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  Catalytic activity, water formation, and sintering: Methane activation over Co- and Fe-doped MgO nanocrystals

Niedermaier, M., Schwab, T., Kube, P., Zickler, G. A., Trunschke, A., & Diwald, O. (2020). Catalytic activity, water formation, and sintering: Methane activation over Co- and Fe-doped MgO nanocrystals. The Journal of Chemical Physics, 152(7): 074713. doi:10.1063/1.5138894.

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1.5138894.pdf (Publisher version), 7MB
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 Creators:
Niedermaier, Matthias1, Author
Schwab, Thomas1, Author
Kube, Pierre2, Author              
Zickler, Gregor A.1, Author
Trunschke, Annette2, Author              
Diwald, Oliver1, Author
Affiliations:
1Department of Chemistry and Physics of Materials, Paris-Lodron University Salzburg, Jakob-Haringer-Strasse 2a, A-5020, ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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 Abstract: Microstructure, structure, and compositional homogeneity of metal oxide nanoparticles can change dramatically during catalysis. Considering the different stabilities of cobalt and iron ions in the MgO host lattice [M. Niedermaier et al., J. Phys. Chem. C 123, 25991 (2019)], we employed MgO nanocube powders with or without transition metal admixtures for the oxidative coupling of methane (OCM) reaction to analyze characteristic differences in catalytic activity and sintering behavior. Undoped MgO nanocrystals exhibit the highest C2 selectivity and retain the nanocrystallinity of the starting material after 24 h time on stream. For the Co–Mg–O nanoparticle powder, which exhibits the highest activity and COx selectivity and where OCM-induced coarsening is strongest, we found that the Co2+ ions remain homogeneously distributed over the MgO lattice. Trivalent Fe ions migrate to the surface of Fe–Mg–O nanoparticles where they form a magnesioferrite phase (MgFe2O4) with a characteristic impact on catalytic performance: Fe–Mg–O is initially less selective than MgO despite its lower activity. An increase in C2 selectivity and a decrease in the CO2/CO ratio with time on stream are attributed to the increasing fraction of coarsened particles that become depleted in redox active Fe. Surface water is a by-product of the OCM reaction, favors mass transport across the particle surfaces, and serves as a sintering aid during catalysis. The characteristic changes in size and morphology of MgO, Co-doped, and Fe-doped MgO particles can be consistently explained by activity and C2 selectivity trends. The original morphology of the nanocubes as a starting material for the OCM reaction does not impact the catalytic activity.

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Language(s): eng - English
 Dates: 2019-11-172020-01-242020-02-202020-02-21
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1063/1.5138894
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Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: 10 Volume / Issue: 152 (7) Sequence Number: 074713 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226