化学
电子转移
吸附
析氧
水溶液
光化学
氧气
氧化还原
太阳能燃料
苯甲醛
选择性
电化学
无机化学
化学工程
材料科学
催化作用
电极
物理化学
光催化
有机化学
工程类
作者
He Li,Cheng Lin,Yaping Yang,Chaoran Dong,Yulin Min,Xiaoqing Shi,Luyang Wang,Siyu Lu,Kan Zhang
标识
DOI:10.1002/anie.202210804
摘要
Water oxidation reaction leaves room to be improved in the development of various solar fuel productions, because of the kinetically sluggish 4-electron transfer process of oxygen evolution reaction. In this work, we realize reactive oxygen species (ROS), H2 O2 and OH⋅, formations by water oxidation with total Faraday efficiencies of more than 90 % by using inter-facet edge (IFE) rich WO3 arrays in an electrolyte containing CO32- . Our results demonstrate that the IFE favors the adsorption of CO32- while reducing the adsorption energy of OH⋅, as well as suppresses surface hole accumulation by direct 1-electron and indirect 2-electron transfer pathways. Finally, we present selective oxidation of benzyl alcohol by in situ using the formed OH⋅, which delivers a benzaldehyde production rate of ≈768 μmol h-1 with near 100 % selectivity. This work offers a promising approach to tune or control the oxidation reaction in an aqueous solar fuel system towards high efficiency and value-added product.
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