无机材料学报 ›› 2020, Vol. 35 ›› Issue (3): 277-283.DOI: 10.15541/jim20190377
所属专题： 2020年环境材料论文精选(三)有机小分子去除； 【虚拟专辑】污染物吸附水处理(2020~2021)
赵超锋1,金佳人1,霍英忠1,孙陆2,艾玥洁1(
)
收稿日期:2019-07-23
修回日期:2019-09-23
出版日期:2020-03-20
网络出版日期:2019-12-04
作者简介:赵超锋(1995-), 男, 硕士研究生. E-mail: cfzhao@ncepu.edu.cn
基金资助:
ZHAO Chaofeng1,JIN Jiaren1,HUO Yingzhong1,SUN Lu2,AI Yuejie1()
Received:2019-07-23
Revised:2019-09-23
Published:2020-03-20
Online:2019-12-04
About author:ZHAO Chaofeng (1995-), male, Master candidate. E-mail:cfzhao@ncepu.edu.cn
Supported by:摘要：
研究采用分子动力学模拟(Molecular dynamics simulation, MD)的方法, 以苯酚、α-萘酚和4-辛基酚为代表, 研究了酚类有机污染物(Phenolic Organic Pollutants, POPs)在氧化石墨烯(Graphene Oxide, GO)上单独和竞争吸附过程。通过自由能计算得到三种POPs在GO表面的吸附能分别为: 4-辛基酚(41.34 kJ/mol)>α-萘酚(33.23 kJ/mol)>苯酚(19.31 kJ/mol)。吸附过程中的主要作用力为POPs的疏水作用, 而分子团簇、范德华相互作用、静电相互作用以及氢键等在一定程度上增加了GO对POPs的吸附能力。在混合体系中, POPs之间存在明显的竞争吸附现象, 吸附过程包含了直接吸附和形成分子团簇的间接性吸附两个过程。本研究结果为含POPs水体的治理以及GO材料的设计和筛选提供了一定的理论依据。
中图分类号:
赵超锋, 金佳人, 霍英忠, 孙陆, 艾玥洁. 氧化石墨烯吸附水体中酚类有机污染物的分子动力学模拟[J]. 无机材料学报, 2020, 35(3): 277-283.
ZHAO Chaofeng, JIN Jiaren, HUO Yingzhong, SUN Lu, AI Yuejie. Adsorption of Phenolic Organic Pollutants on Graphene Oxide: Molecular Dynamics Study[J]. Journal of Inorganic Materials, 2020, 35(3): 277-283.
图1 MD模拟采用的(a)GO模型及其尺寸; (b)苯酚、α-萘酚和4-辛基酚的结构; (c)立方盒子的尺寸及苯酚(绿色)、α-萘酚(紫色)和4-辛基酚(黄色)在GO表面竞争吸附体系的初始结构
Fig. 1 (a) GO model, (b) structures of phenol, α-naphthol and 4-octyl-phenol molecules in MD simulations, and (c) initial configuration of phenol (green), α-naphthol (purple) and 4-octyl-phenol (yellow) molecules in the competitive system
图S1 (a)苯酚、(b)α-萘酚和(c)4-辛基酚单独吸附体系的初始结构图
Fig. 2771 Initial configurations of (a) phenol, (b) α-naphthol and (c) 4-octyl-phenol molecules in the independent system
图2 (a)苯酚、(b)α-萘酚和(c)4-辛基酚在GO表面单独吸附的平衡结构
Fig. 2 Equilibrium structures of (a) phenol, (b) α-naphthol and (c) 4-octyl-phenol molecules adsorbed on GO surface
图3 竞争吸附体系中苯酚(绿色)、α-萘酚(紫色)和4-辛基酚(黄色)在GO表面不同时刻的吸附结构图
Fig. 3 Snapshots of competitive system from simulation process at different time Phenol, α-naphthol and 4-octyl-phenol molecules are shown as green, purple and yellow molecules, respectively. Water molecules are not shown to highlight the configuration
图4 竞争吸附体系中每一个(a)苯酚、(b)α-萘酚和(c)4-辛基酚分子与GO之间质心距离随时间的变化
Fig. 4 Distances of centers of mass between GO and each (a) phenol, (b) α-naphthol and (c) 4-octyl-phenol molecule, as function of time
图5 (a)竞争吸附体系中三种POPs之间的相互作用能量, (b)单独和(c)竞争体系中POPs最大团簇中的分子数, (d)单独和(e)竞争体系中POPs在GO表面的径向分布函数曲线(g(r))以及半径r范围内相应的分子数目曲线(n(r))
Fig. 5 (a) Interaction energies between different POPs molecules in competitive system; The maximal cluster size of POPs in (b) independent and (c) competitive systems, respectively; The radial distribution functions (g(r)) and coordination numbers (n(r)) of POPs in (d) independent and (e) competitive systems, respectively
图6 (a)苯酚、α-萘酚和4-辛基酚分子的吸附自由能; GO与POPs在(b)单独和(c)竞争体系中的相互作用能量; POPs在(d)单独和(e)竞争体系中的疏水面积; GO与POPs官能团在(f)单独和(g)竞争体系中形成的氢键数目
Fig. 6 (a) Potential of mean force of POPs molecules; The interaction energies between GO and POPs molecules in (b) independent and (c) competitive systems, respectively; The hydrophobic areas of POPs molecules in (d) independent and (e) competitive systems, respectively; The hydrogen bonds between GO and POPs molecules in (f) independent and (g) competitive systems, respectively
| Time/ns | Phenol/(kJ•mol-1) | α-naphthol/(kJ•mol-1) | 4-octyl-phenol/(kJ•mol-1) | ||||||
