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What Makes Copper-Exchanged SSZ-13 Zeolite Efficient at Cleaning Car Exhaust Gases?

Autor(en)
Florian Göltl, Rosa E. Bulo, Juergen Hafner, Philippe Sautet
Abstrakt

Recently, the outstanding properties of Cu-SSZ-13 (a zeolite in the chabazite structure) for the selective catalytic reduction of nitrous oxides were discovered. However, the true nature of the active site is still not answered satisfactorily. In this work, we identify the active site for the given reaction from first-principles simulations of the total energy of Cu(II) ions in various positions in combination with previously published catalytic activity as a function of the copper exchange level. This attribution is confirmed by the simulation of vibrational properties of CO adsorbed to the reduced Cu(I) species. The relation between energetic considerations, vibrational calculations, and experiment allows a clear statement about the distribution of active sites in the catalyst. We furthermore discuss the structural properties of the active site leading to the high stability under reaction conditions over a large temperature range. The insights from this work allow a more targeted catalyst design and represent a step toward an industrial application of copper-exchanged zeolites in cleaning car exhaust gases.

Organisation(en)
Computergestützte Materialphysik
Externe Organisation(en)
École normale supérieure de Lyon (ENS Lyon), Vrije Universiteit Amsterdam
Journal
The Journal of Physical Chemistry Letters
Band
4
Seiten
2244-2249
Anzahl der Seiten
6
ISSN
1948-7185
DOI
https://doi.org/10.1021/jz400817c
Publikationsdatum
07-2013
Peer-reviewed
Ja
ÖFOS 2012
103009 Festkörperphysik, 103015 Kondensierte Materie, 103025 Quantenmechanik, 103036 Theoretische Physik
Schlagwörter
Link zum Portal
https://ucrisportal.univie.ac.at/de/publications/2cf8e25b-5f47-4cf8-82c3-f6fedab3d29d