Rational design of selective metal catalysts ...
Type de document :
Article dans une revue scientifique
URL permanente :
Titre :
Rational design of selective metal catalysts for alcohol amination with ammonia
Auteur(s) :
Wang, Tao [Auteur]
Laboratoire de Chimie - UMR5182 [LC]
Ibañez, Javier [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Wang, Kang [Auteur]
Fang, Lin [Auteur]
Sabbe, Maarten [Auteur]
Universiteit Gent = Ghent University [UGENT]
Michel, Carine [Auteur]
Laboratoire de Chimie - UMR5182 [LC]
PAUL, Sébastien [Auteur]
Centrale Lille
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Pera-Titus, Marc [Auteur]
Sautet, Philippe [Auteur]
University of California [Los Angeles] [UCLA]
Laboratoire de Chimie - UMR5182 [LC]
Ibañez, Javier [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Wang, Kang [Auteur]
Fang, Lin [Auteur]
Sabbe, Maarten [Auteur]
Universiteit Gent = Ghent University [UGENT]
Michel, Carine [Auteur]
Laboratoire de Chimie - UMR5182 [LC]
PAUL, Sébastien [Auteur]
Centrale Lille
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Pera-Titus, Marc [Auteur]
Sautet, Philippe [Auteur]
University of California [Los Angeles] [UCLA]
Titre de la revue :
Nature Catalysis
Date de publication :
2019-09
Discipline(s) HAL :
Chimie/Catalyse
Résumé en anglais : [en]
The lack of selectivity for the direct amination of alcohols with ammonia (a modern and clean route for the synthesis of primary amines) is an unsolved problem. Here, we combine first-principles calculations, scaling ...
Lire la suite >The lack of selectivity for the direct amination of alcohols with ammonia (a modern and clean route for the synthesis of primary amines) is an unsolved problem. Here, we combine first-principles calculations, scaling relations, kinetic simulations and catalysis experiments to determine the key factors that govern the activity and selectivity of metal catalysts for this reaction. We show that the loss of selectivity towards primary amines is linked to a surface-mediated C–N bond coupling between two N-containing intermediates: CH3NH and CH2NH. The barrier for this step is low enough to compete with the main surface hydrogenation reactions and it can be used as a descriptor for selectivity. The activity and selectivity maps (using the C and O adsorption energies as descriptors) were combined for the computational screening of 348 dilute bimetallic catalysts. Among the best theoretical candidates, Co98.5Ag1.5 and Co98.5Ru1.5 (5 wt% Co) were identified experimentally to be the most promising catalysts.Lire moins >
Lire la suite >The lack of selectivity for the direct amination of alcohols with ammonia (a modern and clean route for the synthesis of primary amines) is an unsolved problem. Here, we combine first-principles calculations, scaling relations, kinetic simulations and catalysis experiments to determine the key factors that govern the activity and selectivity of metal catalysts for this reaction. We show that the loss of selectivity towards primary amines is linked to a surface-mediated C–N bond coupling between two N-containing intermediates: CH3NH and CH2NH. The barrier for this step is low enough to compete with the main surface hydrogenation reactions and it can be used as a descriptor for selectivity. The activity and selectivity maps (using the C and O adsorption energies as descriptors) were combined for the computational screening of 348 dilute bimetallic catalysts. Among the best theoretical candidates, Co98.5Ag1.5 and Co98.5Ru1.5 (5 wt% Co) were identified experimentally to be the most promising catalysts.Lire moins >
Langue :
Anglais
Comité de lecture :
Oui
Audience :
Internationale
Vulgarisation :
Non
Établissement(s) :
ENSCL
CNRS
Centrale Lille
Univ. Artois
Université de Lille
CNRS
Centrale Lille
Univ. Artois
Université de Lille
Collections :
Équipe(s) de recherche :
Valorisation des alcanes et de la biomasse (VAALBIO)
Date de dépôt :
2019-09-25T15:12:32Z
2020-10-22T15:18:00Z
2020-10-22T15:18:00Z