In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO

Raman spectroscopic technique has been used to characterize a Ru/TiO2 catalyst and to follow in situ their structural changes during the CO selective methanation reaction (S-MET). For a better comprehension of the catalytic mechanism, the in-situ Raman study of the catalysts activation (reduction) p...

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Authors: Martínez Tejada, Leidy Marcela, Muñoz Murillo, Ara, Centeno Gallego, Miguel Ángel, Odriozola Gordón, José Antonio
Format: article
Status:Versión enviada para evaluación y publicación
Publication Date:2016
Country:España
Institution:Universidad de Sevilla (US)
Repository:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:idus.us.es:11441/71311
Online Access:https://hdl.handle.net/11441/71311
https://doi.org/10.1002/jrs.4774
Access Level:Open access
Keyword:Ru/TiO2
CO
CO2
Raman
Anatase
Rutile
Methanation
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spelling In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of COMartínez Tejada, Leidy MarcelaMuñoz Murillo, AraCenteno Gallego, Miguel ÁngelOdriozola Gordón, José AntonioRu/TiO2COCO2RamanAnataseRutileMethanationRaman spectroscopic technique has been used to characterize a Ru/TiO2 catalyst and to follow in situ their structural changes during the CO selective methanation reaction (S-MET). For a better comprehension of the catalytic mechanism, the in-situ Raman study of the catalysts activation (reduction) process, the isolated CO and CO2 methanation reactions and the effect of the composition of the reactive stream (H2O and CO2 presence) have been carried out. Raman spectroscopy evidences that the catalyst is composed by islands of TiO2¿RuO2 solid solutions, constituting Ru¿TiO2 interphases in the form of RuxTi1 xO2 rutile type solid solutions. The activation procedure with H2 at 300 °C promotes the reduction of the RuO2¿TiO2 islands generating Ruo ¿Ti3+ centers. The spectroscopic changes are in agreement with the strong increase in chemical reactivity as increasing the carbonaceous intermediates observed. The selective methanation of CO proceeds after their adsorption on these Ruo ¿Ti3+ active centers and subsequent C-O dissociation throughout the formation of CHx/CnHx/CnHxO/CHx-CO species. These intermediates are transformed into CH4 by a combination of hydrogenation reactions. The formation of carbonaceous species during the methanation of CO and CO2 suggests that the CO presence is required to promote the CO2 methanation. Similar carbonaceous species are detected when the selective CO methanation is carried out with water in the stream. However, the activation of the catalysts occurs at much lower temperatures, and the carbon oxidation is favored by the oxidative effect of water.España Mineco ENE2012- 37431-C03-03Unión Europea Junta de Andalucia FEDER TEP-8196WileyQuímica InorgánicaMinisterio de Economía y Competitividad (MINECO). EspañaJunta de Andalucía2016info:eu-repo/semantics/articleinfo:eu-repo/semantics/submittedVersionapplication/pdfapplication/pdfhttps://hdl.handle.net/11441/71311https://doi.org/10.1002/jrs.4774reponame:idUS. Depósito de Investigación de la Universidad de Sevillainstname:Universidad de Sevilla (US)InglésJournal of Raman Spectroscopy, 47, 189-197.ENE2012- 37431-C03-03TEP-8196http://dx.doi.org/10.1002/jrs.4774info:eu-repo/semantics/openAccessoai:idus.us.es:11441/713112026-06-17T12:51:07Z
dc.title.none.fl_str_mv In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
title In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
spellingShingle In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
Martínez Tejada, Leidy Marcela
Ru/TiO2
CO
CO2
Raman
Anatase
Rutile
Methanation
title_short In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
title_full In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
title_fullStr In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
title_full_unstemmed In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
title_sort In-situ Raman spectroscopy study of Ru/TiO2 catalyst in the selective methanation of CO
dc.creator.none.fl_str_mv Martínez Tejada, Leidy Marcela
Muñoz Murillo, Ara
Centeno Gallego, Miguel Ángel
Odriozola Gordón, José Antonio
author Martínez Tejada, Leidy Marcela
author_facet Martínez Tejada, Leidy Marcela
Muñoz Murillo, Ara
Centeno Gallego, Miguel Ángel
Odriozola Gordón, José Antonio
author_role author
author2 Muñoz Murillo, Ara
Centeno Gallego, Miguel Ángel
Odriozola Gordón, José Antonio
author2_role author
author
author
dc.contributor.none.fl_str_mv Química Inorgánica
Ministerio de Economía y Competitividad (MINECO). España
Junta de Andalucía
dc.subject.none.fl_str_mv Ru/TiO2
CO
CO2
Raman
Anatase
Rutile
Methanation
topic Ru/TiO2
CO
CO2
Raman
Anatase
Rutile
Methanation
description Raman spectroscopic technique has been used to characterize a Ru/TiO2 catalyst and to follow in situ their structural changes during the CO selective methanation reaction (S-MET). For a better comprehension of the catalytic mechanism, the in-situ Raman study of the catalysts activation (reduction) process, the isolated CO and CO2 methanation reactions and the effect of the composition of the reactive stream (H2O and CO2 presence) have been carried out. Raman spectroscopy evidences that the catalyst is composed by islands of TiO2¿RuO2 solid solutions, constituting Ru¿TiO2 interphases in the form of RuxTi1 xO2 rutile type solid solutions. The activation procedure with H2 at 300 °C promotes the reduction of the RuO2¿TiO2 islands generating Ruo ¿Ti3+ centers. The spectroscopic changes are in agreement with the strong increase in chemical reactivity as increasing the carbonaceous intermediates observed. The selective methanation of CO proceeds after their adsorption on these Ruo ¿Ti3+ active centers and subsequent C-O dissociation throughout the formation of CHx/CnHx/CnHxO/CHx-CO species. These intermediates are transformed into CH4 by a combination of hydrogenation reactions. The formation of carbonaceous species during the methanation of CO and CO2 suggests that the CO presence is required to promote the CO2 methanation. Similar carbonaceous species are detected when the selective CO methanation is carried out with water in the stream. However, the activation of the catalysts occurs at much lower temperatures, and the carbon oxidation is favored by the oxidative effect of water.
publishDate 2016
dc.date.none.fl_str_mv 2016
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/submittedVersion
format article
status_str submittedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/11441/71311
https://doi.org/10.1002/jrs.4774
url https://hdl.handle.net/11441/71311
https://doi.org/10.1002/jrs.4774
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Journal of Raman Spectroscopy, 47, 189-197.
ENE2012- 37431-C03-03
TEP-8196
http://dx.doi.org/10.1002/jrs.4774
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Wiley
publisher.none.fl_str_mv Wiley
dc.source.none.fl_str_mv reponame:idUS. Depósito de Investigación de la Universidad de Sevilla
instname:Universidad de Sevilla (US)
instname_str Universidad de Sevilla (US)
reponame_str idUS. Depósito de Investigación de la Universidad de Sevilla
collection idUS. Depósito de Investigación de la Universidad de Sevilla
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,300724

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