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可见光下碳掺杂二氧化钛、氮掺杂二氧化钛及碳氮共掺杂二氧化钛对2-氯苯酚的光催化氧化:羟基自由基的形成及动力学研究

Formation of hydroxyl radicals and kinetic study of 2-chlorophenol photocatalytic oxidation using C-doped TiO2, N-doped TiO2, and C,N Co-doped TiO2 under visible light.

作者信息

Ananpattarachai Jirapat, Seraphin Supapan, Kajitvichyanukul Puangrat

机构信息

Center of Excellence on Environmental Research and Innovation, Faculty of Engineering, Naresuan University, Phitsanulok, 65000, Thailand.

Department of Materials Science and Engineering, University of Arizona, Tucson, AZ, 85721, USA.

出版信息

Environ Sci Pollut Res Int. 2016 Feb;23(4):3884-96. doi: 10.1007/s11356-015-5570-8. Epub 2015 Oct 26.

Abstract

This work reports on synthesis, characterization, adsorption ability, formation rate of hydroxyl radicals (OH(•)), photocatalytic oxidation kinetics, and mineralization ability of C-doped titanium dioxide (TiO2), N-doped TiO2, and C,N co-doped TiO2 prepared by the sol-gel method. X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and UV-visible spectroscopy were used to analyze the titania. The rate of formation of OH(•) for each type of titania was determined, and the OH-index was calculated. The kinetics of as-synthesized TiO2 catalysts in photocatalytic oxidation of 2-chlorophenol (2-CP) under visible light irradiation were evaluated. Results revealed that nitrogen was incorporated into the lattice of titania with the structure of O-Ti-N linkages in N-doped TiO2 and C,N co-doped TiO2. Carbon was joined to the Ti-O-C bond in the C-doped TiO2 and C,N co-doped TiO2. The 2-CP adsorption ability of C,N co-doped TiO2 and C-doped TiO2 originated from a layer composed of a complex carbonaceous mixture at the surface of TiO2. C,N co-doped TiO2 had highest formation rate of OH(•) and photocatalytic activity due to a synergistic effect of carbon and nitrogen co-doping. The order of photocatalytic activity per unit surface area was the same as that of the formation rate of OH(•) unit surface area in the following order: C,N co-doped TiO2 > C-doped TiO2 > N-doped TiO2 > undoped TiO2.

摘要

本研究报道了通过溶胶-凝胶法制备的碳掺杂二氧化钛(TiO₂)、氮掺杂TiO₂和碳氮共掺杂TiO₂的合成、表征、吸附能力、羟基自由基(OH(•))的生成速率、光催化氧化动力学及矿化能力。采用X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)和紫外可见光谱对二氧化钛进行分析。测定了每种二氧化钛的OH(•)生成速率,并计算了OH指数。评估了合成的TiO₂催化剂在可见光照射下对2-氯苯酚(2-CP)光催化氧化的动力学。结果表明,在氮掺杂TiO₂和碳氮共掺杂TiO₂中,氮以O-Ti-N键的结构掺入二氧化钛晶格。在碳掺杂TiO₂和碳氮共掺杂TiO₂中,碳与Ti-O-C键相连。碳氮共掺杂TiO₂和碳掺杂TiO₂对2-CP的吸附能力源于TiO₂表面由复杂含碳混合物组成的一层。由于碳和氮共掺杂的协同效应,碳氮共掺杂TiO₂具有最高的OH(•)生成速率和光催化活性。单位表面积的光催化活性顺序与单位表面积的OH(•)生成速率顺序相同,如下所示:碳氮共掺杂TiO₂ > 碳掺杂TiO₂ > 氮掺杂TiO₂ > 未掺杂TiO₂。

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