The conversion of dinitrogen to more useful and reactive molecules has been the focus of intense research by chemists. In contrast to reductive N 2 fixation, direct oxidation of N 2 by O 2 to nitric oxide under mild conditions via a thermochemical process is extremely challenging. Herein, we report the first example of N 2 and O 2 activation and coupling under thermochemical conditions through the remarkable ability of Y 2 BO + to react with one N 2 and two O 2 molecules. Detailed mechanistic studies using mass spectrometry and quantum chemical calculations revealed that the N 2 activation by Y 2 BO + is facilitated by the double aromatic character of the Y 2 BON 2 + intermediate. Subsequent oxidation with O 2 releases NO in a dearomatization process driven by the formation of stronger Y-O bonds over the Y-N bonds. Our findings represent the first example of N 2 and O 2 activation and coupling under thermochemical conditions at room temperature, providing a novel strategy for small-molecule activation.
Keyphrases
- room temperature
- nitric oxide
- ionic liquid
- small molecule
- hydrogen peroxide
- mass spectrometry
- magnetic resonance
- molecular dynamics
- computed tomography
- high resolution
- magnetic resonance imaging
- liquid chromatography
- minimally invasive
- single cell
- molecular dynamics simulations
- contrast enhanced
- protein protein
- quantum dots
- transition metal