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Effect of Pt Nanoparticle Morphology on the Aerobic Oxidation of Ethylene Glycol to Glycolic Acid in Water
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-11-18 , DOI: 10.1021/acs.inorgchem.4c03970
Werner Oberhauser, Claudio Evangelisti, Xuan Trung Nguyen, Jonathan Filippi, Lorenzo Poggini, Laura Capozzoli, Gabriele Manca, Ella A. Kitching, Thomas J. A. Slater, Mohsen Danaie

Pt nanoparticles (diameter <3 nm), generated by metal vapor synthesis and supported on a high surface area carbon, were used to catalyze the aerobic oxidation of ethylene glycol to glycolic acid (GA) in water under neutral and basic reaction conditions. Controlled heat treatment of the catalyst under a nitrogen atmosphere brought about the formation of a morphologically well-defined catalyst. A combination of atomic resolution electron microscopy, CO stripping voltammetry, and XPS analyses conducted on as-synthesized and heat-treated catalysts demonstrated the crucial role of the nanoparticles’ morphology on the stabilization of catalytically highly active Pt–OH surface species, which were key species for the Pt-catalyzed oxidation of the alcohol to the carbonyl functionality. The boosting effect of base on the catalyst’ s activity and GA selectivity has been proved experimentally (autoclave experiments). The effect of base on the nonmetal-catalyzed reaction steps (i.e., aerobic oxidation of carbonyl to acid functionality) has been proved by DFT calculations.

中文翻译:


Pt 纳米颗粒形态对水中乙二醇有氧氧化为乙醇酸的影响



由金属气相合成生成并负载在高表面积碳上的 Pt 纳米颗粒(直径 <3 nm)用于在中性和碱性反应条件下催化乙二醇在水中有氧氧化为乙醇酸 (GA)。在氮气气氛下对催化剂进行受控热处理,形成了形态明确的催化剂。对合成和热处理催化剂进行的原子分辨率电子显微镜、一氧化碳剥离伏安法和 XPS 分析的组合表明,纳米颗粒的形态对催化高活性 Pt-OH 表面物质的稳定起着关键作用,这些物质是 Pt 催化醇氧化成羰基官能团的关键物质。碱对催化剂活性和 GA 选择性的增强作用已通过实验证明(高压釜实验)。碱对非金属催化反应步骤(即羰基有氧氧化为酸官能团)的影响已通过 DFT 计算得到证明。
更新日期:2024-11-18
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