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Spatial intimacy of binary active-sites for selective sequential hydrogenation-condensation of nitriles into secondary imines.
- Source :
- Nature Communications; 6/7/2021, Vol. 12 Issue 1, p1-8, 8p
- Publication Year :
- 2021
-
Abstract
- Precisely controlling the spatial intimacy of multiple active sites at sub-nanoscale in heterogeneous catalysts can improve their selectivity and activity. Herein, we realize a highly selective nitrile-to-secondary imine transformation through a cascaded hydrogenation and condensation process by Pt<subscript>1</subscript>/CoBO<subscript>x</subscript> comprising the binary active sites of the single-dispersed Pt and interfacial Lewis acidic B. Atomic Pt sites with large inter-distances (>nanometers) only activate hydrogen for nitrile hydrogenation, but inhibit condensation. Both adjacent B...B on CoBO<subscript>x</subscript> and neighbouring Pt...B pairs with close intimacy of ~0.45 nm can satisfy the spatial prerequisites for condensation. Mechanism investigations demonstrate the energetically favorable pathway occurred on adjacent Lewis acidic B sites through the nitrile adsorption (acid-base interaction), hydrogenation via hydrogen spillover from Pt to B sites and sequential condensation. Strong intermolecular tension and steric hindrance of secondary imines on active sites lead to their effective desorption and thereby a high chemoselectivity of secondary imines. Precisely controlling the spatial intimacy of multiple active sites in heterogeneous catalysts can significantly affect the selectivity and activity. Here the authors show a binary active site of single atom Pt and Lewis acidic B with spatial intimacy enables a highly selective nitrile-to-secondary imine transformation. [ABSTRACT FROM AUTHOR]
- Subjects :
- IMINES
STERIC hindrance
NITRILES
CONDENSATION
HYDROGENATION
Subjects
Details
- Language :
- English
- ISSN :
- 20411723
- Volume :
- 12
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Nature Communications
- Publication Type :
- Academic Journal
- Accession number :
- 150747676
- Full Text :
- https://doi.org/10.1038/s41467-021-23705-9