一种环境友好的方法合成金纳米颗粒负载介孔二氧化硅的催化应用

Andrés Guzmán‐Cruz, F. Paraguay-Delgado, M. Pal
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摘要

介孔二氧化硅作为一种具有良好分散性和优异稳定性的金属纳米颗粒载体材料,在各种催化反应中受到广泛关注。然而,缺乏控制合成具有高表面积和理想孔径的介孔二氧化硅来支持金属NPs的合成方案,大大降低了催化剂的催化性能和稳定性。本文报道了一种制备介孔二氧化硅负载金纳米粒子(Au/SiO2)的简便合成方法,用于高效催化还原4-硝基苯酚。利用氯化胆碱/尿素衍生的深共熔溶剂(DES)作为溶剂热反应的有效溶剂和模板剂,探索了一种环保型合成介孔二氧化硅的途径。首先用-NH2基团对介孔二氧化硅进行官能团化,然后在介孔二氧化硅基体上沉积平均尺寸为10 nm的Au纳米粒子。由于负载的Au NPs与介孔二氧化硅载体的强相互作用,合成的复合材料对4-NP还原为4-氨基苯酚表现出优异的催化性能,其速率常数为Kapp= 3.04 x10-1 min-1,与裸介孔二氧化硅催化剂相比,稳定性非常高。目前制造介孔二氧化硅和Au/SiO2催化剂的绿色方法具有很大的前景,因为它是一种更便宜和环保的方法,可以大规模制造用于不同催化反应的其他负载催化剂。
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An Environmentally Friendly Approach for the Synthesis of Au Nanoparticles Supported Mesoporous Silica for Catalytic Applications
Mesoporous silica has received much attention as an attractive support material for metal nanoparticles (NPs) with good dispersion and exceptional stability for various catalytic reactions. However, the lack of synthetic protocols to controlled synthesis of mesoporous silica with high surface area and ideal pore size for supporting metal NPs significantly reduces the catalytic performance and stability of the catalysts. This work reports a facile synthetic route to prepare mesoporous silica-supported Au NPs (Au/SiO2) for efficient catalytic reduction of 4-nitrophenol. An environmentally friendly synthetic route was exploited to prepare mesoporous silica using deep eutectic solvent (DES) derived from choline chloride/urea as an efficient solvent and template in solvothermal reaction. The mesoporous silica was first functionalized with –NH2 groups, and subsequently, Au NPs with an average size of 10 nm were deposited onto the mesoporous silica matrix. Owing to the strong interaction of supported Au NPs with the mesoporous silica support, the resultant composite exhibited excellent catalytic performance towards the reduction of 4-NP to 4-aminophenol with a rate constant of Kapp= 3.04 x10-1 min-1 and exceptionally high stability compared to bare mesoporous silica catalyst. The current green approach to fabricating mesoporous silica and Au/SiO2 catalysts holds great promise since it is a much cheaper and environmentally friendly method for large-scale fabrication of other supported catalysts for different catalytic reactions.
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