期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 17, 页码 5215-5219出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201601357
关键词
heterogeneous catalysis; methane; molybdenum; X-ray techniques; zeolites
资金
- EPSRC
- NWO (TOP NWO-CW Grant)
- EPSRC [EP/K007467/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/K007467/1] Funding Source: researchfish
Combined high-resolution fluorescence detection X-ray absorption near-edge spectroscopy, X-ray diffraction, and X-ray emission spectroscopy have been employed under operando conditions to obtain detailed new insight into the nature of the Mospecies on zeolite ZSM-5 during methane dehydroaromatization. The results show that isolated Mo-oxo species present after calcination are converted by CH4 into metastable MoCxOy species, which are primarily responsible for C2Hx/C3Hx formation. Further carburization leads to MoC3 clusters, whose presence coincides with benzene formation. Both sintering of MoC3 and accumulation of large hydrocarbons on the external surface, evidenced by fluorescence-lifetime imaging microscopy, are principally responsible for the decrease in catalytic performance. These results show the importance of controlling Mo speciation to achieve the desired product formation, which has important implications for realizing the impact of CH4 as a source for platform chemicals.
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