Exploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane
Kurlov, Alexey (ETH Zürich. Department of Mechanical and Process Engineering)
Deeva, Evgeniya B. (ETH Zürich. Department of Mechanical and Process Engineering)
Abdala, Paula M. (ETH Zürich. Department of Mechanical and Process Engineering)
Lebedev, Dmitry (ETH Zürich. Department of Chemistry and Applied Biosciences)
Tsoukalou, Athanasia (ETH Zürich. Department of Mechanical and Process Engineering)
Comas-Vives, Aleix (Universitat Autònoma de Barcelona. Departament de Química)
Fedorov, Alexey (ETH Zürich. Department of Mechanical and Process Engineering)
Müller, Christoph R. (ETH Zürich. Department of Mechanical and Process Engineering)

Date:	2020
Abstract:	The two-dimensional morphology of molybdenum oxycarbide (2D-Mo2COx) nanosheets dispersed on silica is found vital for imparting high stability and catalytic activity in the dry reforming of methane. Here we report that owing to the maximized metal utilization, the specific activity of 2D-Mo2COx/SiO2 exceeds that of other Mo2C catalysts by ca. 3 orders of magnitude. 2D-Mo2COx is activated by CO2, yielding a surface oxygen coverage that is optimal for its catalytic performance and a Mo oxidation state of ca. +4. According to ab initio calculations, the DRM proceeds on Mo sites of the oxycarbide nanosheet with an oxygen coverage of 0. 67 monolayer. Methane activation is the rate-limiting step, while the activation of CO2 and the C-O coupling to form CO are low energy steps. The deactivation of 2D-Mo2COx/SiO2 under DRM conditions can be avoided by tuning the contact time, thereby preventing unfavourable oxygen surface coverages.
Grants:	Agencia Estatal de Investigación PGC2018-100818-A-I00 Ministerio de Educación y Ciencia RyC-2016-19930
Rights:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Language:	Anglès
Document:	Article ; recerca ; Versió publicada
Subject:	Chemical engineering ; Natural gas ; Two-dimensional materials
Published in:	Nature communications, Vol. 11 (October 2020) , art. 4920, ISSN 2041-1723

DOI: 10.1038/s41467-020-18721-0
PMID: 33009379

11 p, 1.4 MB

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