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Gold nanoparticles supported on metal oxides as catalysts for the direct oxidative esterification of alcohols under mild conditions

机译:负载在金属氧化物上的金纳米颗粒作为在温和条件下进行醇类直接氧化酯化的催化剂

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Gold nanoparticles supported on metal oxides were used to catalyze the direct oxidative esterification of alcohols; esters were obtained using molecular oxygen as an oxidant under ambient temperature and pressure. Higher activities for the reaction between the benzyl alcohol and methanol were obtained over Au/CeO2 and Au/ZrO2 than Au/TiO2 (anatase), Au/HT (hydrotalcite) and Au/Al2O3. These catalysts were characterized using transmission electron microscopy (TEM), X-ray diffraction (XRD), atomic absorption spectroscopy (AAS) and X-ray photoelectron spectroscopy (XPS). The distribution of gold nanoparticles was uniform; no change of chemical states occurred for supports and gold nanoparticles after the catalysts were reused 10 times. The oxidative esterification of various alcohols over these catalysts could also occur under optimized reaction conditions. The substituted benzyl alcohols and cinnamyl alcohols were more active than heterocyclic alcohols and aliphatic alcohols because their a-H could be eliminated more easily during the induction of adsorbed dioxygen. Self-oxidative esterification was available for benzyl alcohol in inert solvents with low polarity indexes. A reaction mechanism was proposed for the synthesis of esters from alcohols with molecular oxygen. (C) 2014 Elsevier B.V. All rights reserved.
机译:负载在金属氧化物上的金纳米颗粒用于催化醇类的直接氧化酯化反应。在环境温度和压力下,使用分子氧作为氧化剂可得到酯。在Au / CeO2和Au / ZrO2上,苯甲醇与甲醇之间的反应活性高于Au / TiO2(锐钛矿),Au / HT(水滑石)和Au / Al2O3。使用透射电子显微镜(TEM),X射线衍射(XRD),原子吸收光谱(AAS)和X射线光电子光谱(XPS)对这些催化剂进行了表征。金纳米颗粒的分布是均匀的。催化剂重复使用10次后,载体和金纳米颗粒的化学状态均未发生变化。在优化的反应条件下,各种醇在这些催化剂上的氧化酯化反应也可能发生。取代的苄醇和肉桂醇比杂环醇和脂族醇更具活性,因为在诱导吸附的双氧过程中,它们的a-H可以更容易地被消除。苯甲醇在低极性指数的惰性溶剂中可进行自氧化酯化。提出了由醇与分子氧合成酯的反应机理。 (C)2014 Elsevier B.V.保留所有权利。

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