Al2O3 Surface Complexation for Photocatalytic Organic Transformations

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 o...

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Main Authors: Leow, Wan Ru, Ng, Wilson Kwok Hung, Peng, Tai, Liu, Xinfeng, Li, Bin, Shi, Wenxiong, Lum, Yanwei, Wang, Xiaotian, Sum, Tze Chien, Hirao, Hajime, Chen, Xiaodong, Lang, Xianjun, Li, Shuzhou, Mathews, Nripan, Ager, Joel W.
Other Authors: School of Materials Science & Engineering
Format: Journal Article
Language:English
Published: 2017
Online Access:https://hdl.handle.net/10356/83308
http://hdl.handle.net/10220/42517
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author Leow, Wan Ru
Ng, Wilson Kwok Hung
Peng, Tai
Liu, Xinfeng
Li, Bin
Shi, Wenxiong
Lum, Yanwei
Wang, Xiaotian
Sum, Tze Chien
Hirao, Hajime
Chen, Xiaodong
Lang, Xianjun
Li, Shuzhou
Mathews, Nripan
Ager, Joel W.
author2 School of Materials Science & Engineering
author_facet School of Materials Science & Engineering
Leow, Wan Ru
Ng, Wilson Kwok Hung
Peng, Tai
Liu, Xinfeng
Li, Bin
Shi, Wenxiong
Lum, Yanwei
Wang, Xiaotian
Sum, Tze Chien
Hirao, Hajime
Chen, Xiaodong
Lang, Xianjun
Li, Shuzhou
Mathews, Nripan
Ager, Joel W.
author_sort Leow, Wan Ru
collection NTU
description 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.
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spelling ntu-10356/833082020-06-01T10:01:32Z Al2O3 Surface Complexation for Photocatalytic Organic Transformations Leow, Wan Ru Ng, Wilson Kwok Hung Peng, Tai Liu, Xinfeng Li, Bin Shi, Wenxiong Lum, Yanwei Wang, Xiaotian Sum, Tze Chien Hirao, Hajime Chen, Xiaodong Lang, Xianjun Li, Shuzhou Mathews, Nripan Ager, Joel W. School of Materials Science & Engineering School of Physical and Mathematical Sciences 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. NRF (Natl Research Foundation, S’pore) MOE (Min. of Education, S’pore) 2017-05-30T02:04:32Z 2019-12-06T15:19:41Z 2017-05-30T02:04:32Z 2019-12-06T15:19:41Z 2016 2016 Journal Article Leow, W. R., Ng, W. K. H., Peng, T., Liu, X., Li, B., Shi, W., et al. (2017). Al2O3 Surface Complexation for Photocatalytic Organic Transformations. Journal of the American Chemical Society, 139(1), 269-276. 0002-7863 https://hdl.handle.net/10356/83308 http://hdl.handle.net/10220/42517 10.1021/jacs.6b09934 201160 en Journal of the American Chemical Society © 2016 American Chemical Society
spellingShingle Leow, Wan Ru
Ng, Wilson Kwok Hung
Peng, Tai
Liu, Xinfeng
Li, Bin
Shi, Wenxiong
Lum, Yanwei
Wang, Xiaotian
Sum, Tze Chien
Hirao, Hajime
Chen, Xiaodong
Lang, Xianjun
Li, Shuzhou
Mathews, Nripan
Ager, Joel W.
Al2O3 Surface Complexation for Photocatalytic Organic Transformations
title Al2O3 Surface Complexation for Photocatalytic Organic Transformations
title_full Al2O3 Surface Complexation for Photocatalytic Organic Transformations
title_fullStr Al2O3 Surface Complexation for Photocatalytic Organic Transformations
title_full_unstemmed Al2O3 Surface Complexation for Photocatalytic Organic Transformations
title_short Al2O3 Surface Complexation for Photocatalytic Organic Transformations
title_sort al2o3 surface complexation for photocatalytic organic transformations
url https://hdl.handle.net/10356/83308
http://hdl.handle.net/10220/42517
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