Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 12, Issue 7, Pages 2278-2288Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00083k
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Funding
- National Natural Science Foundation of China [22078227, 22108145]
- State Key Laboratory of Heavy Oil Processing [SKLOP201902005]
- Shandong Province Natural Science Foundation [ZR2020QB189]
- Science and Technology Support Program (Social Development) of Taizhou [SSF20210021]
- Research Foundation for Talented Scholars of Taizhou University [QD2016007, QD2016012]
- Qing Lan Project of Jiangsu Province
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In this study, a Co4Mo12 crystalline material was isolated from an impregnating solution using a self-assembly strategy. This crystalline Co4Mo12 was then used as a molecular platform to understand the sulfidation process in the construction of a high-performance Co-Mo hydrodesulfurization catalyst. The results show that the crystalline Co4Mo12 precursor can serve as an excellent precursor for the rational design and controllable preparation of HDS active sites.
In this work, a Co tetra-capped Keggin crystalline Co4Mo12 was separated from the impregnating solution through a self-assembly strategy. The crystalline Co4Mo12 was structurally characterized and used as a molecular platform to reveal the sulfidation procedure of the precursor in the construction of a superior Co-Mo hydrodesulfurization (HDS) catalyst. The higher HDS reactivity of the sulfide can be attributed to the structure-directing effects of the crystalline Co4Mo12 precursor. During the sulfidation procedure of the crystalline Co4Mo12 precursor, it initially decomposes at 100 degrees C and MoOxSy is produced due to the simple O-S exchange. With the temperature increasing to 180 degrees C, the Keggin-type structure in crystalline Co4Mo12 begins to collapse and four groups of edge-shared CoMo2O(S)(13) triplets are formed. As the temperature continues to increase, the CoMo2O(S)(13) triplets collapse and MoS2 is formed due to the deep O-S exchange at 200 degrees C. In this procedure, the water molecules serving as ligands can retard the sulfidation of Co promoters, which can guarantee Co-promoter interaction and re-dispersion at the edges of MoS2 nanoparticles to form the type II CoMoS active phase with higher performance. These results suggest that the crystalline Co4Mo12 precursor can be a superior precursor for the rational design and controllable preparation of HDS active sites.
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