可调谐的 Pt 纳米催化剂用于肉桂醇的有氧氧化。

Tunable Pt nanocatalysts for the aerobic selox of cinnamyl alcohol.

机构信息

Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.

出版信息

Nanoscale. 2013 Jun 21;5(12):5412-9. doi: 10.1039/c3nr00184a.

Abstract

The selective aerobic oxidation of cinnamyl alcohol over Pt nanoparticles has been tuned via the use of mesoporous silica supports to control their dispersion and oxidation state. High area two-dimensional SBA-15, and three-dimensional, interconnected KIT-6 silica significantly enhance Pt dispersion, and thus surface PtO2 concentration, over that achievable via commercial low surface area silica. Selective oxidation activity scales with Pt dispersion in the order KIT-6 ≥ SBA-15 > SiO2, evidencing surface PtO2 as the active site for cinnamyl alcohol selox to cinnamaldehyde. Kinetic mapping has quantified key reaction pathways, and the importance of high O2 partial pressures for cinnamaldehyde production.

摘要

通过使用介孔硅载体来控制铂纳米粒子的分散和氧化态，从而对肉桂醇的选择性有氧氧化进行了调谐。高面积二维 SBA-15 和三维相互连接的 KIT-6 硅显著提高了铂的分散度，从而提高了表面 PtO2 的浓度，超过了商业低表面积硅所能达到的水平。选择性氧化活性按 Pt 分散度的顺序排列，即 KIT-6≥SBA-15＞SiO2，这表明表面 PtO2 是肉桂醇 selox 向肉桂醛选择性氧化的活性位。动力学映射已经量化了关键反应途径，以及高 O2 分压对肉桂醛生成的重要性。