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
Embargo End Date2021-06-11
Permanent link to this recordhttp://hdl.handle.net/10754/663540
MetadataShow full item record
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).
- 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
- Structure and Evolution of Confined Carbon Species during Methane Dehydroaromatization over Mo/ZSM-5.
- Authors: Kosinov N, Uslamin EA, Coumans FJAG, Wijpkema ASG, Rohling RY, Hensen EJM
- Issue date: 2018 Sep 7