|---|---|---|---|---|---|---|---|---|---|
| Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | |
| 20 | -44.10 | -866.02 | -910.12 | -317.12 | -1172.76 | -1489.87 | -195.98 | -1311.17 | -1507.15 |
| 40 | -174.71 | -877.44 | -1052.16 | -388.46 | -1276.89 | -1665.35 | -162.60 | -1359.01 | -1521.60 |
| 60 | -124.19 | -897.25 | -1021.45 | -405.37 | -1243.64 | -1649.01 | -96.07 | -1340.12 | -1436.19 |
| 80 | -167.61 | -864.44 | -1032.05 | -358.80 | -1313.62 | -1672.42 | -125.83 | -1454.64 | -1580.47 |
| 100 | -237.23 | -880.63 | -1117.87 | -251.36 | -1338.97 | -1590.33 | -62.78 | -1344.93 | -1407.71 |
表S1 在单独吸附体系中GO与苯酚、α-萘酚、4-辛基酚分子在不同时刻的相互作用能量
Table S1 Interaction energies between GO and POPs molecules in independent system at different periods
| Time/ns | Phenol/(kJ•mol-1) | α-naphthol/(kJ•mol-1) | 4-octyl-phenol/(kJ•mol-1) | ||||||
|---|---|---|---|---|---|---|---|---|---|
| Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | |
| 20 | -44.10 | -866.02 | -910.12 | -317.12 | -1172.76 | -1489.87 | -195.98 | -1311.17 | -1507.15 |
| 40 | -174.71 | -877.44 | -1052.16 | -388.46 | -1276.89 | -1665.35 | -162.60 | -1359.01 | -1521.60 |
| 60 | -124.19 | -897.25 | -1021.45 | -405.37 | -1243.64 | -1649.01 | -96.07 | -1340.12 | -1436.19 |
| 80 | -167.61 | -864.44 | -1032.05 | -358.80 | -1313.62 | -1672.42 | -125.83 | -1454.64 | -1580.47 |
| 100 | -237.23 | -880.63 | -1117.87 | -251.36 | -1338.97 | -1590.33 | -62.78 | -1344.93 | -1407.71 |
| Time/ns | Phenol/(kJ•mol-1) | α-naphthol/(kJ•mol-1) | 4-octyl-phenol/(kJ•mol-1) | ||||||
|---|---|---|---|---|---|---|---|---|---|
| Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | |
| 20 | -160.11 | -448.40 | -608.51 | -235.85 | -914.54 | -1150.38 | -71.34 | -980.56 | -1051.90 |
| 40 | -240.86 | -533.62 | -774.48 | -288.30 | -960.43 | -1248.73 | -182.74 | -928.42 | -1111.16 |
| 60 | -334.12 | -573.27 | -907.39 | -354.11 | -993.34 | -1347.46 | -152.72 | -1013.83 | -1166.55 |
| 80 | -215.40 | -672.38 | -887.78 | -363.20 | -959.82 | -1323.02 | -201.10 | -912.11 | -1113.20 |
| 100 | -214.74 | -674.05 | -888.79 | -305.51 | -1069.33 | -1374.84 | -179.30 | -918.63 | -1097.92 |
表S2 在竞争吸附过程中GO与苯酚、α-萘酚、4-辛基酚分子在不同时刻的相互作用能量
Table S2 Interaction energies between GO and POPs molecules in competitive system at different periods
| Time/ns | Phenol/(kJ•mol-1) | α-naphthol/(kJ•mol-1) | 4-octyl-phenol/(kJ•mol-1) | ||||||
|---|---|---|---|---|---|---|---|---|---|
| Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | Coulomb interaction | L-J Potential | Total | |
| 20 | -160.11 | -448.40 | -608.51 | -235.85 | -914.54 | -1150.38 | -71.34 | -980.56 | -1051.90 |
| 40 | -240.86 | -533.62 | -774.48 | -288.30 | -960.43 | -1248.73 | -182.74 | -928.42 | -1111.16 |
| 60 | -334.12 | -573.27 | -907.39 | -354.11 | -993.34 | -1347.46 | -152.72 | -1013.83 | -1166.55 |
| 80 | -215.40 | -672.38 | -887.78 | -363.20 | -959.82 | -1323.02 | -201.10 | -912.11 | -1113.20 |
| 100 | -214.74 | -674.05 | -888.79 | -305.51 | -1069.33 | -1374.84 | -179.30 | -918.63 | -1097.92 |
图S2 单独吸附体系中(a)苯酚、(b)α-萘酚和(c)4-辛基酚的溶剂可及表面积(solvent accessible surface area, SASA)随时间的变化
Fig. S2 SASAs of (a) phenol, (b) α-naphthol and (c) 4-octyl-phenol molecules in the independent system
图S3 竞争吸附体系中(a)苯酚、(b)α-萘酚和(c)4-辛基酚的SASAs随时间的变化
Fig. S3 SASAs of (a) phenol, (b) α-naphthol and (c) 4-octyl-phenol molecules in the competitive system
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