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Chemical gradients in automotive Cu-SSZ-13 catalysts for NO$_{x}$ removal revealed by operando X-ray spectrotomography

Becher, Johannes; Sanchez, Dario Ferreira; Doronkin, Dmitry E.; Zengel, Deniz; Meira, Debora Motta; Pascarelli, Sakura; Grunwaldt, Jan-Dierk; Sheppard, Thomas L.

Abstract:
NOx emissions are a major source of pollution, demanding ever improving performance from catalytic aftertreatment systems. However, catalyst development is often hindered by limited understanding of the catalyst at work, exacerbated by widespread use of model rather than technical catalysts, and global rather than spatially-resolved characterisation tools. Here we combine operando X-ray absorption spectroscopy with microtomography to perform 3D chemical imaging of the chemical state of copper species in a Cu-SSZ-13 washcoated monolith catalyst during NO$_{x}$ reduction. Gradients in copper oxidation state and coordination environment, resulting from an interplay of NOx reduction with adsorption-desorption of NH$_{3}$ and mass transport phenomena, were revealed with micrometre spatial resolution while simultaneously determining catalytic performance. Crucially, direct 3D visualisation of complex reactions on nonmodel catalysts is only feasible using operando X-ray spectrotomography, which can improve our understanding of structure-activity relationships including the observation of mass and heat transport effects.


Postprint §
DOI: 10.5445/IR/1000127732
Veröffentlicht am 15.06.2021
Originalveröffentlichung
DOI: 10.1038/s41929-020-00552-3
Dimensions
Zitationen: 23
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Katalyseforschung und -technologie (IKFT)
Institut für Technische Chemie und Polymerchemie (ITCP)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2021
Sprache Englisch
Identifikator ISSN: 2520-1158
KITopen-ID: 1000127732
HGF-Programm 37.03.01 (POF III, LK 01) Catalysts and Mechanisms
Erschienen in Nature catalysis
Verlag Nature Research
Band 4
Seiten 46–53
Vorab online veröffentlicht am 14.12.2020
Nachgewiesen in Dimensions
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