Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts

In this paper NiW/γ-Al2O3catalysts were prepared by consecutive impregnation of a W/γ-Al2O3 catalyst with an aqueous solution of nickel salt. The structural control of the nickel ion precursor in the impregnation solution was achieved by the addition of 1, 2-cyclohexanediamine-N, N, N’, N’-tetraacet...

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Autores: Santolalla-Vargas, C. E., Santes, Victor, Suárez Toriello, V. A., Reyes, José Antonio de los, Pawelec, Bárbara, García Fierro, José Luis, Domínguez Garcia, Elizabeth, Oliviero, L., Maugé, F.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2020
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/231405
Acceso en línea:http://hdl.handle.net/10261/231405
Access Level:acceso abierto
Palabra clave:Hydrodesulfurization
1, 2-cyclohexanediamine-N, N, N”, N”-tetraacetic acid
Nickel
Tungsten
Adsorbed CO
Thiophene
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spelling Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalystsSantolalla-Vargas, C. E.Santes, VictorSuárez Toriello, V. A.Reyes, José Antonio de losPawelec, BárbaraGarcía Fierro, José LuisDomínguez Garcia, ElizabethOliviero, L.Maugé, F.Hydrodesulfurization1, 2-cyclohexanediamine-N, N, N”, N”-tetraacetic acidNickelTungstenAdsorbed COThiopheneIn this paper NiW/γ-Al2O3catalysts were prepared by consecutive impregnation of a W/γ-Al2O3 catalyst with an aqueous solution of nickel salt. The structural control of the nickel ion precursor in the impregnation solution was achieved by the addition of 1, 2-cyclohexanediamine-N, N, N’, N’-tetraacetic acid (CyDTA) as a chelating agent at different pH. The influence of the sulfidation pressure (1 bar vs 40 bar) on the activity and structure of the NiW catalysts was investigated. The catalysts performances were tested in hydrodesulfurization (HDS) of thiophene after sulfidation at atmospheric or high pressure. The catalysts were characterized by X-Ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR) and infrared spectroscopy of adsorbed CO (IR/CO) to explain the modification in surface species composition due to the chelating agent CyDTA and sulfiding conditions. NiW catalysts prepared in presence of CydTA and sulfided under high pressure displayed the highest HDS activity. These two factors enhanced the sulfidation degree of W-based species as characterized by XPS. A linear correlation was found between the HDS activity and the sulfidation degree. In addition, chelating agent addition induced a decrease on metal-support interaction, as pointed out by TPR, and strongly favored the creation of CUS sites on the NiWS phase as seen by IR/CO. All these features favored a high catalytic activity. In addition, high pressure sulfidation not only leads to more active NiW catalysts but improved the butene-over-butane ratio.J.A. de los Reyes and V.A. Suarez Toriello acknowledge CONACYT-SENER funding for financial support. The authors thank financial support from Instituto Politécnico Nacional (Proyecto SIP 20201116 and 20201629) and the Mexican National Council for Science and Technology (CONACyT; project CB-2017-2018 # A1-S-32418).Peer reviewedElsevier BVInstituto Politécnico Nacional (México)Consejo Nacional de Ciencia y Tecnología (México)Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]2021202120202021info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/231405reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Ingléshttp://dx.doi.org/10.1016/j.cattod.2020.07.015Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2314052026-05-22T06:33:51Z
dc.title.none.fl_str_mv Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
title Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
spellingShingle Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
Santolalla-Vargas, C. E.
Hydrodesulfurization
1, 2-cyclohexanediamine-N, N, N”, N”-tetraacetic acid
Nickel
Tungsten
Adsorbed CO
Thiophene
title_short Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
title_full Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
title_fullStr Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
title_full_unstemmed Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
title_sort Effect of sulfidation pressure on the structure and activity of Ni(CyDTA)W/γ-Al2O3 hydrodesulfurization catalysts
dc.creator.none.fl_str_mv Santolalla-Vargas, C. E.
Santes, Victor
Suárez Toriello, V. A.
Reyes, José Antonio de los
Pawelec, Bárbara
García Fierro, José Luis
Domínguez Garcia, Elizabeth
Oliviero, L.
Maugé, F.
author Santolalla-Vargas, C. E.
author_facet Santolalla-Vargas, C. E.
Santes, Victor
Suárez Toriello, V. A.
Reyes, José Antonio de los
Pawelec, Bárbara
García Fierro, José Luis
Domínguez Garcia, Elizabeth
Oliviero, L.
Maugé, F.
author_role author
author2 Santes, Victor
Suárez Toriello, V. A.
Reyes, José Antonio de los
Pawelec, Bárbara
García Fierro, José Luis
Domínguez Garcia, Elizabeth
Oliviero, L.
Maugé, F.
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Instituto Politécnico Nacional (México)
Consejo Nacional de Ciencia y Tecnología (México)
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Hydrodesulfurization
1, 2-cyclohexanediamine-N, N, N”, N”-tetraacetic acid
Nickel
Tungsten
Adsorbed CO
Thiophene
topic Hydrodesulfurization
1, 2-cyclohexanediamine-N, N, N”, N”-tetraacetic acid
Nickel
Tungsten
Adsorbed CO
Thiophene
description In this paper NiW/γ-Al2O3catalysts were prepared by consecutive impregnation of a W/γ-Al2O3 catalyst with an aqueous solution of nickel salt. The structural control of the nickel ion precursor in the impregnation solution was achieved by the addition of 1, 2-cyclohexanediamine-N, N, N’, N’-tetraacetic acid (CyDTA) as a chelating agent at different pH. The influence of the sulfidation pressure (1 bar vs 40 bar) on the activity and structure of the NiW catalysts was investigated. The catalysts performances were tested in hydrodesulfurization (HDS) of thiophene after sulfidation at atmospheric or high pressure. The catalysts were characterized by X-Ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR) and infrared spectroscopy of adsorbed CO (IR/CO) to explain the modification in surface species composition due to the chelating agent CyDTA and sulfiding conditions. NiW catalysts prepared in presence of CydTA and sulfided under high pressure displayed the highest HDS activity. These two factors enhanced the sulfidation degree of W-based species as characterized by XPS. A linear correlation was found between the HDS activity and the sulfidation degree. In addition, chelating agent addition induced a decrease on metal-support interaction, as pointed out by TPR, and strongly favored the creation of CUS sites on the NiWS phase as seen by IR/CO. All these features favored a high catalytic activity. In addition, high pressure sulfidation not only leads to more active NiW catalysts but improved the butene-over-butane ratio.
publishDate 2020
dc.date.none.fl_str_mv 2020
2021
2021
2021
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/10261/231405
url http://hdl.handle.net/10261/231405
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv http://dx.doi.org/10.1016/j.cattod.2020.07.015

dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier BV
publisher.none.fl_str_mv Elsevier BV
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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