三水铝石矿物颗粒表面吸附芳香族污染物的计算模拟与预测
Computational simulation and prediction for adsorption of aromatic pollutants on gibbsite mineral particle surface
刘治山 1马芳芳 1徐倩 1谢宏彬1
作者信息
- 1. 大连理工大学环境学院,大连,116024
- 折叠
摘要
了解芳香族污染物在矿物颗粒表面的吸附行为对于评估其大气归趋及影响具有重要意义.吸附能(Eads)是描述芳香族污染物在矿物颗粒表面吸附行为的重要参数,然而,目前该数据十分匮乏.考虑到大气中存在大量的芳香族污染物,逐个揭示芳香族污染物在矿物颗粒表面的Eads值需要巨大的计算资源和工作量.因此,亟需建立一种能够快速预测芳香族污染物在矿物颗粒表面Eads值的预测模型.本研究采取第一性原理的方法,探究了21个芳香族污染物在矿物颗粒三水铝石(001)面上的吸附机制.结果发现,21个芳香族污染物与三水铝石(001)面主要形成氢键、O—H…兀键以及O—H…X(X=Cl/Br)相互作用,其Eads值的范围在-12kcal·mol-1至-30kcal·mol-1之间.基于计算得到的21个Eas值,采用多元线性回归分析方法,建立了预测芳香族污染物在三水铝石(001)面上Eds值的定量结构-活性关系模型.该模型具有很好的拟合优度、稳健性和预测能力,能够用来预测含有—CH3、—OH、—COOH、—NO2、—NH2、—CHO、—F、—Cl、—Br官能团的芳香族污染物.本研究结果对于提高目前对芳香族污染物在矿物颗粒表面上吸附行为的理解具有重要意义,并且为进一步揭示芳香族污染物在三水铝石(001)面上的大气转化奠定了基础.
Abstract
Understanding the adsorption behavior of aromatic pollutants on the surface of mineral particles is significant for evaluating their atmospheric fate and impacts.The adsorption energy(Eads)is a crucial parameter to describe the adsorption behavior of aromatic pollutants on the surface of mineral particles.However,only limited aromatic pollutants(i.e.,naphthalene,anthracene,toluene,phenol,et al.)have so far been studied.In view of the large amounts of aromatic pollutants in the atmosphere,it takes lots of work to evaluate the Eads values of aromatic pollutants on the surface of mineral particles one by one.Therefore,it is necessary to establish a high-throughput prediction model to predict the Eads values of aromatic pollutants on the surface of mineral particles.Herein,we employed first-principles calculations to investigate the adsorption mechanism of 21 aromatic pollutants on gibbsite(001)surface.Results indicated that three types of interactions including hydrogen bonds,O—H…π bonds and O—H…X(X=Cl/Br)are formed between 21 aromatic pollutants and gibbsite(001)surface.The calculated Eads values are in the range of-12—-30 kcal·mol-1.Based on the calculated 21 Eads values,a quantitative structure-activity relationship(QSAR)model for predicting the Eads values of aromatic pollutants on gibbsite(001)surface was established.The model has good goodness of fit,robustness and predictive ability,which can be used to predict the Eads values of aromatic pollutants containing—CH3,—OH,—COOH,—NO2,—NH2,—CHO,—F,—Cl and—Br functional groups.The results expand current understanding of the adsorption mechanism of aromatic pollutants on the surface of mineral particles,and provide a foundation for investigating the atmospheric transformation of aromatic pollutants on gibbsite(001)surface in the further.
关键词
芳香族污染物/三水铝石/吸附能/第一性原理计算/定量结构-活性关系Key words
aromatic pollutants/gibbsite/adsorption energy/first-principles calculations/quantitative structure-activity relationship(QSAR)引用本文复制引用
基金项目
国家自然科学基金(22176022)
国家自然科学基金(22206020)
中国博士后科学基金(2022M720640)
出版年
2024
NETL
NSTL
万方数据