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Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy

The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NO(x)) by ammonia (NH(3)). 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 de...

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Autores principales: Greenaway, Alex G., Marberger, Adrian, Thetford, Adam, Lezcano-González, Inés, Agote-Arán, Miren, Nachtegaal, Maarten, Ferri, Davide, Kröcher, Oliver, Catlow, C. Richard A., Beale, Andrew M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7067242/
https://www.ncbi.nlm.nih.gov/pubmed/32190265
http://dx.doi.org/10.1039/c9sc04905c
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author Greenaway, Alex G.
Marberger, Adrian
Thetford, Adam
Lezcano-González, Inés
Agote-Arán, Miren
Nachtegaal, Maarten
Ferri, Davide
Kröcher, Oliver
Catlow, C. Richard A.
Beale, Andrew M.
author_facet Greenaway, Alex G.
Marberger, Adrian
Thetford, Adam
Lezcano-González, Inés
Agote-Arán, Miren
Nachtegaal, Maarten
Ferri, Davide
Kröcher, Oliver
Catlow, C. Richard A.
Beale, Andrew M.
author_sort Greenaway, Alex G.
collection PubMed
description The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NO(x)) by ammonia (NH(3)). 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(+)/Cu(2+) 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)–NH(2) and Cu–NO(3) in the NH(3)-SCR deNO(x) mechanism and for the role of [Cu(2+)(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.
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spelling pubmed-70672422020-03-18 Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) 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. Beale, Andrew M. Chem Sci Chemistry The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NO(x)) by ammonia (NH(3)). 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(+)/Cu(2+) 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)–NH(2) and Cu–NO(3) in the NH(3)-SCR deNO(x) mechanism and for the role of [Cu(2+)(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. Royal Society of Chemistry 2019-11-18 /pmc/articles/PMC7067242/ /pubmed/32190265 http://dx.doi.org/10.1039/c9sc04905c Text en This journal is © The Royal Society of Chemistry 2020 https://creativecommons.org/licenses/by/3.0/This article is freely available. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0)
spellingShingle Chemistry
Greenaway, Alex G.
Marberger, Adrian
Thetford, Adam
Lezcano-González, Inés
Agote-Arán, Miren
Nachtegaal, Maarten
Ferri, Davide
Kröcher, Oliver
Catlow, C. Richard A.
Beale, Andrew M.
Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy
title Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy
title_full Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy
title_fullStr Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy
title_full_unstemmed Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy
title_short Detection of key transient Cu intermediates in SSZ-13 during NH(3)-SCR deNO(x) by modulation excitation IR spectroscopy
title_sort detection of key transient cu intermediates in ssz-13 during nh(3)-scr deno(x) by modulation excitation ir spectroscopy
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7067242/
https://www.ncbi.nlm.nih.gov/pubmed/32190265
http://dx.doi.org/10.1039/c9sc04905c
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