On the dynamic nature of Mo sites for methane dehydroaromatization

The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZ...

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Published in:	Chemical science (Cambridge) Vol. 9; no. 21; pp. 4801 - 4807
Main Authors:	Vollmer, Ina, van der Linden, Bart, Ould-Chikh, Samy, Aguilar-Tapia, Antonio, Yarulina, Irina, Abou-Hamad, Edy, Sneider, Yuri G., Olivos Suarez, Alma I., Hazemann, Jean-Louis, Kapteijn, Freek, Gascon, Jorge
Format:	Journal Article
Language:	English
Published:	England Royal Society of Chemistry 2018 The Royal Society of Chemistry
Subjects:	Benzene Carbon monoxide Carburization (corrosion) Carburizing Catalysis Chemical Sciences Chemistry Coke Coking Methane Molecular chains Molybdenum carbide NMR Nuclear magnetic resonance Refineries
ISSN:	2041-6520, 2041-6539
Online Access:	Get full text
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Abstract	The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear 13 C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo 2 C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane ( 13 CH 4 ). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites.
AbstractList	The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear 13C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo2C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane (13CH4). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites.The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear 13C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo2C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane (13CH4). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites. The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear 13C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo2C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane (13CH4). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites. The dynamic catalytic site on Mo/HZSM-5 for methane dehydroaromatization is formed during the initial phases of the reaction. Labelling experiments show that carbon from the carbidic active site is incorporated into the final products. The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear 13C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo2C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane (13CH4). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites. The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane ( CH ). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites. The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear 13 C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-Mo 2 C nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane ( 13 CH 4 ). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites.
Author	Aguilar-Tapia, Antonio Yarulina, Irina Gascon, Jorge Abou-Hamad, Edy Hazemann, Jean-Louis Kapteijn, Freek Sneider, Yuri G. Olivos Suarez, Alma I. Vollmer, Ina Ould-Chikh, Samy van der Linden, Bart
AuthorAffiliation	a Catalysis Engineering , Chemical Engineering Department , Delft University of Technology , Van der Maasweg 9 , 2629 HZ Delft , The Netherlands . Email: jorge.gascon@kaust.edu.sa e Dipartimento di Ingegneria Chimica Materiali Ambiente , Sapienza Universitá di Roma , Via Eudossiana 18 , 00184 Roma , Italy b King Abdullah University of Science and Technology , KAUST Catalysis Center , Advanced Catalytic Materials , Thuwal 23955 , Saudi Arabia c Inst. Néel , UPR 2940 CNRS – Univ. Grenoble Alpes , F-38000 Grenoble , France d King Abdullah University of Science and Technology , Core Labs , Thuwal 23955 , Saudi Arabia
AuthorAffiliation_xml	– name: c Inst. Néel , UPR 2940 CNRS – Univ. Grenoble Alpes , F-38000 Grenoble , France – name: b King Abdullah University of Science and Technology , KAUST Catalysis Center , Advanced Catalytic Materials , Thuwal 23955 , Saudi Arabia – name: d King Abdullah University of Science and Technology , Core Labs , Thuwal 23955 , Saudi Arabia – name: e Dipartimento di Ingegneria Chimica Materiali Ambiente , Sapienza Universitá di Roma , Via Eudossiana 18 , 00184 Roma , Italy – name: a Catalysis Engineering , Chemical Engineering Department , Delft University of Technology , Van der Maasweg 9 , 2629 HZ Delft , The Netherlands . Email: jorge.gascon@kaust.edu.sa
Author_xml	– sequence: 1 givenname: Ina surname: Vollmer fullname: Vollmer, Ina organization: Catalysis Engineering, Chemical Engineering Department, Delft University of Technology, The Netherlands – sequence: 2 givenname: Bart surname: van der Linden fullname: van der Linden, Bart organization: Catalysis Engineering, Chemical Engineering Department, Delft University of Technology, The Netherlands – sequence: 3 givenname: Samy orcidid: 0000-0002-3486-0944 surname: Ould-Chikh fullname: Ould-Chikh, Samy organization: King Abdullah University of Science and Technology, KAUST Catalysis Center, Advanced Catalytic Materials, Thuwal 23955, Saudi Arabia – sequence: 4 givenname: Antonio surname: Aguilar-Tapia fullname: Aguilar-Tapia, Antonio organization: Inst. Néel, UPR 2940 CNRS – Univ. Grenoble Alpes, F-38000 Grenoble, France – sequence: 5 givenname: Irina orcidid: 0000-0002-9551-4535 surname: Yarulina fullname: Yarulina, Irina organization: Catalysis Engineering, Chemical Engineering Department, Delft University of Technology, The Netherlands, King Abdullah University of Science and Technology – sequence: 6 givenname: Edy surname: Abou-Hamad fullname: Abou-Hamad, Edy organization: King Abdullah University of Science and Technology, Core Labs, Thuwal 23955, Saudi Arabia – sequence: 7 givenname: Yuri G. surname: Sneider fullname: Sneider, Yuri G. organization: Dipartimento di Ingegneria Chimica Materiali Ambiente, Sapienza Universitá di Roma, 00184 Roma, Italy – sequence: 8 givenname: Alma I. surname: Olivos Suarez fullname: Olivos Suarez, Alma I. organization: Catalysis Engineering, Chemical Engineering Department, Delft University of Technology, The Netherlands – sequence: 9 givenname: Jean-Louis surname: Hazemann fullname: Hazemann, Jean-Louis organization: Inst. Néel, UPR 2940 CNRS – Univ. Grenoble Alpes, F-38000 Grenoble, France – sequence: 10 givenname: Freek orcidid: 0000-0003-0575-7953 surname: Kapteijn fullname: Kapteijn, Freek organization: Catalysis Engineering, Chemical Engineering Department, Delft University of Technology, The Netherlands – sequence: 11 givenname: Jorge orcidid: 0000-0001-7558-7123 surname: Gascon fullname: Gascon, Jorge organization: Catalysis Engineering, Chemical Engineering Department, Delft University of Technology, The Netherlands, King Abdullah University of Science and Technology
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Snippet	The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace... The dynamic catalytic site on Mo/HZSM-5 for methane dehydroaromatization is formed during the initial phases of the reaction. Labelling experiments show that...
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SubjectTerms	Benzene Carbon monoxide Carburization (corrosion) Carburizing Catalysis Chemical Sciences Chemistry Coke Coking Methane Molecular chains Molybdenum carbide NMR Nuclear magnetic resonance Refineries
Title	On the dynamic nature of Mo sites for methane dehydroaromatization
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