期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 16, 页码 7574-7583出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c01683
关键词
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资金
- Precursory Research for Embryonic Science and Technology (PRESTO) [JPMJPR1442]
- Japan Science and Technology Agency (JST) [19H02516]
- Ministry of Education, Culture, Sports, Science and Technology, Japan (MEXT)
- Grants-in-Aid for Scientific Research [19H02516] Funding Source: KAKEN
Ammonia is an indispensable chemical. Photocatalytic NH3 production via dinitrogen fixation using water by sunlight illumination under ambient conditions is a promising strategy, although previously reported catalysts show insufficient activity. Herein, we showed that ultraviolet light irradiation of a semiconductor, bismuth oxychloride with surface oxygen vacancies (BiOCl-OVs), in water containing chloride anions (Cl-) under N-2 flow efficiently produces NH3. The surface OVs behave as the N-2 reduction sites by the photoformed conduction band electrons. The valence band holes are consumed by self-oxidation of interlayer Cl- on the catalyst. The hypochloric acid (HClO) formed absorbs ultraviolet light and undergoes photodecomposition into O-2 and Cl-. These consecutive photoreactions produce NH3 with water as the electron donor. The Cl- in solution compensates for the removed interlayer Cl- and inhibits catalyst deactivation. Simulated sunlight illumination of the catalyst in seawater stably generates NH3 with 0.05% solar-to-chemical conversion efficiency, thus exhibiting significant potential of the seawater system for artificial photosynthesis.
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