Pt纳米颗粒形貌对水中乙二醇好氧氧化制乙醇酸的影响

IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Werner Oberhauser*, Claudio Evangelisti*, Xuan Trung Nguyen, Jonathan Filippi, Lorenzo Poggini, Laura Capozzoli, Gabriele Manca, Ella A. Kitching, Thomas J. A. Slater and Mohsen Danaie, 
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引用次数: 0

摘要

采用金属气相合成法制备直径为3nm的铂纳米颗粒,负载在高表面积碳上,在中性和碱性条件下催化乙二醇在水中的好氧氧化制乙醇酸(GA)。在氮气气氛下对催化剂进行控制热处理,形成了形态明确的催化剂。原子分辨电子显微镜、CO溶出伏安法和XPS对合成和热处理催化剂的分析表明,纳米颗粒的形貌对催化高活性的Pt-OH表面物质的稳定起着至关重要的作用,这些物质是pt催化醇氧化成羰基官能团的关键物质。通过实验(高压釜实验)证明了碱对催化剂活性和GA选择性的促进作用。通过DFT计算证明了碱对非金属催化反应步骤(即羰基有氧氧化成酸官能团)的影响。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Effect of Pt Nanoparticle Morphology on the Aerobic Oxidation of Ethylene Glycol to Glycolic Acid in Water

Effect of Pt Nanoparticle Morphology on the Aerobic Oxidation of Ethylene Glycol to Glycolic Acid in Water

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.

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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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