Aerobic Oxidative Synthesis of Formamides from Amines and Bioderived Formyl Surrogates.
Angew Chem Int Ed Engl
; 63(26): e202402241, 2024 Jun 21.
Article
em En
| MEDLINE
| ID: mdl-38567831
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 (O2) as oxidant on g-C3N4 supported Cu catalysts. Combined characterization data from EPR, XAFS, XRD and XPS revealed the formation of single CuN4 sites on supported Cuphen/C3N4 catalysts. EPR spin trapping experiments disclosed â
OOH radicals as reactive oxygen species and â
NR1R2 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 â
NR1R2 and â
OOH radicals based on the well-equilibrated CuII and CuI cycle. Our catalyst has much higher activity (TOF) than those based on noble metals.
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MEDLINE
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En
Ano de publicação:
2024
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Article