The effect of the Mo/W ratio on the catalytic ...
Document type :
Article dans une revue scientifique: Article original
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Title :
The effect of the Mo/W ratio on the catalytic properties of alumina supported hydrotreating catalysts prepared from mixed SiMo6W6 and SiMo9W3 heteropolyacids
Author(s) :
Kokliukhin, A. [Auteur]
Nikulshina, M. [Auteur]
Mozhaev, A. [Auteur]
Lancelot, Christine [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Blanchard, Pascal [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Mentre, Olivier [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Marinova, Maya [Auteur]
Institut Chevreul - FR2638
Lamonier, Carole [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Nikulshin, P. [Auteur]
Nikulshina, M. [Auteur]
Mozhaev, A. [Auteur]
Lancelot, Christine [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Blanchard, Pascal [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Mentre, Olivier [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Marinova, Maya [Auteur]

Institut Chevreul - FR2638
Lamonier, Carole [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Nikulshin, P. [Auteur]
Journal title :
Catalysis Today
Abbreviated title :
Catalysis Today
Volume number :
377
Pages :
100-113
Publication date :
2021-10
ISSN :
09205861
English keyword(s) :
Hydrodesulfurization
hydrogenation
SiMonW12-n HPA
MoW mixed phase
DBT
hydrogenation
SiMonW12-n HPA
MoW mixed phase
DBT
HAL domain(s) :
Chimie/Catalyse
Chimie/Chimie inorganique
Chimie/Chimie inorganique
English abstract : [en]
New mixed H4[SiMonWn-12O40] (n = 6 and 9) Keggin type heteropolyacids (HPAs) have been successfully synthesized, as confirmed by single-crystal XRD, Raman and IR spectroscopy analysis. The resulting polyoxometallates were ...
Show more >New mixed H4[SiMonWn-12O40] (n = 6 and 9) Keggin type heteropolyacids (HPAs) have been successfully synthesized, as confirmed by single-crystal XRD, Raman and IR spectroscopy analysis. The resulting polyoxometallates were used for preparation of hydrotreatment catalysts. Mo(W)/Al2O3 catalysts were synthesized by incipient wetness impregnation of alumina support with water solutions of prepared mixed Keggin HPAs and corresponding counterparts based on mixture of monometallic H4[SiMo12O40] and H4[SiW12O40] HPAs. Oxidic catalysts were analyzed by Raman spectroscopy to determine the precursor structure after deposition. Catalysts in sulfided state were characterized by high-resolution transmission electron microscopy (HRTEM), high angle annular dark field imaging (HAADF) and X-ray photoelectron spectroscopy (XPS) and were tested in co-hydrotreating of dibenzothiophene (DBT) and naphthalene. The use of new mixed Keggin HPAs made it possible to obtain catalysts with mixed MoWS2 active centers, which was confirmed by HAADF. Moreover, the Mo/(Mo+W) ratio has a direct effect on the structure of the active phase species. An ordered core-shell structure with Mo atoms in the core is maintained until the fraction of molybdenum in mixed MoW/Al2O3 catalyst exceeds 50%, where a more disordered structure is observed. Moreover, this Mo/(Mo+W) ratio of 0.5 is optimal to achieve a maximum catalytic activity. Indeed, the turnover frequencies (TOF) of the MoWS2 edge centers with random atoms distribution in a cluster as in Mo9W3/Al2O3, was lower compared to that of Mo6W6/Al2O3 with core-shell structure.Show less >
Show more >New mixed H4[SiMonWn-12O40] (n = 6 and 9) Keggin type heteropolyacids (HPAs) have been successfully synthesized, as confirmed by single-crystal XRD, Raman and IR spectroscopy analysis. The resulting polyoxometallates were used for preparation of hydrotreatment catalysts. Mo(W)/Al2O3 catalysts were synthesized by incipient wetness impregnation of alumina support with water solutions of prepared mixed Keggin HPAs and corresponding counterparts based on mixture of monometallic H4[SiMo12O40] and H4[SiW12O40] HPAs. Oxidic catalysts were analyzed by Raman spectroscopy to determine the precursor structure after deposition. Catalysts in sulfided state were characterized by high-resolution transmission electron microscopy (HRTEM), high angle annular dark field imaging (HAADF) and X-ray photoelectron spectroscopy (XPS) and were tested in co-hydrotreating of dibenzothiophene (DBT) and naphthalene. The use of new mixed Keggin HPAs made it possible to obtain catalysts with mixed MoWS2 active centers, which was confirmed by HAADF. Moreover, the Mo/(Mo+W) ratio has a direct effect on the structure of the active phase species. An ordered core-shell structure with Mo atoms in the core is maintained until the fraction of molybdenum in mixed MoW/Al2O3 catalyst exceeds 50%, where a more disordered structure is observed. Moreover, this Mo/(Mo+W) ratio of 0.5 is optimal to achieve a maximum catalytic activity. Indeed, the turnover frequencies (TOF) of the MoWS2 edge centers with random atoms distribution in a cluster as in Mo9W3/Al2O3, was lower compared to that of Mo6W6/Al2O3 with core-shell structure.Show less >
Language :
Anglais
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
CNRS
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Collections :
Research team(s) :
Catalyse pour l’énergie et la synthèse de molécules plateforme (CEMOP)
Matériaux inorganiques, structures, systèmes et propriétés (MISSP)
Catalyse pour l’énergie et la synthèse de molécules plateforme (CEMOP)
Matériaux inorganiques, structures, systèmes et propriétés (MISSP)
Catalyse pour l’énergie et la synthèse de molécules plateforme (CEMOP)
Submission date :
2022-03-24T09:02:29Z
2023-11-09T08:53:14Z
2023-11-24T09:52:00Z
2023-11-09T08:53:14Z
2023-11-24T09:52:00Z
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