1. Aerobic Oxidative Synthesis of Formamides from Amines and Bioderived Formyl Surrogates.
- Author
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Dai X, Han Y, Jiao H, Shi F, Rabeah J, and Brückner A
- Abstract
Herein we present a new strategy for the oxidative synthesis of formamides from various types of amines and bioderived formyl sources (DHA, GLA and GLCA) and molecular oxygen (O
2 ) as oxidant on g-C3 N4 supported Cu catalysts. Combined characterization data from EPR, XAFS, XRD and XPS revealed the formation of single CuN4 sites on supported Cuphen /C3 N4 catalysts. EPR spin trapping experiments disclosed ⋅OOH radicals as reactive oxygen species and ⋅NR1 R2 radicals being responsible for the initial C-C bond cleavage. Control experiments and DFT calculations showed that the successive C-C bond cleavage in DHA proceeds via a reaction mechanism co-mediated by ⋅NR1 R2 and ⋅OOH radicals based on the well-equilibrated CuII and CuI cycle. Our catalyst has much higher activity (TOF) than those based on noble metals., (© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)- Published
- 2024
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