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负载在介孔二氧化硅上的金纳米颗粒:环己烷选择性氧化中高活性的起源及金纳米颗粒的作用

Gold nanoparticles supported on mesoporous silica: origin of high activity and role of Au NPs in selective oxidation of cyclohexane.

作者信息

Wu Pingping, Bai Peng, Yan Zifeng, Zhao George X S

机构信息

State Key Laboratory of Heavy Oil Processing, PetroChina Key Laboratory of Catalysis, School of Chemical Engineering, China University of Petroleum, Qingdao, China, 266580.

School of Chemical Engineering, The University of Queensland, St Lucia, 4072.

出版信息

Sci Rep. 2016 Jan 5;6:18817. doi: 10.1038/srep18817.

Abstract

Homogeneous immobilization of gold nanoparticles (Au NPs) on mesoporous silica has been achieved by using a one-pot synthesis method in the presence of organosilane mercapto-propyl-trimethoxysilane (MPTMS). The resultant Au NPs exhibited an excellent catalytic activity in the solvent-free selective oxidation of cyclohexane using molecular oxygen. By establishing the structure-performance relationship, the origin of the high activity of mesoporous supported Au catalyst was identified to be due to the presence of low-coordinated Au (0) sites with high dispersion. Au NPs were confirmed to play a critical role in the catalytic oxidation of cyclohexane by promoting the activation of O2 molecules and accelerating the formation of surface-active oxygen species.

摘要

在有机硅烷巯基丙基三甲氧基硅烷(MPTMS)存在的情况下,通过一锅合成法实现了金纳米粒子(Au NPs)在介孔二氧化硅上的均匀固定。所得的Au NPs在使用分子氧进行的无溶剂环己烷选择性氧化中表现出优异的催化活性。通过建立结构-性能关系,确定介孔负载Au催化剂高活性的起源是由于存在高度分散的低配位Au(0)位点。证实Au NPs通过促进O2分子的活化和加速表面活性氧物种的形成,在环己烷的催化氧化中起关键作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3690/4700469/cdeae8ceb502/srep18817-f1.jpg

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