Understanding Aerobic Nitrogen Photooxidation on Titania through In Situ Time-Resolved Spectroscopy.
Angew Chem Int Ed Engl
; 61(51): e202211469, 2022 Dec 19.
Article
en En
| MEDLINE
| ID: mdl-36264279
ABSTRACT
Nitrate is an important raw material for chemical fertilizers, but it is industrially manufactured in multiple steps at high temperature and pressure, urgently motivating the design of a green and sustainable strategy for nitrate production. We report the photosynthesis of nitrate from N2 and O2 on commercial TiO2 in a flow reactor under ambient conditions. The TiO2 photocatalyst offered a high nitrate yield of 1.85â
µmol h-1 as well as a solar-to-nitrate energy conversion efficiency up to 0.13 %. We combined reactivity and in situ Fourier transform infrared spectroscopy to elucidate the mechanism of nitrate formation and unveil the special role of O2 in N≡N bond dissociation. The mechanistic insight into charge-involved N2 oxidation was further demonstrated by in situ transient absorption spectroscopy and electron paramagnetic resonance. This work exhibits the mechanistic origin of N2 photooxidation and initiates a potential method for triggering inert catalytic reactions.
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MEDLINE
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En
Revista:
Angew Chem Int Ed Engl
Año:
2022
Tipo del documento:
Article
País de afiliación:
China