Rational design of selective metal catalysts ...
Document type :
Article dans une revue scientifique
Permalink :
Title :
Rational design of selective metal catalysts for alcohol amination with ammonia
Author(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]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Centrale Lille
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]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Centrale Lille
Pera-Titus, Marc [Auteur]
Sautet, Philippe [Auteur]
University of California [Los Angeles] [UCLA]
Journal title :
Nature Catalysis
Publication date :
2019-09
HAL domain(s) :
Chimie/Catalyse
English abstract : [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 ...
Show more >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.Show less >
Show more >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.Show less >
Language :
Anglais
Peer reviewed article :
Oui
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
ENSCL
CNRS
Centrale Lille
Univ. Artois
Université de Lille
CNRS
Centrale Lille
Univ. Artois
Université de Lille
Collections :
Research team(s) :
Valorisation des alcanes et de la biomasse (VAALBIO)
Submission date :
2019-09-25T15:12:32Z
2020-10-22T15:18:00Z
2020-10-22T15:18:00Z