Al2O3 Surface Complexation for Photocatalytic Organic Transformations,Journal of the American Chemical Society

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Al2O3 Surface Complexation for Photocatalytic Organic Transformations
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2016-12-29 , DOI: 10.1021/jacs.6b09934
Wan Ru Leow ₁ , Wilson Kwok Hung Ng ₂ , Tai Peng ₁ , Xinfeng Liu ₂ , Bin Li ₁ , Wenxiong Shi ₁ , Yanwei Lum _{3,

4} , Xiaotian Wang ₁ , Xianjun Lang ₁ , Shuzhou Li ₁ , Nripan Mathews ₁ , Joel W. Ager _{3,

4} , Tze Chien Sum ₂ , Hajime Hirao ₂ , Xiaodong Chen ₁

Affiliation

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.

中文翻译：

用于光催化有机转化的 Al2O3 表面络合

利用阳光来驱动有机反应构成了有机合成的绿色和可持续战略。在此，我们发现地球上含量丰富的氧化铝 (Al2O3) 尽管通常被认为是绝缘体，但在存在多种染料和 O2 的情况下，可以极大地增加不同苯甲醇的选择性光氧化。这种独特的现象是基于苯甲醇 (BnOH) 与 Al2O3 上的 Brønsted 碱位点的表面络合，这降低了其氧化电位并导致其 HOMO 上移以用于染料的电子提取。O2 与 Al2O3 的表面络合也激活了吸附的 O2 以接收来自光激发染料的电子。

更新日期：2016-12-29

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