Confined carbon mediating dehydroaromatization of methane over Mo/ZSM-5

N. Kosinov, A.S.G. Wijpkema, E. Uslamin, R. Rohling, F.J.A.G. Coumans, B. Mezari, A. Parastaev, A.S. Poryvaev, M.V. Fedin, E.A. Pidko, E.J.M. Hensen

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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.
Originele taal-2Engels
Pagina's (van-tot)1028–1032
TijdschriftAngewandte Chemie
Volume130
Nummer van het tijdschrift4
DOI's
StatusGepubliceerd - 22 jan 2018

Vingerafdruk

Methane
Carbon
Hydrocarbons
Catalyst deactivation
Labeling
Isotopes
Benzene
Natural gas
Microscopic examination
Chemical activation
Spectroscopy
Atoms
Catalysts
Liquids

Citeer dit

Kosinov, N. ; Wijpkema, A.S.G. ; Uslamin, E. ; Rohling, R. ; Coumans, F.J.A.G. ; Mezari, B. ; Parastaev, A. ; Poryvaev, A.S. ; Fedin, M.V. ; Pidko, E.A. ; Hensen, E.J.M. / Confined carbon mediating dehydroaromatization of methane over Mo/ZSM-5. In: Angewandte Chemie. 2018 ; Vol. 130, Nr. 4. blz. 1028–1032.
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abstract = "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.",
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Confined carbon mediating dehydroaromatization of methane over Mo/ZSM-5. / Kosinov, N.; Wijpkema, A.S.G.; Uslamin, E.; Rohling, R.; Coumans, F.J.A.G.; Mezari, B.; Parastaev, A.; Poryvaev, A.S.; Fedin, M.V.; Pidko, E.A.; Hensen, E.J.M.

In: Angewandte Chemie, Vol. 130, Nr. 4, 22.01.2018, blz. 1028–1032.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

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T1 - Confined carbon mediating dehydroaromatization of methane over Mo/ZSM-5

AU - Kosinov, N.

AU - Wijpkema, A.S.G.

AU - Uslamin, E.

AU - Rohling, R.

AU - Coumans, F.J.A.G.

AU - Mezari, B.

AU - Parastaev, A.

AU - Poryvaev, A.S.

AU - Fedin, M.V.

AU - Pidko, E.A.

AU - Hensen, E.J.M.

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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.

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