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Photocatalytic deoxygenation of N–O bonds with Rhenium complexes: from the reduction of nitrous oxide to pyridine N-oxides

Marianne Kjellberg 1 Alexia Ohleier 1 Pierre Thuéry 1 Emmanuel Nicolas 1 Lucile Anthore-Dalion 1 Thibault Cantat 1
1 LCMCE - Laboratoire de Chimie Moléculaire et de Catalyse pour l'Energie (ex LCCEF)
NIMBE UMR 3685 - Nanosciences et Innovation pour les Matériaux, la Biomédecine et l'Energie (ex SIS2M)
Abstract : The accumulation of nitrogen oxides in the environment calls for new pathways to interconvert the various oxidation states of nitrogen, and especially their reduction. However, the large spectrum of reduction potentials covered by nitrogen oxides makes it difficult to find general systems capable of efficiently reducing various N-oxides. Here,photocatalysis unlocks high energy species able both tocircumvent the inherent low reactivity of the greenhouse gas and oxidant N$_2$O (E°(N$_2$O/N$_2$) = +1.77V vs. SHE), and toreduce pyridine N-oxides (E$_{1/2}$(pyridine N-oxide/pyridine)=–1.04V vs.SHE). The rhenium complex [Re(4,4’-tBu-bpy)(CO)$_3$Cl] proved to be efficient in performingboth reactions under ambient conditions, enabling the deoxygenation of N$_2$O as well as synthetically relevant and functionalized pyridine N-oxides.
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Submitted on : Monday, July 5, 2021 - 7:19:21 AM
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Marianne Kjellberg, Alexia Ohleier, Pierre Thuéry, Emmanuel Nicolas, Lucile Anthore-Dalion, et al.. Photocatalytic deoxygenation of N–O bonds with Rhenium complexes: from the reduction of nitrous oxide to pyridine N-oxides. Chemical Science , The Royal Society of Chemistry, 2021, 2021, Accepted manuscrit. ⟨10.1039/D1SC01974K⟩. ⟨cea-03277737⟩

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