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Oxidative esterification of ethylene glycol in methanol to form methyl glycolate over supported Au catalysts

机译:甲醇中乙二醇的氧化酯化以在受支持的AU催化剂上形成甲基乙醇酸酯

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摘要

Au/ZnO and Au/Al2O3 catalysts with various mean Au particle diameters (2.0-7.4 nm) were prepared by the deposition of pre-formed Au colloids. These catalysts were evaluated in the oxidative esterification of ethylene glycol to methyl glycolate. The results show that the catalytic activity per surface Au atom is independent of Au particle diameter in the range of 3-7,4 nm, whereas smaller Au particles (~2.0 nm) show an inferior activity. This behavior was observed on both Au/ZnO and Au/Al2O3 catalysts. This observed correlation between activity and Au particle diameter confirms the assertion that only exposed atoms are catalytically active. We prepared gold nanoparticles with a uniform mean diameter of ~3 nm loaded on various supports, i.e. ZnO, Al2O3, SiO2, TiO2 and CeO2. Among these five catalysts, Au/ZnO gave the best catalytic activity in the reaction followed by Au/Al2O3. Au/SiO2, Au/TiO2 and Au/CeO2 gave significantly lower activities. The variation in catalytic behavior of these gold catalysts on different supports originates from differences in the anchoring of the supported Au particles, the gold oxidation state, the gold-support interaction, and the acidity of the support.
机译:Au/ZnO和Au/Al2O3催化剂具有各种平均AU颗粒直径(2.0-7.4 nm),通过沉积预先形成的AU胶体的沉积来制备。在乙二醇对甲基乙二醇的氧化酯化中评估了这些催化剂。结果表明,每个表面AU原子的催化活性与3-7,4 nm范围内的AU颗粒直径无关,而较小的Au颗粒(~2.0 nm)显示出较低的活性。在AU/ZnO和AU/AL2O3催化剂上都观察到了这种行为。观察到的活动与AU颗粒直径之间的相关性证实了仅暴露原子具有催化活性的断言。我们制备了在各种支撑上载荷的平均直径均匀直径的金纳米颗粒,即ZnO,Al2O3,SIO2,TIO2和CEO2。在这五个催化剂中,Au/ZnO在反应中提供了最佳的催化活性,然后是AU/AL2O3。 AU/SIO2,AU/TIO2和AU/CEO2的活动明显较低。这些金催化剂在不同支撑物上的催化行为的变化源于受支持的Au颗粒的锚定差异,金氧化状态,金支持的相互作用以及支撑的酸度。

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