Yan Tianlan, Jia Yingshuai, Hou Kaige, Gui Zhuxin, Zhang Wenbiao, Du Ke, Pan Di, Li He, Shi Yanghao, Qi Lu, Gao Qingsheng, Zhang Yahong, Tang Yi
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.
iScience. 2024 Apr 26;27(6):109824. doi: 10.1016/j.isci.2024.109824. eCollection 2024 Jun 21.
Hydrodesulfurization (HDS) is a commonly used route for producing clean fuels in modern refinery. Herein, ammonium/amine-intercalated MoS 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 MoS, the initial reaction rate of the HDS of dibenzothiophene (DBT) can be improved from 0.09 to 0.55 μmol·g·s, 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 MoS 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 MoS, respectively. This study provides a practically meaningful guidance for developing more advanced HDS catalysts by the intercalated MoS-derived materials with an in-depth understanding of structure-function relationships.
加氢脱硫（HDS）是现代炼油厂生产清洁燃料常用的工艺路线。在此，成功合成了具有不同1T相含量和硫空位的铵/胺插层MoS催化剂。随着MoS中1T相和硫空位的增加，二苯并噻吩（DBT）加氢脱硫的初始反应速率可从0.09提高到0.55 μmol·g·s，与目前最先进的催化剂相比，具有显著的活性。通过活性评价和催化剂表征的组合研究，我们发现MoS的插层物种通过“插层-脱插层”过程在生成更多1T相和硫空位方面起关键作用，并且MoS上的1T相和硫空位分别可显著促进HDS的加氢和脱硫。该研究为通过插层MoS衍生材料深入理解结构-功能关系来开发更先进的HDS催化剂提供了具有实际意义的指导。
