CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles

CO preferential oxidation (PROX) is an effective method to clean reformate H2 streams to feed low-temperature fuel cells. In this work, the PROX and CO oxidation reactions were studied on preformed Au nanoparticles (NPs) supported on TiO2 anatase. Preformed Au NPs were obtained from gold cores stabi...

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Detalles Bibliográficos
Autores: Divins, Núria J., López, Eduardo, Angurell Purroy, Inmaculada, Neuberg, Stefan, Zapf, Ralf, Kolb, Gunther, Llorca, Jordi, 1966-
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2020
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/176145
Acceso en línea:https://hdl.handle.net/2445/176145
Access Level:acceso abierto
Palabra clave:Oxidació
Nanopartícules
Catalitzadors
Oxidation
Nanoparticles
Catalysts
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spelling CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticlesDivins, Núria J.López, EduardoAngurell Purroy, InmaculadaNeuberg, StefanZapf, RalfKolb, GuntherLlorca, Jordi, 1966-OxidacióNanopartículesCatalitzadorsOxidationNanoparticlesCatalystsCO preferential oxidation (PROX) is an effective method to clean reformate H2 streams to feed low-temperature fuel cells. In this work, the PROX and CO oxidation reactions were studied on preformed Au nanoparticles (NPs) supported on TiO2 anatase. Preformed Au NPs were obtained from gold cores stabilized by dodecanethiols or trimethylsilane-dendrons. A well-controlled size of ca. 2.6 nm and narrow size distributions were achieved by this procedure. The catalysts were characterized by high-resolution transmission electron microscopy and ex situ and in situ X-ray photoelectron spectroscopy (XPS). The XPS results showed that the preformed Au NPs exhibited high thermal stability. The different ligand-derived Au catalysts, as well as a conventional gold catalyst for comparison purposes, were loaded onto cordierite supports with 400 cells per square inch. The activity and selectivity of the samples were evaluated for various operation conditions. The catalyst prepared using dodecanethiol-capped Au NPs showed the best performance. In fact, CO conversions of up to 70% at 40% CO2 selectivity and 90% O2 conversion were observed operating at 363 K in H2-rich atmospheres. The performance of the best catalysts was subsequently tested on stainless steel microreactors. A 500-hour stability test was carried out under a real post-reformate stream, including 18 vol.% CO2 and 29 vol.% H2O. A mean CO conversion of ca. 24% was measured for the whole test operating at 453 K and a gas hourly space velocity (GHSV) of 1.3 × 104 h−1. These results reveal our dodecanethiol- and carbosilane-derived Au catalysts as extremely promising candidates to conduct a PROX reaction while avoiding deactivation, which is one of the major drawbacks of Au/TiO2 catalysts.MDPI2021202120202021info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion21 p.application/pdfhttps://hdl.handle.net/2445/176145Articles publicats en revistes (Química Inorgànica i Orgànica)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésReproducció del document publicat a: https://doi.org/10.3390/catal10091028Catalysts, 2020, vol. 10, num. 9, p. 1028https://doi.org/10.3390/catal10091028cc-by (c) Divins, Núria J. et al., 2020http://creativecommons.org/licenses/by/3.0/esinfo:eu-repo/semantics/openAccessoai:recercat.cat:2445/1761452026-05-29T05:05:01Z
dc.title.none.fl_str_mv CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
title CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
spellingShingle CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
Divins, Núria J.
Oxidació
Nanopartícules
Catalitzadors
Oxidation
Nanoparticles
Catalysts
title_short CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
title_full CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
title_fullStr CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
title_full_unstemmed CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
title_sort CO total and Preferential Oxidation over stable Au/TiO2 catalysts derived from preformed Au nanoparticles
dc.creator.none.fl_str_mv Divins, Núria J.
López, Eduardo
Angurell Purroy, Inmaculada
Neuberg, Stefan
Zapf, Ralf
Kolb, Gunther
Llorca, Jordi, 1966-
author Divins, Núria J.
author_facet Divins, Núria J.
López, Eduardo
Angurell Purroy, Inmaculada
Neuberg, Stefan
Zapf, Ralf
Kolb, Gunther
Llorca, Jordi, 1966-
author_role author
author2 López, Eduardo
Angurell Purroy, Inmaculada
Neuberg, Stefan
Zapf, Ralf
Kolb, Gunther
Llorca, Jordi, 1966-
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Oxidació
Nanopartícules
Catalitzadors
Oxidation
Nanoparticles
Catalysts
topic Oxidació
Nanopartícules
Catalitzadors
Oxidation
Nanoparticles
Catalysts
description CO preferential oxidation (PROX) is an effective method to clean reformate H2 streams to feed low-temperature fuel cells. In this work, the PROX and CO oxidation reactions were studied on preformed Au nanoparticles (NPs) supported on TiO2 anatase. Preformed Au NPs were obtained from gold cores stabilized by dodecanethiols or trimethylsilane-dendrons. A well-controlled size of ca. 2.6 nm and narrow size distributions were achieved by this procedure. The catalysts were characterized by high-resolution transmission electron microscopy and ex situ and in situ X-ray photoelectron spectroscopy (XPS). The XPS results showed that the preformed Au NPs exhibited high thermal stability. The different ligand-derived Au catalysts, as well as a conventional gold catalyst for comparison purposes, were loaded onto cordierite supports with 400 cells per square inch. The activity and selectivity of the samples were evaluated for various operation conditions. The catalyst prepared using dodecanethiol-capped Au NPs showed the best performance. In fact, CO conversions of up to 70% at 40% CO2 selectivity and 90% O2 conversion were observed operating at 363 K in H2-rich atmospheres. The performance of the best catalysts was subsequently tested on stainless steel microreactors. A 500-hour stability test was carried out under a real post-reformate stream, including 18 vol.% CO2 and 29 vol.% H2O. A mean CO conversion of ca. 24% was measured for the whole test operating at 453 K and a gas hourly space velocity (GHSV) of 1.3 × 104 h−1. These results reveal our dodecanethiol- and carbosilane-derived Au catalysts as extremely promising candidates to conduct a PROX reaction while avoiding deactivation, which is one of the major drawbacks of Au/TiO2 catalysts.
publishDate 2020
dc.date.none.fl_str_mv 2020
2021
2021
2021
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/176145
url https://hdl.handle.net/2445/176145
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.3390/catal10091028
Catalysts, 2020, vol. 10, num. 9, p. 1028
https://doi.org/10.3390/catal10091028
dc.rights.none.fl_str_mv cc-by (c) Divins, Núria J. et al., 2020
http://creativecommons.org/licenses/by/3.0/es
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by (c) Divins, Núria J. et al., 2020
http://creativecommons.org/licenses/by/3.0/es
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 21 p.
application/pdf
dc.publisher.none.fl_str_mv MDPI
publisher.none.fl_str_mv MDPI
dc.source.none.fl_str_mv Articles publicats en revistes (Química Inorgànica i Orgànica)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.811543

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