Initial Carbon−Carbon Bond Formation during the Early Stages of Methane Dehydroaromatization
Paioni, Alessandra Lucini
Chowdhury, Abhishek Dutta
KAUST DepartmentChemical Engineering Program
Imaging and Characterization Core Lab
KAUST Catalysis Center (KCC)
Physical Science and Engineering (PSE) Division
Online Publication Date2020-07-20
Print Publication Date2020-09-14
Embargo End Date2021-06-11
Permanent link to this recordhttp://hdl.handle.net/10754/663540
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AbstractMethane dehydroaromatization (MDA) is among the most challenging processes in catalysis science owing to the inherent harsh reaction conditions and fast catalyst deactivation. To improve this process, understanding the mechanism of the initial C−C bond formation is essential. However, consensus about the actual reaction mechanism is still to be achieved. In this work, using advanced magic-angle spinning (MAS) solid-state NMR spectroscopy, we study in detail the early stages of the reaction over a well-dispersed Mo/H-ZSM-5 catalyst. Simultaneous detection of acetylene (i.e., presumably the direct C−C bond-forming product from methane), methylidene, allenes, acetal, and surface-formate species, along with the typical olefinic/aromatic species, allow us to conclude the existence of at least two independent C−H activation pathways. Moreover, this study emphasizes the significance of mobility-dependent host–guest chemistry between an inorganic zeolite and its trapped organic species during heterogeneous catalysis.
CitationÇağlayan, M., Paioni, A. L., Abou-Hamad, E., Shterk, G., Pustovarenko, A., Baldus, M., … Gascon, J. (2020). Initial Carbon-Carbon Bond Formation during the Early Stages of Methane Dehydroaromatization. Angewandte Chemie International Edition. doi:10.1002/anie.202007283
SponsorsFunding for this work was provided by King Abdullah University of Science and Technology (KAUST). ADC also thanks the starting grant support from IAS, Wuhan University. ALP was supported by a TOPPUNT grant (no. 718.015.001) to M.B. from Netherlands Organization of Scientific Research (NWO).
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