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Aerobic selective oxidation of alcohols using La1-xCexCoO3 perovskite catalysts

机译:使用La1-xCexCoO3钙钛矿催化剂对酒精进行好氧选择性氧化

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The synthesis of porous perovskites with high and stable activity for alcohols oxidation using molecular oxygen as oxidant is reported. La1-xCexCoO3 catalysts are prepared by a sol-gel method using methanol and ethylene glycol as complexing agents. Calcination at 600 degrees C allows the formation of macro- and mesopores, in contrast to similar materials that often show a bulk structure. Catalytic tests show that La0.9Ce0.1CoO3 is highly active for benzyl alcohol oxidation with molecular oxygen, with both conversion and selectivity above 95% (60 min, 88 degrees C, 1 atm). Further tests show that 94% of the original activity can be obtained after surface regeneration of the used catalyst. The good catalytic performance is explained by the presence of cerium, which is able to attract and release adsorbed oxygen on the oxygen vacancies. The electrons donated by alcohols improve the ability of oxygen vacancies to activate molecular oxygen into oxygen anions, which react with the alcohol and increase the reaction rate. A mechanism is proposed. (C) 2016 Elsevier Inc. All rights reserved.
机译:报道了使用分子氧作为氧化剂合成具有高且稳定的醇氧化活性的钙钛矿。 La1-xCexCoO3催化剂是使用甲醇和乙二醇作为络合剂,通过溶胶-凝胶法制备的。与通常显示整体结构的类似材料相比,在600摄氏度下煅烧可形成大孔和中孔。催化测试表明,La0.9Ce0.1CoO3对分子氧氧化苄醇具有很高的活性,转化率和选择性均超过95%(60分钟,88摄氏度,1个大气压)。进一步的测试表明,用过的催化剂进行表面再生后,可以获得94%的原始活性。铈的存在说明了良好的催化性能,铈能够在氧空位上吸引和释放吸附的氧。由醇提供的电子提高了氧空位将分子氧活化为氧阴离子的能力,氧阴离子与醇反应并提高了反应速率。提出了一种机制。 (C)2016 Elsevier Inc.保留所有权利。

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