Gold nanoparticles supported on mesoporous silica: origin of high activity and role of Au NPs in selective oxidation of cyclohexane.
Gold nanoparticles supported on mesoporous silica: origin of high activity and role of Au NPs in selective oxidation of cyclohexane.
复制标题
介孔二氧化硅负载的金纳米粒子：高活性的起源以及金纳米粒子在环己烷选择性氧化中的作用
DOI：
10.1038/srep18817
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发表时间：
2016-01-05
影响因子：
4.6
通讯作者：
Zhao GX
中科院分区：
文献类型：
--
作者：
Wu P;Bai P;Yan Z;Zhao GX
以有机硅烷为催化剂，采用一锅合成法实现了金纳米颗粒在介孔二氧化硅上的均相固定化。所制得的Au纳米粒子在分子氧无溶剂选择氧化环己烷反应中表现出良好的催化活性。通过建立结构-性能关系，确定了中孔负载型Au催化剂活性高的原因是低配位、高分散的Au(0)位的存在。Au纳米粒子通过促进O2分子的活化和促进表面活性氧物种的形成，在环己烷的催化氧化中起着关键作用。
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 O2molecules and accelerating the formation of surface-active oxygen species.