Photocatalytic Dinitrogen Fixation with Water on High-Phosphorus-Doped Carbon Nitride with Surface Nitrogen Vacancies.
Langmuir
; 38(23): 7137-7145, 2022 Jun 14.
Article
em En
| MEDLINE
| ID: mdl-35522588
ABSTRACT
Sunlight-driven photocatalytic dinitrogen (N2) fixation with water at ambient conditions is of vital importance for a sustainable energy society. The efficiency of this reaction, however, is still low because of the difficulty in promoting both water oxidation and N2 reduction reactions. Herein, we report that a high-phosphorus-doped carbon nitride with surface nitrogen vacancies (PCN(V)) synthesized by thermal condensation under a hydrogen (H2) atmosphere using phosphorus oxide (P2O5) as a phosphorus source efficiently promotes N2 fixation. The large numbers of the doped P atoms on the PCN(V)-P2O5 catalysts enhance the oxidation of water, while the N vacancies reduce N2, facilitating efficient ammonia (NH3) generation with an apparent quantum yield at 420 nm of 3.4%. Simulated sunlight illumination of the catalyst in water under N2 bubbling produces NH3 with a solar-to-chemical conversion efficiency of 0.16%, which is the highest efficiency among the previously reported powder photocatalysts.
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MEDLINE
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En
Ano de publicação:
2022
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Article