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Abstract:
N2 reduction reaction (NRR) by light is an energy-saving and sustainable ammonia (NH3) synthesis technology. However, it faces significant challenges, including high energy barriers of N2 activation and unclear catalytic active sites. Herein, we propose a strategy of photo-driven ammonia synthesis via a proton-mediated photoelectrochemical device. We used redox-catalysis covalent organic framework (COF), with a redox site (−C=O) for H+ reversible storage and a catalytic site (porphyrin Au) for NRR. In the proton-mediated photoelectrochemical device, the COF can successfully store e− and H+ generated by hydrogen oxidation reaction, forming COF−H. Then, these stored e− and H+ can be used for photo-driven NRR (108.97 umol g−1) under low proton concentration promoted by the H-bond network formed between −OH in COF−H and N2 on Au, which enabled N2 hydrogenation and NH3 production, establishing basis for advancing artificial photosynthesis and enhancing ammonia synthesis technology. © 2025 Wiley-VCH GmbH.
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Angewandte Chemie - International Edition
ISSN: 1433-7851
Year: 2025
Issue: 8
Volume: 64
1 6 . 1 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 3
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