氟改性纳米TiO2的制备及其光催化降解甲基橙机理

doi:10.3866/PKU.WHXB20110520

物理化学学报 >> 2011, Vol. 27 >> Issue (05): 1149-1156.doi: 10.3866/PKU.WHXB20110520

氟改性纳米TiO₂的制备及其光催化降解甲基橙机理

蒋晶晶, 龙明策, 吴德勇, 蔡伟民

上海交通大学环境科学与工程学院, 上海 200240

收稿日期:2010-10-20 修回日期:2011-03-01 发布日期:2011-04-28
通讯作者: 龙明策 E-mail:long_mc@sjtu.edu.cn
基金资助:
高等学校博士学科点专项科研基金新教师基金(20090073120042)资助项目

Preparation of F-Modified Nanosized TiO₂ and Its Methyl Orange Photodegradation Mechanism

JIANG Jing-Jing, LONG Ming-Ce, WU De-Yong, CAI Wei-Min

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China

Received:2010-10-20 Revised:2011-03-01 Published:2011-04-28
Contact: LONG Ming-Ce E-mail:long_mc@sjtu.edu.cn
Supported by:
The project was supported by the Specialized Research Fund for the Doctoral Program of Higher Education of China (20090073120042).

摘要/Abstract

摘要：

采用简易的沉淀-氟化-回流晶化法在低温下制备了氟改性纳米TiO₂ (F-TiO₂), 并通过透射电镜(TEM), X射线衍射(XRD), 傅里叶变换红外(FTIR)光谱, X射线光电子能谱(XPS)和漫反射光谱(DRS)等表征手段研究了粉末的形貌、晶型、元素形态和光吸收性质. 结果表明: 实验制得的F-TiO₂为椭圆形纳米颗粒, 粒径为5-8 nm; 氟离子能够有效抑制板钛矿相TiO₂的生成, 并同时提高锐钛矿相TiO₂的晶化度; 修饰的氟主要分布在TiO₂表面, 以化学吸附态为主, 并伴有少量的间隙氟. 光催化降解甲基橙的实验表明, 氟离子改性的TiO₂同时具有较高的全谱和可见光催化活性. 通过碱洗和焙烧的对照实验分析可知, F-TiO₂在可见光下降解甲基橙的机理是源于一种由TiO₂表面吸附氟和间隙氟共同增强的染料敏化降解作用.

关键词: 氟改性, 二氧化钛, 回流, 可见光活性, 染料敏化

Abstract:

Fluorine-modified nanosized TiO₂ (F-TiO₂) was prepared by a facile precipitation-fluorination- reflux method. Characterizations of transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and diffuse reflectance spectroscopy (DRS) were carried out to investigate various properties of the as-prepared F-TiO₂ powder. We found that the F-TiO₂ particles were small (5-8 nm) and ellipsoidal in shape. The presence of fluorine not only suppressed the formation of a brookite phase, but also improved the crystallinity of the anatase phase. The fluorine atoms were mainly distributed on the surface of TiO₂, and existed in both forms of chemical-adsorption and interstitial-doping. Compared to pure titania, the fluorine-modified TiO₂ powder showed a much higher methyl orange (MO) degradation efficiency under UV light and under visible light. Through the experiments of alkaline washing and heat treatment, we found that the increased MO degradation rate under visible light irradiation was caused by the enhanced self- degradation of the dye over the surface-modified TiO₂.

Key words: Fluorine-modification, Titanium dioxide, Reflux, Visible-light activity, Dye sensitization

MSC2000:

O643

蒋晶晶, 龙明策, 吴德勇, 蔡伟民. 氟改性纳米TiO₂的制备及其光催化降解甲基橙机理[J]. 物理化学学报, 2011, 27(05): 1149-1156.

JIANG Jing-Jing, LONG Ming-Ce, WU De-Yong, CAI Wei-Min. Preparation of F-Modified Nanosized TiO₂ and Its Methyl Orange Photodegradation Mechanism[J]. Acta Phys. -Chim. Sin., 2011, 27(05): 1149-1156.

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氟改性纳米TiO₂的制备及其光催化降解甲基橙机理

Preparation of F-Modified Nanosized TiO₂ and Its Methyl Orange Photodegradation Mechanism

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