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  Crystallographic Orientation Dependence of Surface Segregation and Alloying on PdCu Catalysts for CO2 Hydrogenation

Pielsticker, L., Zegkinoglou, I., Han, Z.-K., Navarro, J. J., Kunze, S., Karslıoğlu, O., et al. (2021). Crystallographic Orientation Dependence of Surface Segregation and Alloying on PdCu Catalysts for CO2 Hydrogenation. The Journal of Physical Chemistry Letters, 12(10), 2570-2575. doi:10.1021/acs.jpclett.1c00179.

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2021_Pielsticker_JPhysChemLett.pdf (Publisher version), 4MB
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 Creators:
Pielsticker, Lukas1, Author
Zegkinoglou, Ioannis1, Author
Han, Zhong-Kang2, Author
Navarro, Juan Jesus3, Author              
Kunze, Sebastian3, Author              
Karslıoğlu, Osman3, Author              
Levchenko, Sergey V.2, Author
Roldan Cuenya, Beatriz3, Author              
Affiliations:
1Faculty of Physics and Astronomy, Ruhr University Bochum, 44780 Bochum, Germany, ou_persistent22              
2Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Moscow 121205, Russia, ou_persistent22              
3Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Abstract: The influence of the crystallographic orientation on surface segregation and alloy formation in model PdCu methanol synthesis catalysts was investigated in situ using near-ambient pressure X-ray photoelectron spectroscopy under CO2 hydrogenation conditions. Combined with scanning tunneling microscopy and density functional theory calculations, the study showed that submonolayers of Pd undergo spontaneous alloy formation on Cu(110) and Cu(100) surfaces in vacuum, whereas they do not form an alloy on Cu(111). Upon heating in H2, inward diffusion of Pd into the Cu lattice is favored, facilitating alloying on all Cu surfaces. Under CO2 hydrogenation reaction conditions, the alloying trend becomes stronger, promoted by the reaction intermediate HCOO*, especially on Pd/Cu(110). This work demonstrates that surface alloying may be a key factor in the enhancement of the catalytic activity of PdCu catalysts as compared to their monometallic counterparts. Furthermore, it sheds light on the hydrogen activation mechanism during catalytic hydrogenation on copper-based catalysts.

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Language(s): eng - English
 Dates: 2021-01-182021-02-242021-03-09
 Publication Status: Published online
 Pages: 6
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpclett.1c00179
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: The Journal of Physical Chemistry Letters
  Abbreviation : J. Phys. Chem. Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 6 Volume / Issue: 12 (10) Sequence Number: - Start / End Page: 2570 - 2575 Identifier: ISSN: 1948-7185
CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185