Initial Carbon−Carbon Bond Formation during the Early Stages of Methane Dehydroaromatization
Name:
Illuminating_anie.202007283.pdf
Size:
884.5Kb
Format:
PDF
Description:
Accepted manuscript
Type
ArticleAuthors
Caglayan, MustafaPaioni, Alessandra Lucini
Abou-Hamad, Edy
Shterk, Genrikh

Pustovarenko, Alexey
Baldus, Marc
Chowdhury, Abhishek Dutta

Gascon, Jorge

KAUST Department
Chemical Engineering ProgramChemical Science
Imaging and Characterization Core Lab
KAUST Catalysis Center (KCC)
NMR
Physical Science and Engineering (PSE) Division
Date
2020-07-20Online Publication Date
2020-07-20Print Publication Date
2020-09-14Embargo End Date
2021-06-11Submitted Date
2020-05-20Permanent link to this record
http://hdl.handle.net/10754/663540
Metadata
Show full item recordAbstract
Methane 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.Citation
Çağlayan, 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.202007283Sponsors
Funding 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).Publisher
WileyJournal
Angewandte ChemiePubMed ID
32521078Additional Links
https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202007283ae974a485f413a2113503eed53cd6c53
10.1002/anie.202007283
Scopus Count
Related articles
- Dual Active Sites on Molybdenum/ZSM-5 Catalyst for Methane Dehydroaromatization: Insights from Solid-State NMR Spectroscopy.
- Authors: Gao W, Qi G, Wang Q, Wang W, Li S, Hung I, Gan Z, Xu J, Deng F
- Issue date: 2021 May 3
- Confined Carbon Mediating Dehydroaromatization of Methane over Mo/ZSM-5.
- Authors: Kosinov N, Wijpkema ASG, Uslamin E, Rohling R, Coumans FJAG, Mezari B, Parastaev A, Poryvaev AS, Fedin MV, Pidko EA, Hensen EJM
- Issue date: 2018 Jan 22
- Reversible Nature of Coke Formation on Mo/ZSM-5 Methane Dehydroaromatization Catalysts.
- Authors: Kosinov N, Uslamin EA, Meng L, Parastaev A, Liu Y, Hensen EJM
- Issue date: 2019 May 20
- Reactivity of C1 surface species formed in methane activation on Zn-modified H-ZSM-5 zeolite.
- Authors: Wu JF, Wang WD, Xu J, Deng F, Wang W
- Issue date: 2010 Dec 17
- Methane dehydroaromatization over Mo-modified H-MFI for gas to liquid catalysts.
- Authors: Aritani H, Shibasaki H, Orihara H, Nakahira A
- Issue date: 2009