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Influences of synthesis conditions and mesoporous structures on the gold nanoparticles supported on mesoporous silica hosts

机译:合成条件和介孔结构对介孔二氧化硅基质负载金纳米颗粒的影响

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Loading gold on mesoporous materials via different methods has been actively attempted in the literature, but the knowledge about the influences of synthesis details and different mesoporous structures on the size and thermal stability of gold nanoparticles supported on mesoporous hosts is still limited. In this study, Au/HMS, Au/MCM-41, Au/MCM-48, Au/SBA-15, and Au/SBA-16 samples were prepared by modifying a variety of mesoporous silicas by amine ligands followed by loading HAuCl4 and calcination. The influences of different amine ligands ((3-aminopropyl)triethoxysilane versus N-[3-(trimethoxy-silyl)propyl]ethylenediamine), solvents (water versus ethanol), calcination temperatures (200 or 550 °C), and mesoporous structures on the size of supported gold nanoparticles were systematically investigated employing nitrogen adsorption-desorption measurement, X-ray diffraction (XRD), diffuse reflectance UV-vis spectroscopy, and transmission electron microscopy (TEM). Interestingly, while big and irregular gold particles situate on MCM-48 with bicontinuous three-dimensional pore structure and relatively small pore size (2.4 nm) upon calcination at 550 °C, homogeneous and small gold nanoparticles maintain inside SBA-15 with one-dimensional pore structure and relatively big pore size (6.8 nm). Apparently, the pore structure and pore size of mesoporous silica hosts play a key role in determining the size and thermal stability of the supported gold nanoparticles. Our results may provide some useful clues for the rational design of supported metal catalysts by choosing suitable mesoporous hosts.
机译:在文献中已经尝试了通过不同的方法将金加载到介孔材料上,但是关于合成细节和不同的介孔结构对介孔主体上负载的金纳米颗粒的尺寸和热稳定性的影响的知识仍然有限。在这项研究中,通过用胺配体修饰各种介孔二氧化硅,然后上样HAuCl4和煅烧。不同胺配体((3-氨基丙基)三乙氧基硅烷与N- [3-(三甲氧基-甲硅烷基)丙基]乙二胺),溶剂(水与乙醇),煅烧温度(200或550°C)和介孔结构的影响利用氮吸附-解吸测量,X射线衍射(XRD),漫反射紫外可见光谱和透射电子显微镜(TEM)对负载的金纳米颗粒的大小进行了系统研究。有趣的是,在550°C下煅烧时,大且不规则的金颗粒位于MCM-48上,具有双连续的三维孔结构和相对较小的孔径(2.4 nm),而均匀且小的金纳米颗粒则保持在SBA-15内部孔结构和相对较大的孔径(6.8纳米)。显然,介孔二氧化硅基质的孔结构和孔径在确定负载型金纳米颗粒的尺寸和热稳定性方面起着关键作用。通过选择合适的介孔主体,我们的结果可能为合理设计负载型金属催化剂提供一些有用的线索。

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