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  Understanding CeO2 as a Deacon catalyst by probe molecule adsorption and in situ infrared characterisations

Farra, R., Wrabetz, S., Schuster, M. E., Stotz, E., Hamilton, N., Amrute, A. P., et al. (2013). Understanding CeO2 as a Deacon catalyst by probe molecule adsorption and in situ infrared characterisations. Physical Chemistry Chemical Physics, 15(10), 3454-3465. doi:10.1039/c2cp42767b.

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 Creators:
Farra, Ramzi1, Author              
Wrabetz, Sabine1, Author              
Schuster, Manfred Erwin1, Author              
Stotz, Eugen1, Author              
Hamilton, Neil1, Author              
Amrute, Amol P.2, Author
Pérez-Ramírez, Javier2, Author
López, Núria3, Author
Teschner, Detre1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Wolfgang-Pauli-Strasse 10, CH-8093 Zurich, Switzerland, ou_persistent22              
3Institute of Chemical Research of Catalonia (ICIQ), Av. Paı¨sos Catalans, 16, 43007 Tarragona, Spain, ou_persistent22              

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 Abstract: CeO2 has been identified as an efficient catalyst for HCl oxidation in the temperature range of 623–723 K provided that the oxygen content in the feed mixture was sufficiently high to avoid bulk chlorination and thus deactivation. Here we characterise ceria in its fresh and post-reaction states by adsorption of CO2, NH3 and CO. Micro-calorimetry, FTIR and TPD experiments are complemented by DFT calculations, which assess adsorption energies and vibrational frequencies. The calculations were performed on the lowest energy surface, CeO2(111), with perfect termination and with various degrees of hydroxylation and/or chlorination. Both experiments and calculations suggest that the basic character of the ceria surface has been eliminated upon reaction in HCl oxidation, indicating that most of the basic lattice O sites are exchanged by chlorine and that the OH groups formed are rather acidic. The density and the strength of surface acidic functions increased significantly upon reaction. An in situ FTIR reaction cell has been designed and constructed to study the evolution of OH group density of the ceria surface during HCl oxidation. The effect of experimental variables, such as pO2, pHCl and temperature, has been investigated. We found that the OH group density positively correlated with the reactivity in the pO2 and temperature series, whereas negative correlation was observed when pHCl was varied. Implications of the above observations to the reaction mechanism are discussed.

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Language(s): eng - English
 Dates: 2012-08-082012-12-302013-01-032013-03-14
 Publication Status: Published in print
 Pages: 12
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/c2cp42767b
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Title: Physical Chemistry Chemical Physics
Source Genre: Journal
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Publ. Info: Cambridge [England] : Royal Society of Chemistry
Pages: - Volume / Issue: 15 (10) Sequence Number: - Start / End Page: 3454 - 3465 Identifier: ISSN: 1463-9076
CoNE: https://pure.mpg.de/cone/journals/resource/954925272413_1