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

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.

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 Creators:
Murugappan, Karthick1, Author
Anderson, Eric M.1, Author
Teschner, Detre2, 3, Author              
Jones, Travis2, Author              
Skorupska, Katarzyna2, 3, Author              
Román-Leshkov, Yuriy1, Author
Affiliations:
1Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA, ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Department of Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion, ou_persistent22              

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 Abstract: 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.

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Language(s): eng - English
 Dates: 2017-12-182018-09-252018-11-05
 Publication Status: Published online
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41929-018-0171-9
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Title: Nature Catalysis
  Abbreviation : Nat. Catal.
Source Genre: Journal
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Publ. Info: Nature Publishing Group
Pages: 8 Volume / Issue: 1 (12) Sequence Number: - Start / End Page: 960 - 967 Identifier: ISSN: 25201158
CoNE: https://pure.mpg.de/cone/journals/resource/25201158