CO Total and preferential oxidation over stable Au/TiO2 catalysts derived from preformed au nanoparticles

Autores
Divins, Núria J.; Lopez, Eduardo; Angurell, Inmaculada; Neuberg, Stefan; Zapf, Ralf; Kolb, Gunther; Llorca Piqué, Jordi
Año de publicación
2020
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
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.
Fil: Divins, Núria J.. Universidad Politécnica de Catalunya; España
Fil: Lopez, Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Angurell, Inmaculada. Universidad de Barcelona. Facultad de Química; España
Fil: Neuberg, Stefan. Fraunhofer Institute of Microengineering and Microsystems; Alemania
Fil: Zapf, Ralf. Fraunhofer Institute of Microengineering and Microsystems; Alemania
Fil: Kolb, Gunther. Fraunhofer Institute of Microengineering and Microsystems; Alemania
Fil: Llorca Piqué, Jordi. Universidad Politécnica de Catalunya; España
Materia
CO OXIDATION
CO-PROX
DENDRIMERS
DENDRONS
FUEL REFORMER
MICROREACTOR
PREFORMED AU NANOPARTICLES
PROX
STABILITY TEST
THIOLS
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/126974
Acceder
id CONICETDig_7daa6469c4b3d994f7170ccab6ce053d
oai_identifier_str oai:ri.conicet.gov.ar:11336/126974
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling CO Total and preferential oxidation over stable Au/TiO2 catalysts derived from preformed au nanoparticlesDivins, Núria J.Lopez, EduardoAngurell, InmaculadaNeuberg, StefanZapf, RalfKolb, GuntherLlorca Piqué, JordiCO OXIDATIONCO-PROXDENDRIMERSDENDRONSFUEL REFORMERMICROREACTORPREFORMED AU NANOPARTICLESPROXSTABILITY TESTTHIOLShttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2CO 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.Fil: Divins, Núria J.. Universidad Politécnica de Catalunya; EspañaFil: Lopez, Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaFil: Angurell, Inmaculada. Universidad de Barcelona. Facultad de Química; EspañaFil: Neuberg, Stefan. Fraunhofer Institute of Microengineering and Microsystems; AlemaniaFil: Zapf, Ralf. Fraunhofer Institute of Microengineering and Microsystems; AlemaniaFil: Kolb, Gunther. Fraunhofer Institute of Microengineering and Microsystems; AlemaniaFil: Llorca Piqué, Jordi. Universidad Politécnica de Catalunya; EspañaMolecular Diversity Preservation International2020-09-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/126974Divins, Núria J.; Lopez, Eduardo; Angurell, Inmaculada; Neuberg, Stefan; Zapf, Ralf; et al.; CO Total and preferential oxidation over stable Au/TiO2 catalysts derived from preformed au nanoparticles; Molecular Diversity Preservation International; Catalysts; 10; 9; 7-9-2020; 1-202073-4344CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.mdpi.com/2073-4344/10/9/1028info:eu-repo/semantics/altIdentifier/doi/10.3390/catal10091028info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:32:50Zoai:ri.conicet.gov.ar:11336/126974instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 10:32:50.266CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
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.
CO OXIDATION
CO-PROX
DENDRIMERS
DENDRONS
FUEL REFORMER
MICROREACTOR
PREFORMED AU NANOPARTICLES
PROX
STABILITY TEST
THIOLS
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.
Lopez, Eduardo
Angurell, Inmaculada
Neuberg, Stefan
Zapf, Ralf
Kolb, Gunther
Llorca Piqué, Jordi
author Divins, Núria J.
author_facet Divins, Núria J.
Lopez, Eduardo
Angurell, Inmaculada
Neuberg, Stefan
Zapf, Ralf
Kolb, Gunther
Llorca Piqué, Jordi
author_role author
author2 Lopez, Eduardo
Angurell, Inmaculada
Neuberg, Stefan
Zapf, Ralf
Kolb, Gunther
Llorca Piqué, Jordi
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv CO OXIDATION
CO-PROX
DENDRIMERS
DENDRONS
FUEL REFORMER
MICROREACTOR
PREFORMED AU NANOPARTICLES
PROX
STABILITY TEST
THIOLS
topic CO OXIDATION
CO-PROX
DENDRIMERS
DENDRONS
FUEL REFORMER
MICROREACTOR
PREFORMED AU NANOPARTICLES
PROX
STABILITY TEST
THIOLS
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv 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.
Fil: Divins, Núria J.. Universidad Politécnica de Catalunya; España
Fil: Lopez, Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Angurell, Inmaculada. Universidad de Barcelona. Facultad de Química; España
Fil: Neuberg, Stefan. Fraunhofer Institute of Microengineering and Microsystems; Alemania
Fil: Zapf, Ralf. Fraunhofer Institute of Microengineering and Microsystems; Alemania
Fil: Kolb, Gunther. Fraunhofer Institute of Microengineering and Microsystems; Alemania
Fil: Llorca Piqué, Jordi. Universidad Politécnica de Catalunya; España
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 2020-09-07
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/126974
Divins, Núria J.; Lopez, Eduardo; Angurell, Inmaculada; Neuberg, Stefan; Zapf, Ralf; et al.; CO Total and preferential oxidation over stable Au/TiO2 catalysts derived from preformed au nanoparticles; Molecular Diversity Preservation International; Catalysts; 10; 9; 7-9-2020; 1-20
2073-4344
CONICET Digital
CONICET
url http://hdl.handle.net/11336/126974
identifier_str_mv Divins, Núria J.; Lopez, Eduardo; Angurell, Inmaculada; Neuberg, Stefan; Zapf, Ralf; et al.; CO Total and preferential oxidation over stable Au/TiO2 catalysts derived from preformed au nanoparticles; Molecular Diversity Preservation International; Catalysts; 10; 9; 7-9-2020; 1-20
2073-4344
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://www.mdpi.com/2073-4344/10/9/1028
info:eu-repo/semantics/altIdentifier/doi/10.3390/catal10091028
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Molecular Diversity Preservation International
publisher.none.fl_str_mv Molecular Diversity Preservation International
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.070432

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