Journal
ADVANCED MATERIALS
Volume 29, Issue 31, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201701774
Keywords
Bi5O7Br nanotubes; nitrogen fixation; oxygen vacancies; photocatalysis; visible light
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Funding
- World Premier International Research Center Initiative (WPI Initiative) on Materials Nanoarchitectonics (MANA), MEXT (Japan)
- National Basic Research Program of China (973 Program) [2014CB239301]
- National Science Foundation of China [21633004, 51572101, 21607047, 21502059]
- Fundamental Research Funds for the Central Universities of China [2015PY120, 2015PY047, 2016PY088]
- State Scholarship Fund by China Scholarship Council (CSC) [201406250019, 201606760019]
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Solar-driven reduction of dinitrogen (N-2) to ammonia (NH3) is severely hampered by the kinetically complex and energetically challenging multielectron reaction. Oxygen vacancies (OVs) with abundant localized electrons on the surface of bismuth oxybromide-based semiconductors are demonstrated to have the ability to capture and activate N-2, providing an alternative pathway to overcome such limitations. However, bismuth oxybromide materials are susceptible to photocorrosion, and the surface OVs are easily oxidized and therefore lose their activities. For realistic photocatalytic N-2 fixation, fabricating and enhancing the stability of sustainable OVs on semiconductors is indispensable. This study shows the first synthesis of self-assembled 5 nm diameter Bi5O7Br nanotubes with strong nanotube structure, suitable absorption edge, and many exposed surface sites, which are favorable for furnishing sufficient visible light-induced OVs to realize excellent and stable photoreduction of atmospheric N-2 into NH3 in pure water. The NH3 generation rate is as high as 1.38 mmol h(-1) g(-1), accompanied by an apparent quantum efficiency over 2.3% at 420 nm. The results presented herein provide new insights into rational design and engineering for the creation of highly active catalysts with light-switchable OVs toward efficient, stable, and sustainable visible light N-2 fixation in mild conditions.
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