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

Autores
Bedia, J.; Arevalo Bastante, A.; Grau, Javier Mario; Dosso, Liza Ainalen; Rodriguez, J.J.; Mayoral, A.; Diaz, I.; Gómez Sainero, L.M.
Año de publicación
2017
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
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 N2 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−1 and apparent activation energies between ≈41 and 44 kJ·mol−1 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%).
Fil: Bedia, J.. Universidad Autónoma de Madrid; España
Fil: Arevalo Bastante, A.. Universidad Autónoma de Madrid; España
Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Dosso, Liza Ainalen. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Rodriguez, J.J.. Universidad Autónoma de Madrid; España
Fil: Mayoral, A.. Universidad de Zaragoza; España
Fil: Diaz, I.. Instituto de Catálisis y Petroleoquímica; España
Fil: Gómez Sainero, L.M.. Universidad Autónoma de Madrid; España
Materia
Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated Zirconia
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/63490
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/63490
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
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, Javier MarioDosso, Liza AinalenRodriguez, J.J.Mayoral, A.Diaz, I.Gómez Sainero, L.M.ChloromethanesHydrodechlorinationPalladiumPlatinumSulfated Zirconiahttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2Bimetallic 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 N2 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−1 and apparent activation energies between ≈41 and 44 kJ·mol−1 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%).Fil: Bedia, J.. Universidad Autónoma de Madrid; EspañaFil: Arevalo Bastante, A.. Universidad Autónoma de Madrid; EspañaFil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Dosso, Liza Ainalen. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Rodriguez, J.J.. Universidad Autónoma de Madrid; EspañaFil: Mayoral, A.. Universidad de Zaragoza; EspañaFil: Diaz, I.. Instituto de Catálisis y Petroleoquímica; EspañaFil: Gómez Sainero, L.M.. Universidad Autónoma de Madrid; EspañaAcademic Press Inc Elsevier Science2017-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/63490Bedia, J.; Arevalo Bastante, A.; Grau, Javier Mario; Dosso, Liza Ainalen; Rodriguez, J.J.; et al.; Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes; Academic Press Inc Elsevier Science; Journal of Catalysis; 352; 8-2017; 562-5710021-9517CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://linkinghub.elsevier.com/retrieve/pii/S0021951717302208info:eu-repo/semantics/altIdentifier/doi/10.1016/j.jcat.2017.06.013info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:08:25Zoai:ri.conicet.gov.ar:11336/63490instacron: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:34982025-09-03 10:08:25.928CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
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, Javier Mario
Dosso, Liza Ainalen
Rodriguez, J.J.
Mayoral, A.
Diaz, I.
Gómez Sainero, L.M.
author Bedia, J.
author_facet Bedia, J.
Arevalo Bastante, A.
Grau, Javier Mario
Dosso, Liza Ainalen
Rodriguez, J.J.
Mayoral, A.
Diaz, I.
Gómez Sainero, L.M.
author_role author
author2 Arevalo Bastante, A.
Grau, Javier Mario
Dosso, Liza Ainalen
Rodriguez, J.J.
Mayoral, A.
Diaz, I.
Gómez Sainero, L.M.
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated Zirconia
topic Chloromethanes
Hydrodechlorination
Palladium
Platinum
Sulfated Zirconia
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv 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 N2 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−1 and apparent activation energies between ≈41 and 44 kJ·mol−1 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%).
Fil: Bedia, J.. Universidad Autónoma de Madrid; España
Fil: Arevalo Bastante, A.. Universidad Autónoma de Madrid; España
Fil: Grau, Javier Mario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Dosso, Liza Ainalen. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Rodriguez, J.J.. Universidad Autónoma de Madrid; España
Fil: Mayoral, A.. Universidad de Zaragoza; España
Fil: Diaz, I.. Instituto de Catálisis y Petroleoquímica; España
Fil: Gómez Sainero, L.M.. Universidad Autónoma de Madrid; España
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 N2 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−1 and apparent activation energies between ≈41 and 44 kJ·mol−1 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 2017-08
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/11336/63490
Bedia, J.; Arevalo Bastante, A.; Grau, Javier Mario; Dosso, Liza Ainalen; Rodriguez, J.J.; et al.; Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes; Academic Press Inc Elsevier Science; Journal of Catalysis; 352; 8-2017; 562-571
0021-9517
CONICET Digital
CONICET
url http://hdl.handle.net/11336/63490
identifier_str_mv Bedia, J.; Arevalo Bastante, A.; Grau, Javier Mario; Dosso, Liza Ainalen; Rodriguez, J.J.; et al.; Effect of the Pt–Pd molar ratio in bimetallic catalysts supported on sulfated zirconia on the gas-phase hydrodechlorination of chloromethanes; Academic Press Inc Elsevier Science; Journal of Catalysis; 352; 8-2017; 562-571
0021-9517
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://linkinghub.elsevier.com/retrieve/pii/S0021951717302208
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.jcat.2017.06.013
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Academic Press Inc Elsevier Science
publisher.none.fl_str_mv Academic Press Inc Elsevier Science
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 13.13397

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