Al2O3 Surface Complexation for Photocatalytic Organic Transformations

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• 作者：Wan Ru Leow ; Wilson Kwok Hung Ng ; Tai Peng ; Xinfeng Liu ; Bin Li ; Wenxiong Shi ; Yanwei Lum ; Xiaotian Wang ; Xianjun LangShuzhou Li ; Nripan MathewsJoel W. Ager ; Tze Chien Sum ; Hajime Hirao ; Xiaodong Chen
• 刊名：Journal of the American Chemical Society
• 出版年：2017
• 出版时间：January 11, 2017
• 年：2017
• 卷：139
• 期：1
• 页码：269-276
• 全文大小：542K
• ISSN：1520-5126

文摘

The use of sunlight to drive organic reactions constitutes a green and sustainable strategy for organic synthesis. Herein, we discovered that the earth-abundant aluminum oxide (Al₂O₃) though paradigmatically known to be an insulator could induce an immense increase in the selective photo-oxidation of different benzyl alcohols in the presence of a large variety of dyes and O₂. This unique phenomenon is based on the surface complexation of benzyl alcohol (BnOH) with the Brønsted base sites on Al₂O₃, which reduces its oxidation potential and causes an upshift in its HOMO for electron abstraction by the dye. The surface complexation of O₂ with Al₂O₃ also activates the adsorbed O₂ for receiving electrons from the photoexcited dyes. This discovery brings forth a new understanding on utilizing surface complexation mechanisms between the reactants and earth abundant materials to effectively achieve a wider range of photoredox reactions.