
He Li,
Yanghao Shi,
Lu Qi,
Qingsheng Gao,
Yahong Zhang,
Yi Tang
Affiliations
Tianlan Yan
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Yingshuai Jia
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Kaige Hou
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Zhuxin Gui
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Wenbiao Zhang
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China; College of Chemistry and Materials Science, and, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, P.R. China
Ke Du
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Di Pan
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
He Li
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Yanghao Shi
College of Chemistry and Materials Science, and, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, P.R. China
Lu Qi
School of Petrochemical Engineering, and, Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Changzhou University, Changzhou, Jiangsu 213164, P.R. China
Qingsheng Gao
College of Chemistry and Materials Science, and, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou 510632, P.R. China; Corresponding author
Yahong Zhang
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China
Yi Tang
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, P.R. China; Corresponding author
Summary: 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·gcat−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.
