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活性炭负载TiO₂对罗丹明B的微波光催化降解:机理研究

Microwave photocatalytic degradation of Rhodamine B using TiO2 supported on activated carbon: mechanism implication.

作者信息

He Zhong, Yang Shaogui, Ju Yongming, Sun Cheng

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210093, China.

出版信息

J Environ Sci (China). 2009;21(2):268-72. doi: 10.1016/s1001-0742(08)62262-7.

Abstract

The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM) and Brunauer-Emmett-Teller (BET). In the process of microwave-enhanced photocatalysis (MPC), RhB (30 mg/L) was almost completely decoloured in 10 min, and the mineralization efficiency was 96.0% in 20 min. The reaction rate constant of RhB in MPC using TiO2-AC by pseudo first-order reaction kinetics was 4.16 times of that using Degussa P25. Additionally, according to gas chromatography/mass spectrometry (GC/MS) and liquid chromatography/mass spectrometry (LC/MS) identification, the major intermediates of RhB in MPC included two kinds of N-de-ethylation intermediates (N,N-diethyl-N'-ethyl-rhodamine (DER)), oxalic acid, malonic acid, succinic acid, and phthalic acid, maleic acid, 3-nitrobenzoic acid, and so on. The degradation of RhB in MPC was mainly attributed to the destruction of the conjugated structure, and then the intermediates transformed to acid molecules which were mineralized to water and carbon dioxide.

摘要

采用负载在活性炭上的二氧化钛(TiO₂-AC)在微波辐射下对罗丹明B(RhB)进行光催化降解。制备了复合催化剂TiO₂-AC,并通过X射线衍射(XRD)、透射电子显微镜(TEM)和布鲁诺尔-埃米特-泰勒(BET)法对其进行了表征。在微波强化光催化(MPC)过程中,30 mg/L的RhB在10分钟内几乎完全脱色,20分钟内矿化效率为96.0%。采用TiO₂-AC通过准一级反应动力学进行MPC时,RhB的反应速率常数是使用德固赛P25时的4.16倍。此外,根据气相色谱/质谱(GC/MS)和液相色谱/质谱(LC/MS)鉴定,MPC中RhB的主要中间体包括两种N-脱乙基中间体(N,N-二乙基-N'-乙基罗丹明(DER))、草酸、丙二酸、琥珀酸、邻苯二甲酸、马来酸、3-硝基苯甲酸等。MPC中RhB的降解主要归因于共轭结构的破坏,然后中间体转化为酸性分子,这些酸性分子被矿化为水和二氧化碳。

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