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Utilizing benign oxidants for selective aerobic oxidations using heterogenized platinum nanoparticle catalysts

机译:利用多元化铂纳米颗粒催化剂,利用良性氧化剂进行选择性好氧氧化

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摘要

By using platinum nanoparticle catalysts that are generated in situ by extrusion from a porous copper chlorophosphate framework, the role of oxidants in the selective oxidation of benzyl alcohol to benzaldehyde was evaluated, with a view to establishing structure-property relationships. With a detailed study of the kinetic properties of the oxidation reaction, it has been determined that the aerobic oxidation pathways progress with lower levels of product selectivity and higher activation energies (72.4 kJmol(-1)) than the peroxide-based ones (23.6 kJmol(-1)); affording valuable insights in the design of solid catalysts for selective oxidation reactions. Furthermore, through the use of X-ray absorption spectroscopy, the effect of calcination temperature on the degree of extrusion and its influence on nanoparticle formation have been evaluated, leading to the establishment of structure-activity correlations between the observed activation energies and the proportion of nanoparticle species generated.
机译:通过使用从多孔氯磷酸铜骨架中挤出原位生成的铂纳米颗粒催化剂,评估了氧化剂在苯甲醇选择性氧化为苯甲醛中的作用,以建立结构-性质关系。通过对氧化反应动力学特性的详细研究,可以确定,与基于过氧化物的氧化反应途径(23.6 kJmol)相比,有氧氧化途径的产物选择性更低,活化能更高(72.4 kJmol(-1))。 (-1));提供了用于选择性氧化反应的固体催化剂设计的宝贵见解。此外,通过使用X射线吸收光谱法,评估了煅烧温度对挤出程度的影响及其对纳米颗粒形成的影响,从而导致在观察到的活化能与氢的比例之间建立了结构活性相关性。生成纳米颗粒。

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