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  Nanocatalysts Unravel the Selective State of Ag

Lamoth, M., Jones, T., Plodinec, M., Machoke, A. G. F., Wrabetz, S., Krämer, M., et al. (2020). Nanocatalysts Unravel the Selective State of Ag. ChemCatChem, 12(11), 2977-2988. doi:10.1002/cctc.202000035.

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 Creators:
Lamoth, Maximilian1, Author              
Jones, Travis1, Author              
Plodinec, Milivoj1, Author              
Machoke, Albert Gonche Fortunatus2, Author
Wrabetz, Sabine1, Author              
Krämer, Michael3, Author
Karpov, Andrey3, Author
Rosowski, Frank3, 4, Author
Piccinin, Simone5, Author
Schlögl, Robert1, 2, Author              
Frei, Elias1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              
3Process Research and Chemical Engineering Process Catalysis Research, BASF SE, Ludwigshafen, 67063, Germany, ou_persistent22              
4BasCat-UniCat BASF Joint Lab, Technical University Berlin, Hardenbergstraße 36, Berlin, 10623, Germany, ou_persistent22              
5Istituto Officina dei Materiali (CNR-IOM), Area Science Park Basovizza S.S. 14, Km. 163,5, Trieste, 34149, Italy , ou_persistent22              

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Free keywords: Ag nanoparticles Ag−O interaction ethylene epoxidation oxophilicity selective state supported Ag catalysts
 Abstract: In the present work, we report on a comparative study of model catalysts during ethylene epoxidation reaction under industrially relevant conditions. The catalysts consist of Ag nanoparticles <6 nm and a reference sample ∼100 nm. Combining catalytic data with transmission electron microscopy, thermal desorption spectroscopy, and density functional theory allows us to show that catalytic performance is linked to the oxygen concentration in/on the Ag particles. Isotope experiments using 18O2 and C18O2 are conducted to gain insight into the nature and location of oxygen in/on the Ag nanoparticles. The oxygen species responsible for the CO2 formation and inhibition of the overall catalytic activity are identified, and the abundance of those species is shown to depend strongly on the pre-treatment and reaction conditions, showing both are critical for effective oxygen management. By comparison with a conventional Ag/α-Al2O3 catalyst, we demonstrate a low concentration of oxygen in/on Ag leads to the highest selectivity regardless of particle size. However, particle size dependent oxophilicity leads to significantly lower TOFs for the Ag nanoparticles. This study provides fundamental understanding of the performance of supported Ag particles in ethylene epoxidation and offers new strategies to improve performance under industrially relevant conditions.

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Language(s): eng - English
 Dates: 2020-01-082020-03-232020-06-05
 Publication Status: Published online
 Pages: 12
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/cctc.202000035
 Degree: -

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Title: ChemCatChem
  Other : ChemCatChem
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 12 Volume / Issue: 12 (11) Sequence Number: - Start / End Page: 2977 - 2988 Identifier: ISSN: 1867-3880
CoNE: https://pure.mpg.de/cone/journals/resource/1867-3880