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  In Situ EPR Study of the Redox Properties of CuO-CeO2 Catalysts for Preferential CO Oxidation (PROX)

Wang, F., Buchel, R., Savitsky, A., Zalibera, M., Widmann, D., Pratsinis, S. E., et al. (2016). In Situ EPR Study of the Redox Properties of CuO-CeO2 Catalysts for Preferential CO Oxidation (PROX). ACS Catalysis, 6(6), 3520-3530. doi:10.1021/acscatal.6b00589.

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 Creators:
Wang, Feng1, Author              
Buchel, Robert2, Author
Savitsky, Anton3, Author
Zalibera, Michal3, Author
Widmann, Daniel4, Author
Pratsinis, Sotiris E.2, Author
Lubitz, Wolfgang3, Author
Schüth, Ferdi1, Author              
Affiliations:
1Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
2Department of Mechanical and Process Engineering, ETH Zürich, 8092 Zürich, Switzerland, ou_persistent22              
3Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34-36, D-45470 Mülheim an der Ruhr, Germany, ou_persistent22              
4Ulm University, Institute of Surface Chemistry & Catalysis, D-89069 Ulm, Germany, ou_persistent22              

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Free keywords: CuO−CeO2 catalyst; EPR; in situ spectroscopy; preferential CO oxidation; redox mechanism
 Abstract: Understanding the redox properties of metal oxide based catalysts is a major task in catalysis research. In situ electron paramagnetic resonance (EPR) spectroscopy is capable of monitoring the change of metal ion valences and formation of active sites during redox reactions, allowing for the identification of ongoing redox pathways. Here in situ EPR spectroscopy combined with online gas analysis, supported by ex situ X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), X-ray absorption near edge structure (XANES), temporal analysis of product (TAP), and mass spectrometry (MS) studies, was utilized to study the redox behavior of CuO-CeO2 catalysts under PROX conditions (preferential oxidation of carbon monoxide in hydrogen). Two redox mechanisms are revealed: (i) a synergetic mechanism that involves the redox pair Ce4+/Ce3+ during oxidation of Cu0/Cu+ species to Cu2+ and (ii) a direct mechanism that bypasses the redox pair Ce4+/Ce3+. In addition, EPR experiments with isotopically enriched 17O2 established the synergetic mechanism as the major redox reaction pathway. The results emphasize the importance of the interactions between Cu and Ce atoms for catalyst performance. With the guidance of these results, an optimized CuO-CeO2 catalyst could be designed. A rather wide temperature operation window of 11 K (from 377 to 388 K), with 99% conversion efficiency and 99% selectivity, was achieved for the preferential oxidation of CO in a H2 feed.

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Language(s): eng - English
 Dates: 2016-04-182016-09-02
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.6b00589
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 6 (6) Sequence Number: - Start / End Page: 3520 - 3530 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435