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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Detalles Bibliográficos
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
Descripción
Sumario: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.