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Detection of key transient Cu intermediates in SSZ-13 during NH3-SCR deNOx by modulation excitation IR spectroscopy

Greenaway, Alex G., Marberger, Adrian, Thetford, Adam, Lezcano-González, Inés, Agote-Arán, Miren, Nachtegaal, Maarten, Ferri, Davide, Kröcher, Oliver, Catlow, C. Richard A. and Beale, Andrew M. 2020. Detection of key transient Cu intermediates in SSZ-13 during NH3-SCR deNOx by modulation excitation IR spectroscopy. Chemical Science 11 (2) , pp. 447-455. 10.1039/C9SC04905C

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Abstract

The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NOx) by ammonia (NH3). In this work, Cu-SSZ-13 has been studied at 250 °C under high conversion using a modulation excitation approach and analysed with phase sensitive detection (PSD). While the complementary X-ray absorption near edge structure (XANES) spectroscopy measurements showed that the experiments were performed under cyclic Cu+/Cu2+ redox, Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) experiments provide spectroscopic evidence for previously postulated intermediates Cu–N([double bond, length as m-dash]O)–NH2 and Cu–NO3 in the NH3-SCR deNOx mechanism and for the role of [Cu2+(OH−)]+. These results therefore help in building towards a more comprehensive understanding of the reaction mechanism which to date has only been postulated in silico.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Royal Society of Chemistry
ISSN: 2041-6520
Funders: EPSRC
Date of First Compliant Deposit: 28 January 2020
Date of Acceptance: 15 November 2019
Last Modified: 29 Jan 2020 10:30
URI: http://orca.cf.ac.uk/id/eprint/129084

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