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首页> 外文期刊>The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical >Electron spin resonance studies on the oxidation mechanism of sterically hindered cyclic amines in TiO2 photocatalytic systems
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Electron spin resonance studies on the oxidation mechanism of sterically hindered cyclic amines in TiO2 photocatalytic systems

机译：电子自旋共振研究TiO2光催化体系中位阻环胺的氧化机理

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摘要

A sterically hindered cyclic amine, 4-hydroxy-2,2,6,6-tetramethylpiperidine (HTMP), is converted to the corresponding aminoxyl radical (nitroxide radical), 4-hydroxy-2,2,6,6-tetramethyl piperidine 1-oxyl (TEMPOL radical) as a result of a photocatalytic reaction in TiO2 aqueous suspension. The time profile of the radical formation and the effect of additives, such as SCN-, I-, methanol, and H2O2, on the initial formation rate were measured in order to elucidate the reaction mechanism. The experimental observations indicated that the direct photocatalytic oxidation of HTMP followed by reaction with O-2 is the dominant process in the formation of TEMPOL radicals. Electrochemical measurements showed that HTMP is oxidized at 0.7 V (vs NHE), which is consistent with the proposed mechanism. The possibility of other processes, involving reactions with singlet molecular oxygen, superoxide radical, and hydroxyl radical, were excluded from the reaction mechanism.
机译：位阻环胺4-羟基-2,2,6,6-四甲基哌啶（HTMP）被转化为相应的氨基羟自由基（硝基氧自由基）4-羟基-2,2,6,6-四甲基哌啶1 -氧基（TEMPOL自由基）是TiO2水性悬浮液中光催化反应的结果。测量自由基形成的时间曲线以及添加剂（如SCN-，I-，甲醇和H2O2）对初始形成速率的影响，以阐明反应机理。实验观察表明，HTMP的直接光催化氧化以及与O-2的反应是TEMPOL自由基形成的主要过程。电化学测量表明，HTMP在0.7 V（vs NHE）下被氧化，这与所提出的机理是一致的。从反应机理中排除了涉及与单线态分子氧，超氧自由基和羟基自由基反应的其他过程的可能性。

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