Molecular Engineering of Trifunctional Supported Catalysts for the Aerobic Oxidation of Alcohols. Issue 37 (19th July 2016)

• Record Type: Journal Article
• Authors: Fernandes, Antony E.; Riant, Olivier; Jensen, Klavs F.; Jonas, Alain M.
• Is Part Of: Angewandte Chemie international edition. Volume 55:Issue 37(2016)
• Page Start: 11044
• Page End: 11048
• Publication Date: 2016-07-19
• Subjects: alcohol oxidation -- CuAAC -- multifunctional catalysts -- supported catalysis -- synergistic effects; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201603673
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: We describe a simple and general method for the preparation and molecular engineering of supported trifunctional catalysts and their application in the representative Cu/TEMPO/NMI‐catalyzed aerobic oxidation of benzyl alcohol. The methodology allows in one single step to immobilize, with precise control of surface composition, both pyta, Cu I, TEMPO, and NMI sites on azide‐functionalized silica particles. To optimize the performance of the heterogeneous trifunctional catalysts, synergistic interactions are finely engineered through modulating the degree of freedom of the imidazole site as well as tuning the relative surface composition, leading to catalysts with an activity significantly superior to the corresponding homogeneous catalytic system. Abstract : A simple and modular strategy is reported for the preparation and engineering of trifunctional supported catalysts bearing Cu, TEMPO, and NMI sites for application in the aerobic oxidation of alcohols. Variation of the linker length on the NMI component and optimization of surface composition allowed synergistic interactions to be tailored for optimal activity and recycling.