当前位置: X-MOL 学术ACS Sustain. Chem. Eng. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
AgNPs Immobilized over Functionalized 2D Hexagonal SBA-15 for Catalytic C–H Oxidation of Hydrocarbons with Molecular Oxygen under Solvent-Free Conditions
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2020-03-31 , DOI: 10.1021/acssuschemeng.9b07409
Rima Biswas 1 , Sabuj Kanti Das 2 , Samanka Narayan Bhaduri 1 , Asim Bhaumik 2 , Papu Biswas 1
Affiliation  

Activation of C–H bonds of hydrocarbons is one of the thrust areas of research over the years. Designing a robust catalyst, which can work efficiently under eco-friendly conditions for this reaction still remains a big challenge today. Highly dispersed aggregation-free silver nanoparticles (AgNPs) are immobilized over 2D hexagonally ordered functionalized mesoporous silica material via surface thioether functionalization, and the resulting supported AgNPs (AgMS) displayed environmentally benign selective oxidation of C–H bonds of the aliphatic and monocyclic hydrocarbons into their respective carbonyl compounds. AgNPs-supported mesoporous materials are characterized by powder X-ray diffraction, nitrogen adsorption–desorption, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. The AgMS material retains mesoporosity with a narrow pore size distribution (D ∼ 5.7 nm) together with a high BET surface area of 844 m2g–1 after loading of AgNPs. The AgMS catalyst exhibited excellent activity toward liquid phase oxidation of C–H bonds under solvent-free and base-free neat conditions using molecular oxygen as the oxidant. This methodology was successfully applied for the oxidation of substituted toluene, benzylic C–H bonds, and cycloalkanes with very good conversion and selectivity. Moreover, the hydrocarbon conversion and selectivity for the carbonyl products in this partial oxidation reaction have been retained after six reaction cycles. Therefore, immobilization of AgNPs at the surface of ordered mesoporous silica offers a very efficient route in designing a readily separable, reusable, very robust, and promising catalyst for C–H bond activation under eco-friendly reaction conditions.

中文翻译:

在无溶剂条件下,固定在功能化的二维六角形SBA-15上的AgNP用于分子氧催化烃的CH–H氧化

碳氢键的氢键活化是多年来研究的重点领域之一。设计一种坚固的催化剂,该催化剂在生态友好的条件下可以有效地进行该反应仍然是当今的一大挑战。高度分散的无聚集银纳米颗粒(AgNPs)通过表面硫醚官能化固定在二维六方有序功能化介孔二氧化硅材料上,所得负载的AgNPs(AgMS)对脂族和单环烃的C–H键表现出对环境无害的选择性氧化成它们各自的羰基化合物。AgNPs介孔材料的特征是粉末X射线衍射,氮吸附-解吸,扫描电子显微镜,透射电子显微镜和X射线光电子能谱。d〜5.7纳米)的844高BET表面积一起米2-1加载AgNP后。AgMS催化剂在无溶剂和无碱纯净条件下,使用分子氧作为氧化剂,对C–H键的液相氧化表现出优异的活性。该方法已成功地用于氧化取代的甲苯,苄基CH键和环烷烃,并具有很好的转化率和选择性。而且,在该部分氧化反应中,在六个反应循环后,仍保留了烃的转化率和羰基产物的选择性。因此,将AgNPs固定在有序介孔二氧化硅表面上提供了一条非常有效的途径,可以设计出在生态友好的反应条件下,易于分离,可重复使用,非常耐用且有希望的C–H键活化催化剂。
更新日期:2020-04-23
down
wechat
bug