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  Carbide-Modified Pd on ZrO2 as Active Phase for CO2-Reforming of Methane—A Model Phase Boundary Approach

Köpfle, N., Ploner, K., Lackner, P., Götsch, T., Thurner, C., Carbonio, E., et al. (2020). Carbide-Modified Pd on ZrO2 as Active Phase for CO2-Reforming of Methane—A Model Phase Boundary Approach. Catalysts, 10(9): 1000. doi:10.3390/catal10091000.

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 Creators:
Köpfle, Norbert1, Author
Ploner, Kevin1, Author
Lackner, Peter2, Author
Götsch, Thomas1, 3, Author              
Thurner, Cristoph1, Author
Carbonio, Emilia3, 4, Author              
Hävecker, Michael3, 5, Author              
Knop-Gericke, Axel3, 5, Author              
Schlicker, Lukas6, Author
Doran, Andrew7, Author
Kober, Delf6, Author
Gurlo, Aleksander6, Author
Willinger, Marc8, Author
Penner, Simon1, Author
Schmid, Michael2, Author
Klötzer, Bernhard1, Author
Affiliations:
1Institute of Physical Chemistry, University of Innsbruck, Innrain 52 c, A-6020 Innsbruck, Austria, ou_persistent22              
2Institute of Applied Physics, TU Wien, Wiedner, Hauptstr. 8-10/134, 1040 Wien, Austria, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
4Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, BESSY II, Albert-Einstein-Straße 15, D-10623 Berlin, Germany, ou_persistent22              
5Max Planck Institute for Chemical Energy Conversion, Department of Heterogeneous Reactions, Stiftstraße 34-36, D-45470 Mülheim an der Ruhr, Germany, ou_persistent22              
6Institut für Werkstoffwissenschaften und -technologien, Fachgebiet Keramische Werkstoffe, Technische Universität Berlin, D-10623 Berlin, Germany, ou_persistent22              
7Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA, ou_persistent22              
8Scientific Center for Optical and Electron Microscopy, ScopeM, ETH Zürich, 8093 Zürich, Switzerland, ou_persistent22              

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 Abstract: Starting from subsurface Zr0-doped “inverse” Pd and bulk-intermetallic Pd0Zr0 model catalyst precursors, we investigated the dry reforming reaction of methane (DRM) using synchrotron-based near ambient pressure in-situ X-ray photoelectron spectroscopy (NAP-XPS), in-situ X-ray diffraction and catalytic testing in an ultrahigh-vacuum-compatible recirculating batch reactor cell. Both intermetallic precursors develop a Pd0–ZrO2 phase boundary under realistic DRM conditions, whereby the oxidative segregation of ZrO2 from bulk intermetallic PdxZry leads to a highly active composite layer of carbide-modified Pd0 metal nanoparticles in contact with tetragonal ZrO2. This active state exhibits reaction rates exceeding those of a conventional supported Pd–ZrO2 reference catalyst and its high activity is unambiguously linked to the fast conversion of the highly reactive carbidic/dissolved C-species inside Pd0 toward CO at the Pd/ZrO2 phase boundary, which serves the role of providing efficient CO2 activation sites. In contrast, the near-surface intermetallic precursor decomposes toward ZrO2 islands at the surface of a quasi-infinite Pd0 metal bulk. Strongly delayed Pd carbide accumulation and thus carbon resegregation under reaction conditions leads to a much less active interfacial ZrO2–Pd0 state.

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Language(s): eng - English
 Dates: 2020-08-212020-07-132020-08-242020-09-02
 Publication Status: Published online
 Pages: 29
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.3390/catal10091000
 Degree: -

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Title: Catalysts
  Abbreviation : Catalysts
Source Genre: Journal
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Publ. Info: Basel : MDPI
Pages: 29 Volume / Issue: 10 (9) Sequence Number: 1000 Start / End Page: - Identifier: ISSN: 2073-4344
CoNE: https://pure.mpg.de/cone/journals/resource/2073-4344