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首页> 外文期刊>Chemistry: A European journal >Hydrotalcite-supported gold catalyst for the oxidant-free dehydrogenation of benzyl alcohol: Studies on support and gold size effects
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Hydrotalcite-supported gold catalyst for the oxidant-free dehydrogenation of benzyl alcohol: Studies on support and gold size effects

机译：水滑石负载的金催化剂用于苯甲醇的无氧化剂脱氢：载体和金的尺寸效应研究

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摘要

Gold nanoparticles with uniform mean sizes (a≈3 nm) loaded onto various supports have been prepared and studied for the oxidant-free dehydrogenation of benzyl alcohol to benzaldehyde and hydrogen. The use of hydrotalcite (HT), which possesses both strong acidity and strong basicity, provides the best catalytic performance. Au/HT catalysts with various mean Au particle sizes (2.1-21 nm) have been successfully prepared by a deposition-precipitation method under controlled conditions. Detailed catalytic reaction studies with these catalysts demonstrate that the Au-catalyzed dehydrogenation of benzyl alcohol is a structure-sensitive reaction. The turnover frequency (TOF) increases with decreasing Au mean particle size (from 12 to 2.1 nm). A steep rise in TOF occurs when the mean Au particle size becomes smaller than 4 nm. Our present work suggests that the acid-base properties of the support and the size of Au nanoparticles are two key factors controlling the alcohol dehydrogenation catalysis. A reaction mechanism is proposed to rationalize these results. It is assumed that the activation of the β-C?￡?H bond of alcohol, which requires the coordinatively unsaturated Au atoms, is the rate-determining step.
机译：制备并负载在各种载体上的均一大小均一（a≈3nm）的金纳米颗粒，并对其进行了无氧化剂的苯甲醇脱氢制苯甲醛和氢的研究。具有强酸性和强碱性的水滑石（HT）的使用提供了最佳的催化性能。已经通过在受控条件下的沉积沉淀法成功制备了具有各种平均Au粒径（2.1-21 nm）的Au / HT催化剂。使用这些催化剂进行的详细催化反应研究表明，Au催化的苄醇脱氢反应对结构敏感。周转频率（TOF）随着Au平均粒径的减小（从12到2.1 nm）而增加。当平均Au粒径小于4 nm时，TOF急剧上升。我们目前的工作表明，载体的酸碱性质和Au纳米粒子的尺寸是控制醇脱氢催化的两个关键因素。提出了一种反应机制来合理化这些结果。假定需要配位不饱和Au原子的醇的β-C1 -C H键的活化是决定速率的步骤。

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