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厚介孔γ-氧化铝膜的合成、Pt 纳米粒子的负载以及复合膜作为可重复使用催化剂的应用。

Synthesis of thick mesoporous gamma-alumina films, loading of Pt nanoparticles, and use of the composite film as a reusable catalyst.

机构信息

Sol-Gel Division, Central Glass and Ceramic Research Institute, Council of Scientific and Industrial Research, 196 Raja S. C. Mullick Road, Jadavpur, Kolkata 700032, India.

出版信息

ACS Appl Mater Interfaces. 2009 Apr;1(4):833-40. doi: 10.1021/am800241x.

Abstract

Nanocrystalline mesoporous gamma-Al2O3 film of high thickness has been developed and characterized. The films were prepared on ordinary glass substrates by a single dip-coating method using boehmite (AlOOH) sols derived from aluminum tri-sec-butoxide in presence of cetyltrimethylammonium bromide (CTAB) as structure-directing agent. The dried films were heat-treated at 500 degrees C in air to remove the organics and strengthen the network. The GIXRD of the heat-treated (500 degrees C) film shows a broad peak in the low-angle region supporting the formation of worm-hole-like disordered mesostructures. The high-angle GIXRD, FTIR, and TEM of the films confirm the formation of gamma-Al2O3. N2 adsorption-desorption analyses showed that the heat-treated (500 degrees C) film has a BET surface area of 171 m(2) g(-1) with a pore volume of 0.188 cm(3) g(-1) and mean pore diameter 4.3 nm. Pt nanoparticles (NPs) (approximately 2.7 mol % with respect to the equivalent AlO(1.5)) were generated inside the mesopores of the heat-treated films simply by soaking H2PtCl6 solutions into it, and followed by thermal decomposition at 500 degrees C. The surface area and pore volume of the Pt-incorporated film have been reduced to 101 m(2) g(-1) and 0.119 cm(3) g(-1) respectively, confirming the inclusion of Pt NPs inside the pores. FESEM and TEM studies revealed uniform distribution of Pt NPs (2-8.5 nm; average diameter 4.9 nm) in the films. Catalytic properties of the Pt-incorporated films were investigated in two model (one inorganic and other organic) systems: reduction of hexacyanoferrate(III) ions by thiosulfate to ferrocyanide, and p-nitrophenol to p-aminophenol. In both the cases, the catalyst showed excellent activities, and the reduction reactions followed smoothly, showing isosbestic points in the UV-visible spectra. The catalyst films can be separated easily after the reactions and reused several times.

摘要

已经开发和表征了具有高厚度的纳米晶介孔 γ-Al2O3 薄膜。通过使用正硅酸乙酯(TEOS)在十六烷基三甲基溴化铵(CTAB)存在下制备的水铝石(AlOOH)溶胶,通过单次浸涂法在普通玻璃基板上制备了薄膜。将干燥的薄膜在空气中于 500°C 下热处理以除去有机物并增强网络。热处理(500°C)后的薄膜的 GIXRD 在低角度区域显示出宽峰,支持蠕虫孔状无序介孔结构的形成。高角度 GIXRD、FTIR 和薄膜的 TEM 证实了 γ-Al2O3 的形成。N2 吸附-解吸分析表明,热处理(500°C)后的薄膜具有 171 m2g-1 的 BET 表面积,0.188 cm3g-1 的孔体积和 4.3nm 的平均孔径。通过简单地将 H2PtCl6 溶液浸泡在其中,然后在 500°C 下进行热分解,在热处理后的薄膜的介孔中生成了 Pt 纳米颗粒(NPs)(相对于 AlO1.5 约为 2.7mol%)。负载 Pt 的薄膜的表面积和孔体积分别减少到 101 m2g-1 和 0.119 cm3g-1,这证实了 Pt NPs 包含在孔内。FESEM 和 TEM 研究表明,Pt NPs(2-8.5nm;平均直径 4.9nm)在薄膜中均匀分布。在两个模型(一个无机和另一个有机)系统中研究了负载 Pt 的薄膜的催化性能:六氰合铁(III)离子通过硫代硫酸盐还原为亚铁氰化物,以及对硝基苯酚还原为对氨基酚。在这两种情况下,催化剂都表现出优异的活性,还原反应顺利进行,在紫外可见光谱中出现等色点。反应后可以很容易地分离催化剂薄膜并重复使用几次。

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