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在无碱条件下使用负载金钯纳米粒子选择性氧化正丁醇。

Selective oxidation of n-butanol using gold-palladium supported nanoparticles under base-free conditions.

机构信息

Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF10 3AT (UK).

出版信息

ChemSusChem. 2015 Feb;8(3):473-80. doi: 10.1002/cssc.201403190. Epub 2014 Dec 17.

Abstract

The base-free selective catalytic oxidation of n-butanol by O2 in an aqueous phase has been studied using Au-Pd bimetallic nanoparticles supported on titania. Au-Pd/TiO2 catalysts were prepared by different methods: wet impregnation, physical mixing, deposition-precipitation and sol immobilisation. The sol immobilisation technique, which used polyvinyl alcohol (PVA) as the stabilizing agent, gave the catalyst with the smallest average particle size and the highest stable activity and selectivity towards butyric acid. Increasing the amount of PVA resulted in a decrease in the size of the nanoparticles. However, it also reduced activity by limiting the accessibility of reactants to the active sites. Heating the catalyst to reflux with water at 90 °C for 1 h was the best method to enhance the surface exposure of the nanoparticles without affecting their size, as determined by TEM, X-ray photoelectron spectroscopy and CO chemisorption analysis. This catalyst was not only active and selective towards butyric acid but was also stable under the operating conditions.

摘要

使用负载在二氧化钛上的金钯双金属纳米粒子研究了在水相中原位氧气无碱选择性催化氧化正丁醇。通过不同的方法制备了 Au-Pd/TiO2 催化剂:浸渍沉淀法、物理混合法、沉积沉淀法和溶胶固定化法。使用聚乙烯醇(PVA)作为稳定剂的溶胶固定化技术得到的催化剂具有最小的平均粒径和最高的稳定活性和丁酸选择性。增加 PVA 的量会导致纳米粒子的尺寸减小。然而,这也会通过限制反应物到达活性位点的可及性来降低活性。将催化剂在 90°C 的水中回流加热 1 小时是提高纳米粒子表面暴露度的最佳方法,而不会影响 TEM、X 射线光电子能谱和 CO 化学吸附分析所确定的其粒径。该催化剂不仅对丁酸具有活性和选择性,而且在操作条件下也很稳定。

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