Exploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane

Alexey Kurlov, Evgeniya B. Deeva, Paula M. Abdala, Dmitry Lebedev, Athanasia Tsoukalou, Aleix Comas-Vives (), Alexey Fedorov () and Christoph R. Müller ()
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Alexey Kurlov: ETH Zürich
Evgeniya B. Deeva: ETH Zürich
Paula M. Abdala: ETH Zürich
Dmitry Lebedev: ETH Zürich
Athanasia Tsoukalou: ETH Zürich
Aleix Comas-Vives: Universitat Autònoma de Barcelona
Alexey Fedorov: ETH Zürich
Christoph R. Müller: ETH Zürich

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-18721-0

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