期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 17, 页码 9301-9305出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202015769
关键词
EPR spectroscopy; hydrogenation; molybdenum sulfide clusters; transition metal sulfides; zeolites
资金
- Chevron Energy Technology Company
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences (Transdisciplinary Approaches to Realize Novel Catalytic Pathways) [FWP 47319]
- DOE Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL)
- Leibniz Supercomputing Center
- Projekt DEAL
Supercages of FAU-type zeolites provide a robust scaffold for stabilizing molybdenum sulfide clusters, leading to stable catalytic activity for ethene hydrogenation. The Mo4S4 clusters trapped within the FAU structure have a distorted cubane structure similar to the FeMo-cofactor in nitrogenase, and both clusters exhibit identical catalytic activity per sulfide cluster. Additionally, these FAU-encaged clusters show superior stability compared to layered MoS2 structures under the same reaction conditions.
Supercages of faujasite (FAU)-type zeolites serve as a robust scaffold for stabilizing dinuclear (Mo2S4) and tetranuclear (Mo4S4) molybdenum sulfide clusters. The FAU-encaged Mo4S4 clusters have a distorted cubane structure similar to the FeMo-cofactor in nitrogenase. Both clusters possess unpaired electrons on Mo atoms. Additionally, they show identical catalytic activity per sulfide cluster. Their catalytic activity is stable (>150 h) for ethene hydrogenation, while layered MoS2 structures deactivate significantly under the same reaction conditions.
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