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Operando NAP-XPS unveils differences in MoO3 and Mo2C during hydrodeoxygenation

MPG-Autoren
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Teschner,  Detre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion;

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Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Skorupska,  Katarzyna
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion;

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Zitation

Murugappan, K., Anderson, E. M., Teschner, D., Jones, T., Skorupska, K., & Román-Leshkov, Y. (2018). Operando NAP-XPS unveils differences in MoO3 and Mo2C during hydrodeoxygenation. Nature Catalysis, 1(12), 960-967. doi:10.1038/s41929-018-0171-9.


Zitierlink: https://hdl.handle.net/21.11116/0000-0002-CAB2-1
Zusammenfassung
MoO3 and Mo2C have emerged as remarkable catalysts for the selective hydrodeoxygenation (HDO) of a wide range of oxygenates at low temperatures (that is, ≤673 K) and H2 pressures (that is, ≤1 bar). Although both catalysts can selectively cleave C–O bonds, the nature of their active sites remains unclear. Here we used operando near-ambient pressure X-ray photoelectron spectroscopy to reveal important differences in the Mo 3d oxidation states between the two catalysts during the hydrodeoxygenation of anisole. This technique revealed that, although both catalysts featured a surface oxycarbidic phase, the oxygen content and the underlying phase of the material impacted the reactivity and product selectivity during the hydrodeoxygenation. MoO3 transitioned between 5+ and 6+ oxidation states during the operation, consistent with an oxygen-vacancy driven mechanism wherein the oxygenate is activated at undercoordinated Mo sites. In contrast, Mo2C showed negligible oxidation state changes during hydrodeoxygenation and maintained mostly 2+ states throughout the reaction.