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纳米金嵌入介孔硅中作为一种高活性和强稳定性的催化剂。

Nanoscale gold intercalated into mesoporous silica as a highly active and robust catalyst.

机构信息

Department of Chemistry and Geochemistry, Colorado School of Mines, Golden, CO 80401, USA.

出版信息

Nanotechnology. 2012 Jul 27;23(29):294010. doi: 10.1088/0957-4484/23/29/294010. Epub 2012 Jun 28.

Abstract

Stable gold/mesoporous silica nanocomposites (with Au nanoparticles intercalated in the walls of mesoporous silica) were successfully synthesized by the hydrothermal method and applied as catalysts. A challenging issue associated with intercalation and the use of coordinating agents is the effect of the coordinating agent on the mesoporous silica structure and periodicity. This investigation is targeted at elaborating the effect of the coordinating agent on the resulting mesoporous structure. The amount of Au coordinating agent bis[3-(triethoxysilyl)propyl]-tetrasulfide (TESPTS) was systematically altered to synthesize a range of materials with varying Au loadings and morphologies. These materials were characterized by N(2) adsorption-desorption, x-ray diffraction, transmission electron microscopy and UV-visible spectroscopy. The structures of the catalysts were found to range from mesoporous to vesical- and foam-like upon varying the TESPTS/polymer template (P123) ratio. Additionally, the sizes of Au nanoparticles increased by increasing the amount of TESPTS. The catalytic properties of the resulting materials were examined using oxidation of benzyl alcohol and reduction of 4-nitrophenol as probe reactions. The intercalated systems demonstrated high activity and more importantly were robust and readily reusable. This approach to imparting stability to nanoscale materials may be much more broadly applicable and expand the types of environments in which they can be utilized.

摘要

稳定的金/介孔硅纳米复合材料(金纳米粒子嵌入介孔硅的壁中)通过水热法成功合成,并用作催化剂。与嵌入和使用配位剂相关的一个挑战性问题是配位剂对介孔硅结构和周期性的影响。这项研究旨在详细说明配位剂对所得介孔结构的影响。系统地改变 Au 配位剂双[3-(三乙氧基硅基)丙基]四硫化物(TESPTS)的量,以合成具有不同 Au 负载量和形貌的一系列材料。这些材料通过 N(2)吸附-解吸、X 射线衍射、透射电子显微镜和紫外-可见光谱进行了表征。发现催化剂的结构从介孔到囊泡状和泡沫状,随着 TESPTS/聚合物模板(P123)比的变化而变化。此外,通过增加 TESPTS 的量,Au 纳米粒子的尺寸增大。使用苯甲醇氧化和 4-硝基苯酚还原作为探针反应来考察所得材料的催化性能。嵌入体系表现出高活性,更重要的是它们稳定且易于重复使用。这种赋予纳米材料稳定性的方法可能具有更广泛的适用性,并扩展它们可以使用的环境类型。

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