Mechanistic QSAR models for interpreting degradation rates of sulfonamides in UV-photocatalysis systems
Mechanistic QSAR models for interpreting degradation rates of sulfonamides in UV-photocatalysis systems
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用于解释紫外光催化系统中磺胺类药物降解率的机械 QSAR 模型
DOI：
10.1016/j.chemosphere.2015.05.075
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发表时间：
2015-11-01
期刊：
影响因子：
8.8
通讯作者：
Zou, Xiaoming
中科院分区：
文献类型：
--
作者：
Huang, Xiangfeng;Feng, Yi;Zou, Xiaoming
光催化法是处理抗生素废水最有效的方法之一。因此，确定抗生素在降解过程中的降解速率与其结构特征之间的关系具有重要意义。研究了纳米二氧化钛（nTiO（2））与紫外光（UV）和nTiO（2）/活性炭纤维（ACF）与UV组成的光催化体系对10种磺胺类药物的光催化降解特性。结果表明，SA的最大表观降解速率常数（Kapp）约为最小表观降解速率常数的5倍。基于降解机理和偏最小二乘回归（PLS）方法，建立了两个体系的最佳定量构效关系（QSAR）模型。机理模型表明，水杨酸在TiO 2体系中的降解规律与其最高占据分子轨道（E-homo）、亲核进攻最大值（f（+）（x））和主链原子上最负部分电荷最小值（q（C）（min））密切相关，而OH自由基的最大攻击值f（0）（x）和表观吸附速率常数k（ad）是影响活性炭在TiO 2/ACF体系中降解规律的关键因素。(C)2015爱思唯尔有限公司版权所有。
Photocatalysis is one of the most effective methods for treating antibiotic wastewater. Thus, it is of great significance to determine the relationship between degradation rates and structural characteristics of antibiotics in photocatalysis processes. In the present study, the photocatalytic degradation characteristics of 10 sulfonamides (SAs) were studied using two photocatalytic systems composed of nanophase titanium dioxide (nTiO(2)) plus ultraviolet (UV) and nTiO(2)/activated carbon fiber (ACF) plus UV. The results indicated that the largest apparent SA degradation rate constant (K-app) is approximately 5 times as large as that of the smallest one. Based on the degradation mechanism and the partial least squares regression (PLS) method, optimum Quantitative Structure Activity Relationship (QSAR) models were developed for the two systems. Mechanistic models indicated that the degradation rule of SAs in the TiO2 systems strongly relates to their highest occupied molecular orbital (E-homo), the maximum values of nucleophilic attack (f(+)(x)), and the minimum values of the most negative partial charge on a main-chain atom (q(C)(min)), whereas the maximum values of OH radical attack (f(0)(x)) and the apparent adsorption rate constant values (k(ad)) are key factors affecting the degradation rule of SAs in the TiO2/ACF system. (C) 2015 Elsevier Ltd. All rights reserved.