Photocatalytic degradation kinetics and mechanism of antivirus drug-lamivudine in TiO2 dispersion

Photocatalytic degradation kinetics and mechanism of antivirus drug-lamivudine in TiO2 dispersion
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抗病毒药物拉米夫定在TiO2分散体中的光催化降解动力学及机理

DOI:
10.1016/j.jhazmat.2011.09.077
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发表时间:
2011-12-15
影响因子:
13.6
通讯作者:
Nie, Xiangping
Nie, Xiangping
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
An, Taicheng;An, Jibin;Nie, Xiangping

文献摘要

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基于响应面法,采用单变量单次设计和中心复合设计,系统优化了抗病毒药物拉米夫定在TiO2水溶液分散体中的光催化降解动力学。选取TiO2含量、初始pH和拉米夫定浓度三个变量,考察拉米夫定降解效率与自变量的关系。响应面法模拟结果表明,TiO2含量和初始拉米夫定浓度对拉米夫定的降解效率影响较大。当TiO2用量合适且初始拉米夫定浓度保持在最低时,降解效率最高。此外,通过添加不同的清除剂,研究了光催化过程中产生的各种主要反应物质的贡献实验,发现羟基自由基是参与拉米夫定在水相TiO2中降解的主要反应物质。采用HPLC/MS/MS鉴定了6种降解中间体,并结合HPLC/MS/MS、离子色谱、总有机碳和前沿电子密度、点电荷等理论数据,提出了拉米夫定光催化降解机理。(C) 2011 Elsevier B.V.版权所有
Photocatalytic degradation kinetics of antivirus drug-lamivudine in aqueous TiO2 dispersions was systematically optimized by both single-variable-at-a-time and central composite design based on the response surface methodology. Three variables, TiO2 content, initial pH and lamivudine concentration, were selected to determine the dependence of degradation efficiencies of lamivudine on independent variables. Response surface methodology modeling results indicated that degradation efficiencies of lamivudine were highly affected by TiO2 content and initial lamivudine concentration. The highest degradation efficiency was achieved at suitable amount of TiO2 and with maintaining initial lamivudine concentration to a minimum. In addition, the contribution experiments of various primary reactive species produced during the photocatalysis were investigated with the addition of different scavengers and found that hydroxyl radicals was the major reactive species involved in lamivudine degradation in aqueous TiO2. Six degradation intermediates were identified using HPLC/MS/MS, and photocatalytic degradation mechanism of lamivudine was proposed by utilizing collective information from both experimental results of HPLC/MS/MS, ion chromatography as well as total organic carbon and theoretical data of frontier electron densities and point charges. (C) 2011 Elsevier B.V. All rights reserved.