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合成高活性纳米晶硫酸化二氧化钛-二氧化硅的新途径:硫酸根物种与二氧化硅在提高光催化效率方面的协同效应。

New route to synthesize highly active nanocrystalline sulfated titania-silica: synergic effects between sulfate species and silica in enhancing the photocatalysis efficiency.

作者信息

Xie Chao, Yang Qiujing, Xu Zili, Liu Xingjuan, Du Yaoguo

机构信息

College of Environment and Resources, Jilin University, Changchun 130023, China.

出版信息

J Phys Chem B. 2006 May 4;110(17):8587-92. doi: 10.1021/jp060266d.

DOI:10.1021/jp060266d
PMID:16640411
Abstract

A simple and efficient approach has been set up for fabricating highly active sulfated titania-silica (SO(4)(2-)/TiO(2)-SiO(2)): Ti(SO(4))(2) was hydrolyzed in the presence of silica, making it possible to sulfate titania and form titania-silica mixed oxide in one step. This study was focused on investigating the roles of sulfate species and silica in improving the physicochemical properties and photoactivity of SO(4)(2-)/TiO(2)-SiO(2) through comparison with sulfated titania (SO(4)(2-)/TiO(2)) and sulfate-free catalysts (TiO(2) and TiO(2)-SiO(2)). Various characterization methods, including X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and surface photovoltage spectroscopy (SPS), were employed to test these materials. The results revealed that for SO(4)(2-)/TiO(2) and TiO(2)-SiO(2) the sole presence of either sulfate species or silica imposes negative effects on the photocatalysis behavior of titania, leading them to have negligible photoactivities. On the contrary, in the case of SO(4)(2-)/TiO(2)-SiO(2), sulfate species and silica were proved to act in a cooperative manner; therefore, the following enhanced structure and surface properties of SO(4)(2-)/TiO(2)-SiO(2) were obtained: (i) relatively well-crystallized and smaller-size (15.4 nm) anatase-phase titania was formed upon 500 degrees C calcination without forming rutile phase and (ii) the formation of active surface sulfate species promotes the separation of photoinduced electron-hole pairs and therefore accelerates the photocatalysis reaction. Therefore, its photoactivity is enhanced as a result of the favorable synergic effects between sulfate species and silica due to their simultaneous presence.

摘要

已经建立了一种简单有效的方法来制备高活性硫酸化二氧化钛 - 二氧化硅(SO(4)(2-)/TiO(2)-SiO(2)):Ti(SO(4))(2) 在二氧化硅存在下进行水解,使得一步实现二氧化钛的硫酸化并形成二氧化钛 - 二氧化硅混合氧化物成为可能。本研究旨在通过与硫酸化二氧化钛(SO(4)(2-)/TiO(2))和无硫酸盐催化剂(TiO(2) 和 TiO(2)-SiO(2))比较,研究硫酸根物种和二氧化硅在改善 SO(4)(2-)/TiO(2)-SiO(2) 的物理化学性质和光活性方面的作用。采用了各种表征方法,包括 X 射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、X 射线光电子能谱(XPS)和表面光电压光谱(SPS)来测试这些材料。结果表明,对于 SO(4)(2-)/TiO(2) 和 TiO(2)-SiO(2),单独存在硫酸根物种或二氧化硅都会对二氧化钛的光催化行为产生负面影响,导致它们的光活性可忽略不计。相反,在 SO(4)(2-)/TiO(2)-SiO(2) 的情况下,硫酸根物种和二氧化硅被证明以协同方式起作用;因此,获得了以下增强的 SO(4)(2-)/TiO(2)-SiO(2) 的结构和表面性质:(i)在 500℃煅烧时形成了结晶度相对较好且尺寸较小(15.4nm)的锐钛矿相二氧化钛,未形成金红石相;(ii)活性表面硫酸根物种的形成促进了光生电子 - 空穴对的分离,因此加速了光催化反应。因此,由于硫酸根物种和二氧化硅同时存在所产生的有利协同效应,其光活性得到增强。

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