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Kinetic study on photocatalytic hydrogenation of acetophenone derivatives on titanium dioxide

机译：动力学研究乙烯酮衍生物在二氧化钛上的光催化氢化

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摘要

Acetophenone (AP) derivatives were photocatalytically hydrogenated to afford the corresponding secondary alcohols with excellent chemical efficiencies on titanium dioxide (Degussa P25, TiO2) under UV light irradiation. Maximum reaction rates (k_(max)) and apparent adsorption constants [K_(LH)) under irradiation were obtained from the Langmuir-Hinshelwood kinetic analysis. The k_(max) values showed a tendency to decrease with the decreasing reduction potentials (E_(red)) of the AP derivatives, while the K_(LH) values were distributed in the range of 280-780 L mol~(-1). Among these, simple AP exhibited the greatest adsorptivity upon the UV irradiated TiO2 surface. Additionally, it was demonstrated that the electrons trapped at surface defect Ti (Tist) sites on the TiO2 actually hydrogenated the AP derivatives. The amount of reacted electrons also showed a tendency to decrease with decreasing E_(red) values, in accord with the dependence on k_(max). These results indicate that the electrons accumulated at shallow Ti_(st) states easily participate in the hydrogenation of AP derivatives, whereas those trapped at deeper states hardly react with the substrates. The results strongly support the electron transfer reaction model via the Ti_(st) sites in the photocatalytic hydrogenation on TiO2.
机译：将苯乙酮（AP）衍生物衍生成光催化，以在紫外线照射下对二氧化钛（Degussa p25，TiO2）具有出色化学效率的相应二次醇。从Langmuir-Hinshelwood动力学分析中获得了辐照下的最大反应速率（K_（Max））和明显的吸附常数[K_（LH））。 K_（Max）值显示出随着AP衍生物的降低电位（E_（RED））的降低趋势，而K_（LH）值分布在280-780 L mol〜（-1）的范围内。 。其中，简单的AP在UV辐照的TiO2表面上表现出最大的吸附性。此外，证明了TiO2上的表面缺陷Ti（TIST）位点的电子实际上氢化了AP衍生物。根据对K_（Max）的依赖性，反应电子的量还显示出随着E_（红色）值降低而减小的趋势。这些结果表明，在浅层ti_（st）状态下积累的电子容易参与AP衍生物的氢化，而被困在更深层状态的电子几乎不会与底物反应。结果通过TiO2上光催化氢化中的TI_（ST）位点强烈支持电子转移反应模型。

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