New insights in single-step hydrodeoxygenation ...
Document type :
Article dans une revue scientifique: Article original
Permalink :
Title :
New insights in single-step hydrodeoxygenation of glycerol to propylene by coupling rational catalyst design with systematic analysis
Author(s) :
El Doukkali, Mohamed [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
PAUL, Sébastien [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Dumeignil, Franck [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
PAUL, Sébastien [Auteur]

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

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Journal title :
Applied Catalysis B: Environmental
Volume number :
324
Pages :
122280
Publication date :
2023-05-05
ISSN :
0926-3373
Keyword(s) :
Rational catalyst design
Mo delta+ active -sites
in-situ/ex-situ analyses
Single-step hydrodeoxygenation
Glycerol -to -propylene routes
Mo delta+ active -sites
in-situ/ex-situ analyses
Single-step hydrodeoxygenation
Glycerol -to -propylene routes
HAL domain(s) :
Chimie/Catalyse
English abstract : [en]
Glycerol-to-propylene routes involve overlapped hydrodeoxygenation (HDO) events on the active sites of heterogeneous catalysts which stability in aqueous media is a challenge. Herein, we proposed a rationalized approach ...
Show more >Glycerol-to-propylene routes involve overlapped hydrodeoxygenation (HDO) events on the active sites of heterogeneous catalysts which stability in aqueous media is a challenge. Herein, we proposed a rationalized approach to develop such catalysts by using hydrophobic-inert silica supports to protect highly reactive sub- 2 nm Mo particles against leaching and sintering. Propylene yield from 84.1% to 65.6% were obtained on MoOx nanoparticles at space-velocity ~1.7 h-1 and H2-pressure ~50 bar. Carburizing MoOx nanoparticles to β-Mo2C leads to an extremely efficient HDO catalyst, featuring, unprecedented TOF!"#!$%&'& ranging from ~153.1 h-1 to 226.4 h-1, while η-MoC phase gave better hydrogenation activity. Coupling in-situ XPS and kinetic data reveal that Mo5+, Mo3+ and Mo2+-C species play a critical role in the HDO events. Glycerol-to- propylene progresses over MoOx via successive Mo5+/Mo6+ and Mo3+/Mo4+ cycles, while over β-Mo2C/η- MoC, it occurs mostly on carbidic-oxycarbide surface. Surface accumulation of CxHyOz species caused Moδ+ re-oxidation, which hinders the HDO eventsShow less >
Show more >Glycerol-to-propylene routes involve overlapped hydrodeoxygenation (HDO) events on the active sites of heterogeneous catalysts which stability in aqueous media is a challenge. Herein, we proposed a rationalized approach to develop such catalysts by using hydrophobic-inert silica supports to protect highly reactive sub- 2 nm Mo particles against leaching and sintering. Propylene yield from 84.1% to 65.6% were obtained on MoOx nanoparticles at space-velocity ~1.7 h-1 and H2-pressure ~50 bar. Carburizing MoOx nanoparticles to β-Mo2C leads to an extremely efficient HDO catalyst, featuring, unprecedented TOF!"#!$%&'& ranging from ~153.1 h-1 to 226.4 h-1, while η-MoC phase gave better hydrogenation activity. Coupling in-situ XPS and kinetic data reveal that Mo5+, Mo3+ and Mo2+-C species play a critical role in the HDO events. Glycerol-to- propylene progresses over MoOx via successive Mo5+/Mo6+ and Mo3+/Mo4+ cycles, while over β-Mo2C/η- MoC, it occurs mostly on carbidic-oxycarbide surface. Surface accumulation of CxHyOz species caused Moδ+ re-oxidation, which hinders the HDO eventsShow less >
Language :
Anglais
Peer reviewed article :
Oui
Audience :
Internationale
Popular science :
Non
European Project :
ANR Project :
Administrative institution(s) :
Université de Lille
CNRS
Centrale Lille
ENSCL
Univ. Artois
CNRS
Centrale Lille
ENSCL
Univ. Artois
Collections :
Research team(s) :
Valorisation des alcanes et de la biomasse (VAALBIO)
Submission date :
2023-10-20T06:56:34Z
2023-11-20T17:39:00Z
2023-11-20T17:39:00Z
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Annexes
- Supporting Info.pdf
- N/A
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