Adsorption of Phenol by Oxidized Multi-Walled Carbon Nanotubes

doi:10.13209/j.0479-8023.2019.061

Acta Scientiarum Naturalium Universitatis Pekinensis ›› 2019, Vol. 55 ›› Issue (5): 961-967.DOI: 10.13209/j.0479-8023.2019.061

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Adsorption of Phenol by Oxidized Multi-Walled Carbon Nanotubes

HAI Hao¹, WANG Ke¹, MA Yibo¹, ZHANG Jing¹, XIA Jianxin¹, XING Xuan^1,†, WANG Ting²

1. College of Life and Environmental Sciences, Minzu University of China, Beijing 100081 2. Department of Environmental Science and Engineering, Peking University, Beijing 100871

Received:2018-08-07 Revised:2018-09-14 Online:2019-09-20 Published:2019-09-20
Contact: XING Xuan, E-mail: xingxuanpku(at)163.com

多壁碳纳米管氧化改性及其对酚类吸附性能的研究

海浩¹, 王可¹, 马忆波¹, 张璟¹, 夏建新¹, 邢璇^1,†, 王婷²

1. 中央民族大学生命与环境科学学院, 北京 100081 2. 北京大学环境科学与工程学院, 北京 100871

通讯作者: 邢璇, E-mail: xingxuanpku(at)163.com
基金资助:
国家自然科学基金(51409285)资助

Abstract

Abstract:

Organic compounds pollution, especially phenolic compounds, has been a serious problem recently. Multi-walled carbon nanotubes (MWCNTs) were oxidized by mixed acid oxidation method to remove phenolic compounds by adsorption. Five typical phenolic compounds including phenol, p-cresol, p-methoxyphenol, phydroxybenzaldehyde and p-nitrophenol were selected and to be adsorbed on MWCNTs and MWCNTs-O, respectively. Results showed that compared with the unmodified MWCNTs, the adsorption capacity of five phenolic compounds on MWCNTs-O increased significantly. The adsorption amount of five phenols on MWCNTs-O was different and the order was p-nitrophenol >p-methoxyphenol > p-hydroxybenzaldehyde > p-cresol > phenol. Adsorption isotherm data for the five phenols fitted Langmuir model well, which proved that phenolic compounds on MWCNTs was monolayer chemisorption. Surface functional groups analyzation of MWCNTs-O indicated that acidic oxygen-containing functional groups increased. TEM and Raman spectroscopy showed the winding degree of MWCNTs decreased, and overall dispersion and the degree of graphitization increased. π-π conjugation between vertical π electrons on MWCNTs-O and π electrons of phenolic compounds was formed and the electronic energy (EE) could be used as indicator for phenols adsorption on MWCNTs-O.

Key words: multi-walled carbon nanotubes, phenols, oxidation modification, adsorption, π-π conjugation

摘要：

针对目前有机废水(尤其是酚类废水)污染严重的问题, 通过混酸氧化法对多壁碳纳米管(multi-walled carbon nanotubes, MWCNTs)进行氧化改性(MWCNT-O), 并研究其改性前后对苯酚、对甲苯酚、对甲氧基苯酚、对羟基苯甲醛和对硝基苯酚5种典型酚的吸附作用。结果表明: 298 K下, 与未改性的MWCNTs相比, MWCNTs-O对5种酚类物质的吸附量均有提升。5种酚类物质在MWCNTs-O表面的吸附量有差别, 顺序为对硝基苯酚>对甲氧基苯酚>对羟基苯甲醛>对甲苯酚>苯酚。吸附过程符合Langmuir吸附等温方程, 主要为单分子层化学吸附。对MWCNTs-O进行表面官能团测试、透射电镜分析和拉曼光谱分析, 发现氧化改性后材料表面的酸性含氧官能团增多, 缠绕度降低, 整体分散性增强, 石墨化程度有所提升。通过研究分子结构与吸附量之间的关系, 发现吸附量与酚类物质的电子能量(electronic energy, EE)有显著的相关性, MWCNTs-O表面垂直的π电子和酚类物质的π电子形成π-π共轭作用。因此, EE 可以作为酚类物质在MWCNTs-O表面平衡吸附量的预测性指标。

关键词: 多壁碳纳米管, 酚类物质, 氧化改性, 吸附, π-π 共轭

HAI Hao, WANG Ke, MA Yibo, ZHANG Jing, XIA Jianxin, XING Xuan, WANG Ting. Adsorption of Phenol by Oxidized Multi-Walled Carbon Nanotubes[J]. Acta Scientiarum Naturalium Universitatis Pekinensis, 2019, 55(5): 961-967.

海浩, 王可, 马忆波, 张璟, 夏建新, 邢璇, 王婷. 多壁碳纳米管氧化改性及其对酚类吸附性能的研究[J]. 北京大学学报自然科学版, 2019, 55(5): 961-967.

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Adsorption of Phenol by Oxidized Multi-Walled Carbon Nanotubes

多壁碳纳米管氧化改性及其对酚类吸附性能的研究

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