摘要
有机污染物的环境归趋主要由其分配性质决定,如正辛醇/水分配系数(K_(OW)).本文采用密度泛函理论,在B3LYP/6-311G^(**)的水平上对PAEs的结构进行优化振动分析,Gaussian输出的15种量子化学参数被用来对该类物质正辛醇/水分配系数(K_(OW))进行定量结构-性质关系(QSPR)研究.采用一种顺序方法:相关分析、主成分分析、多元线性回归和统计验证,建立了QSPR模型.结果表明,单个描述符(平均极化率α)在确定K_(OW)中起重要作用,显式函数关系式为lg K_(OW)=-3.468+0.041α,lg K_(OW)的值随着α的增大而线性增大.模型具有良好的拟合能力(R^2=0.99,RMSE=0.33)、稳健性(Q^2_(LOO)=0.97,Q^2_(BOOT)=0.98)和预测能力(Q^2_(ext)=0.98),可利用该模型对其他PAEs分子的lg K_(OW)进行预测.
The environmental fate of organic pollutants is governed primarily by their partitioning property such as n-octanol/water partition coefficient（ KOW）. In this work Density functional theory（ DFT） calculations at the B3 LYP/6-311 G＊＊level of theory were carried out to optimize the geometries and vibrational analysis of all the phthalic acid esters. From the Gaussian output files,15 theoretical parameters were obtained and were used for the quantitative structure-property relationship（ QSPR） study for KOW. In the present study,the development of the QSPR model employed a sequential approach： correlation analysis,principal component analysis,multi-linear regression. The result indicates that the single descriptor,average polarizability（ α）,plays an important role in determining the partitioning properties with a global standardized function of lg KOW=-3.468＋0.041α,from which we can see that the values of lg KOW increased with the increase of α. The resulting model had satisfactory goodness-of-fit（ R-2= 0.99,RMSE = 0.33）,robustness（ QLOO^2= 0.97,QBOOT^2= 0.98）and predictive ability（ Qext^2= 0.98）,so it can be used to predict the lg KOWvalues for other PAEs.
作者
渠艳飞
马邕文
万金泉
王艳
QU Yanfei;MA Yongwen;WAN Jinquan;WANG Yan(College of Environment and Energy, South China University of Technology, Guangzhou, 510006, China;The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, South China University of Technology,Guangzhou, 510006, China;State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, 510641, China)
出处
《环境化学》
CAS
CSCD
北大核心
2017年第11期2325-2332,共8页
Environmental Chemistry
基金
国家自然科学基金(31570568
31670585)
制浆造纸重点实验室开放基金(201535)
广州市科技计划项目(201607010079
201607020007)
广东省科技计划项目(2016A020221005)资助~~
