Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes

Bimetallic Pt:Pd catalysts with different molar ratios and 0.5 wt.% overall metal load supported on sulfated zirconia catalysts were synthesized and tested in the gas-phase hydrodechlorination (HDC) of chloromethanes and their mixtures. The catalysts were characterized by adsorption–desorption of N...

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Autores: Bedia, J., Arevalo-Bastante, A., Grau, J. M., Dosso, L. A., Rodriguez, Juan J., Mayoral, Álvaro, Díaz Carretero, Isabel, Gómez-Sainero, L.M.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2017
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/182802
Acceso en línea:http://hdl.handle.net/10261/182802
Access Level:acceso abierto
Palabra clave:Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated zirconia
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spelling Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanesBedia, J.Arevalo-Bastante, A.Grau, J. M.Dosso, L. A.Rodriguez, Juan J.Mayoral, ÁlvaroDíaz Carretero, IsabelGómez-Sainero, L.M.ChloromethanesHydrodechlorinationPalladiumPlatinumSulfated zirconiaBimetallic Pt:Pd catalysts with different molar ratios and 0.5 wt.% overall metal load supported on sulfated zirconia catalysts were synthesized and tested in the gas-phase hydrodechlorination (HDC) of chloromethanes and their mixtures. The catalysts were characterized by adsorption–desorption of N at −196 °C, X-ray diffraction, X-ray photoelectronic spectroscopy, temperature-programmed reduction, and aberration-corrected scanning transmission electron microscopy (STEM). The effect of the Pt:Pd molar ratio on the activity, stability, and selectivity was analyzed. The high acidity of the sulfated zirconia results in metal particles of small size (mainly <5 nm), as confirmed by STEM. The bimetallic catalysts showed higher stability than the monometallic ones, as demonstrated in long-term experiments (80 h on stream), confirming the positive effect of combining the two metallic phases. Turnover frequency (TOF) values in the range 0.0007–0.0168 s and apparent activation energies between ≈41 and 44 kJ·mol were obtained. TOF values for dichloromethane HDC increased with increasing mean metal particle size within the range of this work (≈1.2–2.3 nm). The catalysts with Pt:Pd molar ratios of 1:3 and 1:1 showed significantly better performance than the 3:1 one for overall dechlorination due to their higher atomic metal content and TOF at the same total metal weight load (0.5%).Spanish ‘‘Ministerio de Economía y Competitividad (MINECO)” for financial support (Projects CTM2011-28352 and CTM2014-53008-R). A. Arevalo Bastanteacknowledges MINECO for her research granPeer ReviewedElsevierMinisterio de Economía y Competitividad (España)2019201920172019info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/182802reponame: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/CTM2014-53008-Rhttp://dx.doi.org/10.1016/j.jcat.2017.06.013info:eu-repo/semantics/openAccessoai:digital.csic.es:10261/1828022026-05-22T06:33:51Z
dc.title.none.fl_str_mv Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
title Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
spellingShingle Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
Bedia, J.
Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated zirconia
title_short Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
title_full Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
title_fullStr Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
title_full_unstemmed Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
title_sort Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes
dc.creator.none.fl_str_mv Bedia, J.
Arevalo-Bastante, A.
Grau, J. M.
Dosso, L. A.
Rodriguez, Juan J.
Mayoral, Álvaro
Díaz Carretero, Isabel
Gómez-Sainero, L.M.
author Bedia, J.
author_facet Bedia, J.
Arevalo-Bastante, A.
Grau, J. M.
Dosso, L. A.
Rodriguez, Juan J.
Mayoral, Álvaro
Díaz Carretero, Isabel
Gómez-Sainero, L.M.
author_role author
author2 Arevalo-Bastante, A.
Grau, J. M.
Dosso, L. A.
Rodriguez, Juan J.
Mayoral, Álvaro
Díaz Carretero, Isabel
Gómez-Sainero, L.M.
author2_role author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Ministerio de Economía y Competitividad (España)
dc.subject.none.fl_str_mv Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated zirconia
topic Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated zirconia
description Bimetallic Pt:Pd catalysts with different molar ratios and 0.5 wt.% overall metal load supported on sulfated zirconia catalysts were synthesized and tested in the gas-phase hydrodechlorination (HDC) of chloromethanes and their mixtures. The catalysts were characterized by adsorption–desorption of N at −196 °C, X-ray diffraction, X-ray photoelectronic spectroscopy, temperature-programmed reduction, and aberration-corrected scanning transmission electron microscopy (STEM). The effect of the Pt:Pd molar ratio on the activity, stability, and selectivity was analyzed. The high acidity of the sulfated zirconia results in metal particles of small size (mainly <5 nm), as confirmed by STEM. The bimetallic catalysts showed higher stability than the monometallic ones, as demonstrated in long-term experiments (80 h on stream), confirming the positive effect of combining the two metallic phases. Turnover frequency (TOF) values in the range 0.0007–0.0168 s and apparent activation energies between ≈41 and 44 kJ·mol were obtained. TOF values for dichloromethane HDC increased with increasing mean metal particle size within the range of this work (≈1.2–2.3 nm). The catalysts with Pt:Pd molar ratios of 1:3 and 1:1 showed significantly better performance than the 3:1 one for overall dechlorination due to their higher atomic metal content and TOF at the same total metal weight load (0.5%).
publishDate 2017
dc.date.none.fl_str_mv 2017
2019
2019
2019
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/10261/182802
url http://hdl.handle.net/10261/182802
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/CTM2014-53008-R
http://dx.doi.org/10.1016/j.jcat.2017.06.013
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 15.811543

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