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Issue 1, 2015
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Revisiting the nature of Cu sites in the activated Cu-SSZ-13 catalyst for SCR reaction

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Abstract

Cu-SSZ-13 is a highly active NH3-SCR catalyst for the abatement of harmful nitrogen oxides (NOx, x = 1, 2) from the exhausts of lean-burn engines. The study of Cu-speciation occurring upon thermal dehydration is a key step for the understanding of the enhanced catalytic properties of this material and for identifying the SCR active sites and their redox capability. Herein, we combined FTIR, X-ray absorption (XAS) and emission (XES) spectroscopies with DFT computational analysis to elucidate the nature and location of the most abundant Cu sites in the activated catalyst. Different Cu species have been found to be dominant as a function of the dehydration temperature and conditions. Data analysis revealed that the dehydration process of Cu cations is essentially completed at 250 °C, with the formation of dehydrated [CuOH]+ species hosted in close proximity to 1-Al sites in both d6r and 8r units of the SSZ-13 matrix. These species persist at higher temperatures only if a certain amount of O2 is present in the gas feed, while under inert conditions they undergo virtually total “self-reduction” as a consequence of an OH extra-ligand loss, resulting in bi-coordinated bare Cu+ cations. Synchrotron characterization supported by computational analysis allowed an unprecedented quantitative refinement of the local environment and structural parameters of these Cu(II) and Cu(I) species.

Graphical abstract: Revisiting the nature of Cu sites in the activated Cu-SSZ-13 catalyst for SCR reaction

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Supplementary files

Article information


Submitted
20 Sep 2014
Accepted
13 Oct 2014
First published
13 Oct 2014

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2015,6, 548-563
Article type
Edge Article
Author version available

Revisiting the nature of Cu sites in the activated Cu-SSZ-13 catalyst for SCR reaction

E. Borfecchia, K. A. Lomachenko, F. Giordanino, H. Falsig, P. Beato, A. V. Soldatov, S. Bordiga and C. Lamberti, Chem. Sci., 2015, 6, 548
DOI: 10.1039/C4SC02907K

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