Single-Site Molybdenum on Solid Support Materials for Catalytic Hydrogenation of N2-into-NH3
Correction(s) for this article
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Corrigendum: Molybdenum on Solid Support Materials for Catalytic Hydrogenation of N2-into-NH3
- Luis Miguel Azofra,
- Natalia Morlanés,
- Albert Poater,
- Manoja K. Samantaray,
- Balamurugan Vidjayacoumar,
- Khalid Albahily,
- Luigi Cavallo,
- Jean-Marie Basset,
- Volume 58Issue 20Angewandte Chemie International Edition
- pages: 6476-6476
- First Published online: May 6, 2019
Corresponding Author
Dr. Luis Miguel Azofra
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Natalia Morlanés
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Albert Poater
Institut de Química Computacional i Catàlisi, Departament de Química, Universitat de Girona, Campus de Montilivi, s/n, 17003 Girona, Catalonia, Spain
Search for more papers by this authorDr. Manoja K. Samantaray
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Balamurugan Vidjayacoumar
SABIC (Saudi Basic Industries Corporation), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Khalid Albahily
SABIC (Saudi Basic Industries Corporation), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorCorresponding Author
Prof. Dr. Luigi Cavallo
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorCorresponding Author
Prof. Dr. Jean-Marie Basset
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorCorresponding Author
Dr. Luis Miguel Azofra
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Natalia Morlanés
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Albert Poater
Institut de Química Computacional i Catàlisi, Departament de Química, Universitat de Girona, Campus de Montilivi, s/n, 17003 Girona, Catalonia, Spain
Search for more papers by this authorDr. Manoja K. Samantaray
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Balamurugan Vidjayacoumar
SABIC (Saudi Basic Industries Corporation), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorDr. Khalid Albahily
SABIC (Saudi Basic Industries Corporation), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorCorresponding Author
Prof. Dr. Luigi Cavallo
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorCorresponding Author
Prof. Dr. Jean-Marie Basset
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 Saudi Arabia
Search for more papers by this authorGraphical Abstract
It'll be fixed in a Mo: N2-into-NH3 conversion is one of the most important processes in the chemical industry. A set of molybdenum on solid support materials catalyse N2 fixation under just atmospheric pressure and only 400 °C. They allow for an in-depth elucidation of the mechanistic events taking place which is supported by DFT analysis.
Abstract
Very stable in operando and low-loaded atomic molybdenum on solid-support materials have been prepared and tested to be catalytically active for N2-into-NH3 hydrogenation. Ammonia synthesis is reported at atmospheric pressure and 400 °C with NH3 rates of approximately 1.3×103 μmol h−1 gMo−1 using a well-defined Mo-hydride grafted on silica (SiO2-700). DFT modelling on the reaction mechanism suggests that N2 spontaneously binds on monopodal [(≡Si−O-)MoH3]. Based on calculations, the fourth hydrogenation step involving the release of the first NH3 molecule represents the rate-limiting step of the whole reaction. The inclusion of cobalt co-catalyst and an alkali caesium additive impregnated on a mesoporous SBA-15 support increases the formation of NH3 with rates of circa 3.5×103 μmol h−1 gMo−1 under similar operating conditions and maximum yield of 29×103 μmol h−1 gMo−1 when the pressure is increased to 30 atm.
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