Artificial Photosynthesis of Alcohols by Multi‐Functionalized Semiconductor Photocathodes

Novel artificial photosynthesis systems are devised as cells of dye/Pd/NR‐MOx (M=Ti, Zn)∥CoPi/W:BiVO4 that convert efficiently CO2 to alcohols. The photocathodes are aminofunctionalized, palladium‐deposited, and in situ sensitized nano‐TiO2 or ZnO/FTO (FTO: fluorine‐doped tin oxide) electrodes that...

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Bibliographic Details
Published in:ChemSusChem 2017-04, Vol.10 (8), p.1742-1748
Main Authors: Zhang, Yuqian, Han, Bo, Xu, Yanjie, Zhao, Dongning, Jia, Yongjian, Nie, Rong, Zhu, Zhouhe, Chen, Fengjuan, Wang, Jianguo, Jing, Huanwang
Format: Article
Language:English
Subjects:
Alcohols
Alcohols - chemical synthesis
artificial photosynthesis
carbon dioxide reduction
Dyes
Electrodes
Ethyl alcohol
Methyl alcohol
Microscopy, Electron, Transmission
Palladium
Photocathodes
photoelectrocatalysis
Photosynthesis
quantum efficiency
Semiconductors
Spectrophotometry, Ultraviolet
water splitting
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Summary:Novel artificial photosynthesis systems are devised as cells of dye/Pd/NR‐MOx (M=Ti, Zn)∥CoPi/W:BiVO4 that convert efficiently CO2 to alcohols. The photocathodes are aminofunctionalized, palladium‐deposited, and in situ sensitized nano‐TiO2 or ZnO/FTO (FTO: fluorine‐doped tin oxide) electrodes that are characterized by X‐ray photoelectron spectroscopy (XPS), TEM, XRD, UV/Vis spectra, and evaluated by electrochemical techniques. The cell of dye/Pd/S‐TiO2∥CoPi/W:BiVO4 uniquely generates ethanol under irradiation of 200 mW cm−2, reaching 0.56 % quantum efficiency (QE) at −0.56 V and 0.13 % QE without external electron supply. The cell of dye/Pd/ N‐ZnO∥CoPi/W:BiVO4 produces solely methanol at a rate of 42.8 μm h−1 cm−2 at −0.56 V of a Si solar cell, which is far less than the electrochemical voltage of water splitting (1.23 V). Its QE reaches to 0.38 %, which is equal to plants. The isotopic labeling experiments confirm the carbon source and oxygen releasing. The selectivity for alcohols of multi‐functionalized semiconductors is discussed. Photo‐prepared alcohols: New artificial photosynthesis cells composed of organic–inorganic composite photocathode consisting of TiO2/ZnO mimicking the photosystem I (PS I) and Calvin cycle and BiVO4 mimicking photosystem II (PS II) are devised, fabricated, and used to convert CO2 to ethanol or methanol as unique product powered by a silica solar cell mimicking the membrane voltage.
ISSN:1864-5631
1864-564X
DOI:10.1002/cssc.201601828