分子模拟多溴联苯醚在石英砂纳米孔中的吸附行为.pdf

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分子模拟多溴联苯醚在石英砂纳米孔中的吸附行为
隋红3,李琳·3,陈道穀2,吴国钟
(天津大学化工学院精馏技术国家工程研究中心,天津30002:2清华大学深圳研究生院海洋学部,深圳市
近海动力环境演变重点实验室,广东深圳518055;3天津化学化工协同创新中心,天津300072
摘要:多溴联苯醚(PBDE)是一种广泛使用的阻燃剂,也是普遍关注的持久性有机污染物之一。利用分子模拟
手段建立5种低溴代PBDF分子(BDE-28、BDE-47、BDE-77、BDE-99、BDE-153)在石英砂纳米孔(2.0nm、
2.5nm、3.0m、3.5nm)中的吸附模型,利用孔径变化模拟土壤的物理老化过程,并研究土壤有机质(SOM)对
PBDE吸附能与均方位移(MSD)的影响。结果表明,孔径的缩小降低了体系的总势能和非键能,使其体系更加
稳定;然而PBDE与石英砂之间的吸附能随孔径的縮小而增大,且该吸附能以范德华力为主,占体系吸附能的
84.0%。SOM的加入则导致体系的总势能和非键能以及PBDE与石英砂之间的吸附能均降低,虽然与石英砂孔
内表面的吸附能降低有利于PBDE分子的迁移,但由于SOM与PBDE之间的吸附作用占主导,抑制了PBDE在
纳米孔中的扩散,因此PBDE的MSD值反而降低。
关键词:分子模拟;多溴联苯醚;石英砂纳米孔;土壤有机质;吸附
中图分类号:X131.3文献标志码:A文章编号:1000-6613(2015)09-3444-08
DO:10.16085/ ]. Issn.1000-6613、2015.09.037
Molecular dynamic simulation of adsorption of poly brominated diphenyl
ethers in silica nanopores
SUI Hong ", LI Lin
CHEN Daoyi, WU Guozhong
National Engineering Research Center of Distillation Technology, School of Chemical Engineering and Technology
Tianjin University, Tianjin 300072, China; Shenzhen Key Laboratory for Coastal Ocean Dynamics and Environment
Division of Ocean Science and Technology, Graduate School at Shenzhen, Tsinghua University, Shenzhen 518055
Guangdong, China; Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China)
Abstract: Polybrominated diphenyl ethers (PBDES)are widely used flame retardants, which have
become one branch of persistent organic pollutants with worldwide concern. In order to investigate
adsorption of PBDES in silica nanopores, molecular dynamic simulations were performed for five
PBDES, including BDE-28, BDE-47, BDE-77, BDE-99 and BDE-153 in silica nanopores with
respective apertures of 2.Onm, 2.5nm, 3.Onm and 3.5nm. The system energy declined with the decrease
in aperture, but an opposite tendency was observed for the adsorption energy between PBDES and
silica nanopores. The adsorption energy was dominated by van der Waals force which accounted for
84.0% of the overall adsorption energy. The mean square displacement(MSD)values for PBDES in the
silica nanopores decreased with the increase of adsorption energy. Additionally, the presence of soil
收稿日期:2015-02-02;修改稿日期:2015-04-10
项目(201309006)。
基金项目:国家自然科学基金(41471258)、天津市自然科学基金第一作者:隋红(1976-),女,副教授,主要从事士壤修复、精馏
(12 JCQNJC0S30)、深堋市近海动力环境演变重点实验室项目方面的研究。联系人:吴国钟,讲师,主要从事石油污染士的环境
(ZDSY20130402163735964)、深圳市海外高层次人オ创新创业专项
评估与修复研究。E-mailw.guozhong@sz.tsinghua.edu.cn
项目(KQC20110950083A)及国家环境保护公益性行业科研专项