期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 17, 页码 9546-9552出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202101058
关键词
CH3OH-to-HCHO conversion; Fe-O-Mo; heterojunction; PEC
资金
- Natural Science Foundation of China [21875048]
- Outstanding Youth Project of Guangdong Natural Science Foundation [2020B1515020028]
- Yangcheng Scholars Research Project of Guangzhou [201831820]
- Science and Technology Research Project of Guangzhou [202002010007]
The study demonstrated the application of a Fe2O3/MoO3 heterojunction in the photoelectrocatalytic conversion of small-molecule alcohols, enhancing the optical carrier transfer rate and optimizing selectivity by constructing interfacial internal electric fields and charge transfer channels. FeMo-2 showed significantly improved performance compared to single Fe2O3, indicating a significant advantage in selectivity and reactivity for HCHO.
The catalytic conversion of alcohols under mild conditions is a great challenge because it is constrained by low selectivity and low activity. Herein, we demonstrate a hollow nanotube Fe2O3/MoO3 heterojunction (FeMo-2) for the photoelectrocatalytic conversion of small-molecule alcohols. Experimental and theoretical analyses reveal that the optical carrier transfer rate is enhanced by constructing interfacial internal electric fields and Fe-O-Mo charge transfer channels. For the formox process, heterojunctions possess superior HCHO-selective reaction paths and free energy transitions, optimizing the selectivity of HCHO and enhancing the reactivity. FeMo-2 shows a greatly improved performance compared to single Fe2O3; the photocurrent density of FeMo-2 reaches 0.66 mA cm(-2), which is 3.88 times that of Fe2O3 (0.17 mA cm(-2)), and the Faraday efficiency of the CH3OH-to-HCHO conversion is 95.7 %. This work may deepen our understanding of interfacial charge separation and has potential for the production of HCHO and for conversion reactions of other small-molecule alcohols at cryogenic temperatures.
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