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TiO2 纳米粒子掺杂 SiO2 介孔薄膜:一种催化纳米反应器。

TiO2 nanoparticles doped SiO2 films with ordered mesopore channels: a catalytic nanoreactor.

机构信息

Nano-Structured Materials Division, CSIR-Central Glass and Ceramic Research Institute, 196, Raja S. C. Mullick Road, Kolkata 700032, India.

出版信息

Dalton Trans. 2014 Apr 7;43(13):5221-9. doi: 10.1039/c3dt53265h.

Abstract

Titanium dioxide (TiO2) incorporated ordered 2D hexagonal mesoporous silica (SiO2) films on a glass substrate were fabricated for use as a catalytic nanoreactor. Films were prepared using a tetraethyl orthosilicate (TEOS) derived SiO2 sol and a commercially available dispersion of TiO2 nanoparticles (NPs) in the presence of pluronic P123 as the structure directing agent. The effect of TiO2 doping (4-10 mol% with respect to the equivalent SiO2) into the ordered mesoporous SiO2 matrix was thoroughly investigated. The undoped SiO2 film showed a mesostructural transformation after heat-treatment at 350 °C whereas incorporation of TiO2 restricted such a transformation. Among all the TiO2 incorporated films, TEM showed that the 7 equivalent mol% TiO2 doped SiO2 film (ST-7) had an optimal composition which could retain the more organized 2D hexagonal (space group p6mm)-like mesostructures after heat-treatment. The catalytic activities of the TiO2 doped (4-10 mol%) films were investigated for the reduction of toxic KMnO4 in an aqueous medium. ST-7 film showed the maximum catalytic activity, as well as reusability. A TEM study on the resultant solution after KMnO4 reduction revealed the formation of MnO2 nanowires. It was understood that the embedded TiO2 NPs bonded SiO2 matrix increased the surface hydroxyl groups of the composite films resulting in the generation of acidic sites. The catalytic process can be explained by this enhanced surface acidity. The mesoporous channel of the ST-7 films with TiO2 doping can be used as a nanoreactor to form extremely thin MnO2 nanowires.

摘要

在玻璃基底上制备了负载二氧化钛(TiO2)的有序二维六方介孔二氧化硅(SiO2)薄膜,用作催化纳米反应器。该薄膜采用正硅酸乙酯(TEOS)衍生的 SiO2 溶胶和市售的 TiO2 纳米颗粒(NPs)分散体,在 Pluronic P123 作为结构导向剂的条件下制备。深入研究了 TiO2 掺杂(相对于等当量 SiO2 为 4-10mol%)对有序介孔 SiO2 基质的影响。未经掺杂的 SiO2 薄膜在 350°C 热处理后表现出介孔结构转变,而掺入 TiO2 则限制了这种转变。在所有掺杂 TiO2 的薄膜中,TEM 显示 7 当量 mol% TiO2 掺杂的 SiO2 薄膜(ST-7)具有最佳组成,在热处理后可以保留更有序的二维六方(空间群 p6mm)类似介孔结构。研究了掺杂(4-10mol%)TiO2 的薄膜对有毒 KMnO4 在水介质中的还原的催化活性。ST-7 薄膜表现出最大的催化活性和可重复使用性。对 KMnO4 还原后所得溶液的 TEM 研究表明形成了 MnO2 纳米线。据理解,嵌入的 TiO2 NPs 键合的 SiO2 基质增加了复合薄膜的表面羟基基团,从而产生酸性位。可以通过这种增强的表面酸度来解释催化过程。具有 TiO2 掺杂的 ST-7 薄膜的介孔通道可用作纳米反应器,以形成极薄的 MnO2 纳米线。

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