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首页> 外文期刊>ACS catalysis >Understanding of the Oxidation Behavior of Benzyl Alcohol by Peroxymonosulfate via Carbon Nanotubes Activation
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Understanding of the Oxidation Behavior of Benzyl Alcohol by Peroxymonosulfate via Carbon Nanotubes Activation

机译：通过碳纳米管激活对苄醇的氧化行为理解

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摘要

Selective oxidation of benzyl alcohol (BzOH) into benzaldehyde (BzH) is very important in synthetic chemistry. Peroxymonosulfate (PMS) is a cheap, stable, and soluble solid oxidant, holding promise for organic oxidation reactions. Herein, we report the catalytic PMS activation via carbon nanotubes (CNTs) for the selective oxidation of BzOH under mild conditions without other additives. A remarkable promotion of BzH yield with a selectivity over 80% was achieved on modified CNTs, i.e., O-CNTs via the radical oxidation process, and the oxygen functionalities for catalysis were comprehensively investigated by experimental study and theoretical exploration. To understand the different surface oxygen species on CNTs for the activation of PMS, density functional theory (DFT) calculations were performed to investigate the adsorption behavior of PMS on various CNTs. The electrophilic oxygen was identified as the electron captor to activate PMS by O-O bond cleavage to form SO5 center dot- and SO4 center dot- radicals. The nucleophilic carbonyl groups can also induce a redox cycle to generate (OH)-O-center dot and SO4 center dot- radicals, but phenolic hydroxyl groups impede the radical process with antioxidative functionality. The carbocatalysis-assisted PMS activation may provide a cheap process for the selective oxidation of alcohols into aldehydes or ketones. The insight achieved from this fundamental study may be further applied to other organic syntheses via selective oxidation.
机译：对苯甲醛（BZH）的选择性氧化成苯甲醛（BZH）在合成化学中非常重要。过氧氧键硫酸盐（PMS）是一种廉价，稳定的和可溶性的固体氧化剂，保持有机氧化反应的希望。在此，我们通过碳纳米管（CNT）报告催化PMS活化，用于在不含其他添加剂的温和条件下选择性氧化BZOH。通过自由基氧化过程，在改性的CNT中实现了具有超过80％的选择性的BZH产量的显着促进，并通过实验研究和理论探索全面研究了催化的催化氧函数。为了了解CNT上的不同表面氧物质，用于激活PMS，进行密度泛函理论（DFT）计算以研究各种CNT上PMS的吸附行为。将亲电氧鉴定为电子备峰，以通过O-O键切割激活PM，以形成SO5中心点和SO4中心点。亲核羰基也可以诱导氧化还原循环以产生（OH）-O-中心点和SO4中心点，但酚羟基妨碍抗氧化功能的自由基方法。携碳催化辅助PMS活化可提供廉价的方法，用于选择性氧化醇纳醛或酮。通过选择性氧化可以进一步应用于该基本研究所达到的洞察力。

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