Confined Carbon Mediating Dehydroaromatization of Methane over Mo/ZSM-5. / Kosinov, Nikolay; Wijpkema, Alexandra S.G.; Uslamin, Evgeny et al.
In: Angewandte Chemie - International Edition, Vol. 57, No. 4, 22.01.2018, p. 1016-1020.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Confined Carbon Mediating Dehydroaromatization of Methane over Mo/ZSM-5
AU - Kosinov, Nikolay
AU - Wijpkema, Alexandra S.G.
AU - Uslamin, Evgeny
AU - Rohling, Roderigh
AU - Coumans, Ferdy J.A.G.
AU - Mezari, Brahim
AU - Parastaev, Alexander
AU - Poryvaev, Artem S.
AU - Fedin, Matvey V.
AU - Pidko, Evgeny A.
AU - Hensen, Emiel J.M.
N1 - © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
PY - 2018/1/22
Y1 - 2018/1/22
N2 - Non-oxidative dehydroaromatization of methane (MDA) is a promising catalytic process for direct valorization of natural gas to liquid hydrocarbons. The application of this reaction in practical technology is hindered by a lack of understanding about the mechanism and nature of the active sites in benchmark zeolite-based Mo/ZSM-5 catalysts, which precludes the solution of problems such as rapid catalyst deactivation. By applying spectroscopy and microscopy, it is shown that the active centers in Mo/ZSM-5 are partially reduced single-atom Mo sites stabilized by the zeolite framework. By combining a pulse reaction technique with isotope labeling of methane, MDA is shown to be governed by a hydrocarbon pool mechanism in which benzene is derived from secondary reactions of confined polyaromatic carbon species with the initial products of methane activation.
AB - Non-oxidative dehydroaromatization of methane (MDA) is a promising catalytic process for direct valorization of natural gas to liquid hydrocarbons. The application of this reaction in practical technology is hindered by a lack of understanding about the mechanism and nature of the active sites in benchmark zeolite-based Mo/ZSM-5 catalysts, which precludes the solution of problems such as rapid catalyst deactivation. By applying spectroscopy and microscopy, it is shown that the active centers in Mo/ZSM-5 are partially reduced single-atom Mo sites stabilized by the zeolite framework. By combining a pulse reaction technique with isotope labeling of methane, MDA is shown to be governed by a hydrocarbon pool mechanism in which benzene is derived from secondary reactions of confined polyaromatic carbon species with the initial products of methane activation.
KW - dehydroaromatization
KW - hydrocarbons
KW - methane
KW - Mo/ZSM-5
KW - organocatalysis
UR - http://www.scopus.com/inward/record.url?scp=85039059826&partnerID=8YFLogxK
U2 - 10.1002/anie.201711098
DO - 10.1002/anie.201711098
M3 - Article
C2 - 29181863
AN - SCOPUS:85039059826
VL - 57
SP - 1016
EP - 1020
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
IS - 4
ER -
ID: 9265658