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Photocatalytic Cascade Reaction Driven by Directed Charge Transfer over VS-Zn0.5Cd0.5S/GO for Controllable Benzyl Oxidation
Advanced Science ( IF 14.3 ) Pub Date : 2023-05-01 , DOI: 10.1002/advs.202207250 Xue Bai 1 , Mengyao She 1, 2 , Yali Ji 1 , Zhe Zhang 1 , Wenhua Xue 3 , Enzhou Liu 3 , Kerou Wan 4 , Ping Liu 1 , Shengyong Zhang 1 , Jianli Li 1
Advanced Science ( IF 14.3 ) Pub Date : 2023-05-01 , DOI: 10.1002/advs.202207250 Xue Bai 1 , Mengyao She 1, 2 , Yali Ji 1 , Zhe Zhang 1 , Wenhua Xue 3 , Enzhou Liu 3 , Kerou Wan 4 , Ping Liu 1 , Shengyong Zhang 1 , Jianli Li 1
Affiliation
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Photocatalysis is an important technique for synthetic transformations. However, little attention has been paid to light-driven synergistic redox reactions for directed synthesis. Herein, the authors report tunable oxidation of benzyl to phenylcarbinol with the modest yield (47%) in 5 h via singlet oxygen (1O2) and proton-coupled electron transfer (PCET) over the photocatalyst Zn0.5Cd0.5S (ZCS)/graphene oxide (GO) under exceptionally mild conditions. Theoretical calculations indicate that the presence of S vacancies on the surface of ZCS/GO photocatalyst is crucial for the adsorption and activation of O2, successively generating the superoxide radical (•O2−) and 1O2, attributing to the regulation of local electron density on the surface of ZCS/GO and photogenerated holes (h+). Meanwhile, accelerated transfer of photogenerated electrons (e−) to GO caused by the π–π stacking effect is conducive to the subsequent aldehyde hydrogenation to benzyl alcohol rather than non-selective oxidation of aldehyde to carboxylic acid. Anisotropic charge transport driven by the built-in electric field can further promote the separation of e− and h+ for multistep reactions. Promisingly, one-pot photocatalytic conversion of p-xylene to 4-methylbenzyl alcohol is beneficial for reducing the harmful effects of aromatics on human health. Furthermore, this study provides novel insights into the design of photocatalysts for cascade reactions.
中文翻译：
VS-Zn0.5Cd0.5S/GO 上定向电荷转移驱动的光催化级联反应用于可控苄基氧化
光催化是合成转化的重要技术。然而，用于定向合成的光驱动协同氧化还原反应却很少受到关注。在此，作者报告了在光催化剂 Zn 0.5 Cd 0.5 S (ZCS ) 上通过单线态氧 ( 1 O 2 ) 和质子耦合电子转移 (PCET)在 5 小时内可将苄基可调氧化为苯基甲醇，产率适中 (47%) /氧化石墨烯（GO）在极其温和的条件下。理论计算表明，ZCS/GO光催化剂表面S空位的存在对于O 2的吸附和活化至关重要，从而先后产生超氧自由基（· O 2 -）和1 O 2，这归因于局部调节ZCS/GO 表面的电子密度和光生空穴 (h + )。同时， π - π堆积效应引起的光生电子（e - ）向GO的加速转移有利于随后的醛加氢生成苯甲醇，而不是醛非选择性氧化为羧酸。由内置电场驱动的各向异性电荷传输可以进一步促进多步反应中e -和 h +的分离。对二甲苯一锅光催化转化为4-甲基苯甲醇有希望有利于减少芳烃对人体健康的有害影响。此外，这项研究为级联反应光催化剂的设计提供了新的见解。
更新日期：2023-05-01
中文翻译：
VS-Zn0.5Cd0.5S/GO 上定向电荷转移驱动的光催化级联反应用于可控苄基氧化
光催化是合成转化的重要技术。然而，用于定向合成的光驱动协同氧化还原反应却很少受到关注。在此，作者报告了在光催化剂 Zn 0.5 Cd 0.5 S (ZCS ) 上通过单线态氧 ( 1 O 2 ) 和质子耦合电子转移 (PCET)在 5 小时内可将苄基可调氧化为苯基甲醇，产率适中 (47%) /氧化石墨烯（GO）在极其温和的条件下。理论计算表明，ZCS/GO光催化剂表面S空位的存在对于O 2的吸附和活化至关重要，从而先后产生超氧自由基（· O 2 -）和1 O 2，这归因于局部调节ZCS/GO 表面的电子密度和光生空穴 (h + )。同时， π - π堆积效应引起的光生电子（e - ）向GO的加速转移有利于随后的醛加氢生成苯甲醇，而不是醛非选择性氧化为羧酸。由内置电场驱动的各向异性电荷传输可以进一步促进多步反应中e -和 h +的分离。对二甲苯一锅光催化转化为4-甲基苯甲醇有希望有利于减少芳烃对人体健康的有害影响。此外，这项研究为级联反应光催化剂的设计提供了新的见解。
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