4.8 Article

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

Journal

CHEMICAL SCIENCE
Volume 12, Issue 30, Pages 10266-10272

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1sc01974k

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Funding

  1. CEA
  2. CNRS
  3. ERC [818260]
  4. Institut de France
  5. LABEX Charmmmat
  6. ADEME
  7. European Research Council (ERC) [818260] Funding Source: European Research Council (ERC)

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The accumulation of nitrogen oxides in the environment requires new pathways for interconverting different oxidation states of nitrogen and particularly their reduction; photocatalysis plays a key role in this, efficiently reducing various types of nitrogen oxides.
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 to circumvent the inherent low reactivity of the greenhouse gas and oxidant N2O (E-0(N2O/N-2) = +1.77 V vs. SHE), and to reduce pyridine N-oxides (E-1/2(pyridine N-oxide/pyridine) = -1.04 V vs. SHE). The rhenium complex [Re(4,40-tBu-bpy)(CO)(3)Cl] proved to be efficient in performing both reactions under ambient conditions, enabling the deoxygenation of N2O as well as synthetically relevant and functionalized pyridine N-oxides.

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