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

Alex G. Greenaway; Adrian Marberger; Adam Thetford; Inés Lezcano-González; Miren Agote-Arán; Maarten Nachtegaal; Davide Ferri; Oliver Kröcher; C. Richard A. Catlow; Andrew M. Beale

doi:10.1039/c9sc04905c

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

Alex G. Greenaway, Adrian Marberger, Adam Thetford, Inés Lezcano-González, Miren Agote-Arán, Maarten Nachtegaal, Davide Ferri, Oliver Kröcher, C. Richard A. Catlow, Andrew M. Beale^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NO_x) 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(O)-NH₂ and Cu-NO₃ in the NH₃-SCR deNO_x 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.

Original language	English
Pages (from-to)	447-455
Number of pages	9
Journal	Chemical Science
Volume	11
Issue number	2
DOIs	https://doi.org/10.1039/c9sc04905c
Publication status	Published - 2020
Externally published	Yes

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@article{147a0004d5984c26bd91c4f6b1aaf647,

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

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(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.",

author = "Greenaway, {Alex G.} and Adrian Marberger and Adam Thetford and In{\'e}s Lezcano-Gonz{\'a}lez and Miren Agote-Ar{\'a}n and Maarten Nachtegaal and Davide Ferri and Oliver Kr{\"o}cher and Catlow, {C. Richard A.} and Beale, {Andrew M.}",

note = "Publisher Copyright: {\textcopyright} 2020 The Royal Society of Chemistry.",

year = "2020",

doi = "10.1039/c9sc04905c",

language = "English",

volume = "11",

pages = "447--455",

journal = "Chemical Science",

issn = "2041-6520",

publisher = "Royal Society of Chemistry",

number = "2",

}

TY - JOUR

T1 - Detection of key transient Cu intermediates in SSZ-13 during NH3-SCR deNOx by modulation excitation IR spectroscopy

AU - Greenaway, Alex G.

AU - Marberger, Adrian

AU - Thetford, Adam

AU - Lezcano-González, Inés

AU - Agote-Arán, Miren

AU - Nachtegaal, Maarten

AU - Ferri, Davide

AU - Kröcher, Oliver

AU - Catlow, C. Richard A.

AU - Beale, Andrew M.

PY - 2020

Y1 - 2020

N2 - 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(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.

AB - 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(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.

UR - http://www.scopus.com/inward/record.url?scp=85077734790&partnerID=8YFLogxK

U2 - 10.1039/c9sc04905c

DO - 10.1039/c9sc04905c

M3 - Article

AN - SCOPUS:85077734790

SN - 2041-6520

VL - 11

SP - 447

EP - 455

JO - Chemical Science

JF - Chemical Science

IS - 2

ER -

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

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