Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts

The assessment of an integral catalytic reactor facilitating operando spectroscopic measurements on a monolith has been carried out using NH3-SCR on a vanadia-based catalyst as a probe reaction. The NH3-SCR mechanism is revisited by studying the adsorbed ammonia and ionically bound ammonium ions and...

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Autores: Rasmussen, Soren B., Portela, Raquel, Bazin, Philippe, Ávila García, Pedro, Bañares, Miguel A., Daturi, Marco
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/162717
Acceso en línea:http://hdl.handle.net/10261/162717
Access Level:acceso abierto
Palabra clave:V2O5-WO3/TiO2-sepiolite honeycomb
NH3-SCR
Operando FTIR
Acid sites
MCR-ALS
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spelling Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalystsRasmussen, Soren B.Portela, RaquelBazin, PhilippeÁvila García, PedroBañares, Miguel A.Daturi, MarcoV2O5-WO3/TiO2-sepiolite honeycombNH3-SCROperando FTIRAcid sitesMCR-ALSThe assessment of an integral catalytic reactor facilitating operando spectroscopic measurements on a monolith has been carried out using NH3-SCR on a vanadia-based catalyst as a probe reaction. The NH3-SCR mechanism is revisited by studying the adsorbed ammonia and ionically bound ammonium ions and their relations to Lewis and Brønsted acid sites during reaction. The simultaneous presence of molecular water and ammonia adsorbed on the surface is intrinsic to low temperature NH3-SCR, and their IR absorption bands overlap in the bending region around 1600 cm−1. This has to be tackled in order to genuinely reproduce real reaction conditions and simultaneously extract relevant spectroscopic data of a working industrial monolithic catalyst. This operando study on a V2O5-WO3/TiO2–sepiolite monolith is performed without added water in the gas phase, but water formed upstream is adsorbed further down, and thus detected by FTIR spectroscopy. We observed that Multivariate Curve Resolution Alternating Least Squares (MCR-ALS) analysis of the 1620 cm−1 envelope of peaks can successfully resolve the bands of adsorbed H2O and NH3 in the monolith during transients between NH3 and NO + O2 flow. Their evolution along with that of surface ammonium ions indicates that generated water hydrolyzes molecularly dispersed vanadia species of the catalyst creating new Brønsted acid sites, and that adsorbed ammonia is either used for the SCR reaction, or converted into the ammonium ion, which then participates in the SCR reaction.This collaborative work was supported by the Spanish Ministry of Science and Innovation (CTQ2014-57578-R). MAB thanks the “Chaire d’Excellence” (FEDER − Région Basse de Normandie, France) and the “Otto Mønsted Visiting Professor” (Denmark) awards. MD and PB also thank the LABEX EMC3 for providing part of the support to this study via the contract “DRUID”.Peer reviewedElsevierMinisterio de Ciencia e Innovación (España)European CommissionConseil Régional de Basse NormandieConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]201820182018info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/162717reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2014-57578-Rhttp://dx.doi.org/10.1016/j.apcatb.2017.10.026Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/1627172026-05-22T06:33:51Z
dc.title.none.fl_str_mv Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
title Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
spellingShingle Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
Rasmussen, Soren B.
V2O5-WO3/TiO2-sepiolite honeycomb
NH3-SCR
Operando FTIR
Acid sites
MCR-ALS
title_short Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
title_full Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
title_fullStr Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
title_full_unstemmed Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
title_sort Transient operando study on the NH3/NH4+ interplay in V-SCR monolithic catalysts
dc.creator.none.fl_str_mv Rasmussen, Soren B.
Portela, Raquel
Bazin, Philippe
Ávila García, Pedro
Bañares, Miguel A.
Daturi, Marco
author Rasmussen, Soren B.
author_facet Rasmussen, Soren B.
Portela, Raquel
Bazin, Philippe
Ávila García, Pedro
Bañares, Miguel A.
Daturi, Marco
author_role author
author2 Portela, Raquel
Bazin, Philippe
Ávila García, Pedro
Bañares, Miguel A.
Daturi, Marco
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv Ministerio de Ciencia e Innovación (España)
European Commission
Conseil Régional de Basse Normandie
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv V2O5-WO3/TiO2-sepiolite honeycomb
NH3-SCR
Operando FTIR
Acid sites
MCR-ALS
topic V2O5-WO3/TiO2-sepiolite honeycomb
NH3-SCR
Operando FTIR
Acid sites
MCR-ALS
description The assessment of an integral catalytic reactor facilitating operando spectroscopic measurements on a monolith has been carried out using NH3-SCR on a vanadia-based catalyst as a probe reaction. The NH3-SCR mechanism is revisited by studying the adsorbed ammonia and ionically bound ammonium ions and their relations to Lewis and Brønsted acid sites during reaction. The simultaneous presence of molecular water and ammonia adsorbed on the surface is intrinsic to low temperature NH3-SCR, and their IR absorption bands overlap in the bending region around 1600 cm−1. This has to be tackled in order to genuinely reproduce real reaction conditions and simultaneously extract relevant spectroscopic data of a working industrial monolithic catalyst. This operando study on a V2O5-WO3/TiO2–sepiolite monolith is performed without added water in the gas phase, but water formed upstream is adsorbed further down, and thus detected by FTIR spectroscopy. We observed that Multivariate Curve Resolution Alternating Least Squares (MCR-ALS) analysis of the 1620 cm−1 envelope of peaks can successfully resolve the bands of adsorbed H2O and NH3 in the monolith during transients between NH3 and NO + O2 flow. Their evolution along with that of surface ammonium ions indicates that generated water hydrolyzes molecularly dispersed vanadia species of the catalyst creating new Brønsted acid sites, and that adsorbed ammonia is either used for the SCR reaction, or converted into the ammonium ion, which then participates in the SCR reaction.
publishDate 2018
dc.date.none.fl_str_mv 2018
2018
2018
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/162717
url http://hdl.handle.net/10261/162717
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2014-57578-R
http://dx.doi.org/10.1016/j.apcatb.2017.10.026
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,81155

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