Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production

A series of materials based on the immobilization of the 12-tungstophosphoric heteropolyacid over zirconia supports have been prepared and applied as heterogeneous acid catalysts in the esterification of palmitic acid with methanol as a model reaction for the preliminary stage of the biodiesel produ...

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Autores: Alcañiz Monge, Juan, El Bakkali, Bouchra, Trautwein, Guido, Reinoso, Santiago
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Universidad Pública de Navarra
Repositorio:Academica-e. Repositorio Institucional de la Universidad Pública de Navarra
OAI Identifier:oai:academica-e.unavarra.es:2454/38633
Acceso en línea:https://hdl.handle.net/2454/38633
Access Level:acceso abierto
Palabra clave:Immobilized heteropolyacid
Zirconia support
Textural properties
Palmitic acid esterification
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spelling Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel productionAlcañiz Monge, JuanEl Bakkali, BouchraTrautwein, GuidoReinoso, SantiagoImmobilized heteropolyacidZirconia supportTextural propertiesPalmitic acid esterificationA series of materials based on the immobilization of the 12-tungstophosphoric heteropolyacid over zirconia supports have been prepared and applied as heterogeneous acid catalysts in the esterification of palmitic acid with methanol as a model reaction for the preliminary stage of the biodiesel production. The title materials have been obtained through the sol-gel method combined with a subsequent hydrothermal treatment at mild conditions, which affords catalysts with larger porosity and higher thermal and chemical stability under the esterification reaction conditions than other preparative approaches. Generating the zirconia support by hydrolysis of an alkoxyde precursor in the presence of the heteropolyacid leads to materials with homogeneously well-dispersed clusters, as well as to an increasing contribution of the tetragonal ZrO2 crystalline phase, a decreasing size of the nanoparticles and larger microporous volumes as the loading of the Keggin-type species increases. The 12-tungstophosphoric acid retains its catalytic activity in the esterification of palmitic acid with methanol at 60 °C upon immobilization over zirconia and conversions even higher than those observed under homogeneous conditions are obtained due to the active contribution of the support. The sample with a 30% mass percentage of heteropolyacid has been identified as the most efficient catalyst because it affords conversions above the 90% and shows the lower loss of activity over successive reaction runs among all of our materials. This loss of activity has been analyzed on the basis of the leaching of the catalyst and the fouling of the materials.This work was financially supported by Generalitat Valenciana through FEDER funds (grant PROMETEO2/2014/010) and by the Spanish Ministerio de Economía y Competitividad (grant CTQ2015-64801-R). S.R. acknowledges financial support from InaMat and from the program 'Ayudas para la Captación del Talento adscritas a los Institutos de Investigación de la UPNA' funded by a collaboration agreement with Obra Social la Caixa and Fundación Caja Navarra.ElsevierInstitute for Advanced Materials and Mathematics - INAMAT2Universidad Pública de Navarra / Nafarroako Unibertsitate Publikoa2018info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttps://hdl.handle.net/2454/38633reponame:Academica-e. Repositorio Institucional de la Universidad Pública de Navarrainstname:Universidad Pública de NavarraInglésinfo:eu-repo/grantAgreement/MINECO//CTQ2015-64801-R© 2017 Elsevier B.V. This manuscript version is made available under the CC-BY-NC-ND 4.0https://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:academica-e.unavarra.es:2454/386332026-06-17T12:41:47Z
dc.title.none.fl_str_mv Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
title Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
spellingShingle Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
Alcañiz Monge, Juan
Immobilized heteropolyacid
Zirconia support
Textural properties
Palmitic acid esterification
title_short Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
title_full Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
title_fullStr Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
title_full_unstemmed Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
title_sort Zirconia-supported tungstophosphoric heteropolyacid as heterogeneous acid catalyst for biodiesel production
dc.creator.none.fl_str_mv Alcañiz Monge, Juan
El Bakkali, Bouchra
Trautwein, Guido
Reinoso, Santiago
author Alcañiz Monge, Juan
author_facet Alcañiz Monge, Juan
El Bakkali, Bouchra
Trautwein, Guido
Reinoso, Santiago
author_role author
author2 El Bakkali, Bouchra
Trautwein, Guido
Reinoso, Santiago
author2_role author
author
author
dc.contributor.none.fl_str_mv Institute for Advanced Materials and Mathematics - INAMAT2
Universidad Pública de Navarra / Nafarroako Unibertsitate Publikoa
dc.subject.none.fl_str_mv Immobilized heteropolyacid
Zirconia support
Textural properties
Palmitic acid esterification
topic Immobilized heteropolyacid
Zirconia support
Textural properties
Palmitic acid esterification
description A series of materials based on the immobilization of the 12-tungstophosphoric heteropolyacid over zirconia supports have been prepared and applied as heterogeneous acid catalysts in the esterification of palmitic acid with methanol as a model reaction for the preliminary stage of the biodiesel production. The title materials have been obtained through the sol-gel method combined with a subsequent hydrothermal treatment at mild conditions, which affords catalysts with larger porosity and higher thermal and chemical stability under the esterification reaction conditions than other preparative approaches. Generating the zirconia support by hydrolysis of an alkoxyde precursor in the presence of the heteropolyacid leads to materials with homogeneously well-dispersed clusters, as well as to an increasing contribution of the tetragonal ZrO2 crystalline phase, a decreasing size of the nanoparticles and larger microporous volumes as the loading of the Keggin-type species increases. The 12-tungstophosphoric acid retains its catalytic activity in the esterification of palmitic acid with methanol at 60 °C upon immobilization over zirconia and conversions even higher than those observed under homogeneous conditions are obtained due to the active contribution of the support. The sample with a 30% mass percentage of heteropolyacid has been identified as the most efficient catalyst because it affords conversions above the 90% and shows the lower loss of activity over successive reaction runs among all of our materials. This loss of activity has been analyzed on the basis of the leaching of the catalyst and the fouling of the materials.
publishDate 2018
dc.date.none.fl_str_mv 2018
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2454/38633
url https://hdl.handle.net/2454/38633
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/MINECO//CTQ2015-64801-R
dc.rights.none.fl_str_mv © 2017 Elsevier B.V. This manuscript version is made available under the CC-BY-NC-ND 4.0
https://creativecommons.org/licenses/by-nc-nd/4.0/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv © 2017 Elsevier B.V. This manuscript version is made available under the CC-BY-NC-ND 4.0
https://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:Academica-e. Repositorio Institucional de la Universidad Pública de Navarra
instname:Universidad Pública de Navarra
instname_str Universidad Pública de Navarra
reponame_str Academica-e. Repositorio Institucional de la Universidad Pública de Navarra
collection Academica-e. Repositorio Institucional de la Universidad Pública de Navarra
repository.name.fl_str_mv
repository.mail.fl_str_mv
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