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Molybdenum Speciation and its Impact on Catalytic Activity during Methane Dehydroaromatization in Zeolite ZSM-5 as Revealed by Operando X-Ray Methods

Lezcano-González, I; Oord, R; Rovezzi, M; Glatzel, P; Botchway, SW; Weckhuysen, BM; Beale, AM; (2016) Molybdenum Speciation and its Impact on Catalytic Activity during Methane Dehydroaromatization in Zeolite ZSM-5 as Revealed by Operando X-Ray Methods. Angewandte Chemie , 55 (17) pp. 5215-5219. 10.1002/anie.201601357. Green open access

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Abstract

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 Mo species on zeolite ZSM-5 during methane dehydroaromatization. The results show that isolated Mo-oxo species present after calcination are converted by CH4 into metastable MoCx Oy species, which are primarily responsible for C2 Hx /C3 Hx 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.

Type: Article
Title: Molybdenum Speciation and its Impact on Catalytic Activity during Methane Dehydroaromatization in Zeolite ZSM-5 as Revealed by Operando X-Ray Methods
Location: Germany
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/anie.201601357
Publisher version: http://dx.doi.org/10.1002/anie.201601357
Language: English
Additional information: © 2016 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
Keywords: X-ray techniques, heterogeneous catalysis, methane, molybdenum, zeolites
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/1493390
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