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制备一种磁铁矿/重氮官能化还原氧化石墨烯杂化物作为易于再生的吸附剂,用于从水溶液中高效去除氯酚。

Fabrication of a magnetite/diazonium functionalized-reduced graphene oxide hybrid as an easily regenerated adsorbent for efficient removal of chlorophenols from aqueous solution.

作者信息

Shen Xiaoqin, Chen Xiaolei, Sun Dejun, Wu Tao, Li Yujiang

机构信息

Shandong Provincial Research Center for Water Pollution Control, School of Environmental Science & Engineering, Shandong University Jinan 250100 PR China

Key Laboratory of Colloid & Interface Science of Education Ministry, Shandong University Jinan 250100 PR China

出版信息

RSC Adv. 2018 Feb 15;8(14):7351-7360. doi: 10.1039/c8ra00503f. eCollection 2018 Feb 14.

Abstract

A magnetic hybrid nanomaterial, which contains magnetite (FeO) particles and diazonium functionalized-reduced graphene oxide (DF-RGO), was fabricated a three-pot reaction. First, the reduced graphene oxide (RGO) was synthesized a redox reaction. Second, diazonium functionalized-RGO was prepared a feasible chemical reaction. Third, FeO particles were loaded onto the surface of DF-RGO by covalent bonding, fabricating the M-DF-RGO hybrid. The fabricated hybrid was characterized by SEM, TEM, AFM, XRD, XPS, FT-IR, TGA, Raman spectroscopy, and magnetometry. The resulting M-DF-RGO hybrid possessed unique magnetic properties and was applied to remove 4-chlorophenol (4-CP) and 2,4-dichlorophenol (2,4-DCP) from aqueous solution. The adsorption of 4-CP and 2,4-DCP on the M-DF-RGO hybrid was performed under various conditions, with respect to initial chlorophenol concentration, pH, and contact time. The results suggest that the adsorption of 4-CP and 2,4-DCP onto the M-DF-RGO hybrid is strongly dependent on pH and weakly dependent on contact time. In addition, the adsorption isotherm of 4-CP and 2,4-DCP on the M-DF-RGO hybrid fits the Freundlich model well and the adsorption capacities of 4-CP and 2,4-DCP on M-DF-RGO reached 55.09 and 127.33 mg g, respectively, at pH 6 and 25 °C. In this situation, intermolecular interactions including π-π interactions and hydrogen bonding are operative. The calculated results of density functional theory further demonstrate that 2,4-DCP molecules could be more easily absorbed than 4-CP molecules by the M-DF-RGO hybrid. Moreover, the M-DF-RGO hybrid could be easily separated by a magnetic separation process, and showed good recyclability of more than five cycles.

摘要

一种包含磁铁矿(FeO)颗粒和重氮官能化还原氧化石墨烯(DF-RGO)的磁性杂化纳米材料通过三锅反应制备而成。首先,通过氧化还原反应合成还原氧化石墨烯(RGO)。其次,通过可行的化学反应制备重氮官能化RGO。第三,通过共价键将FeO颗粒负载到DF-RGO表面,制备出M-DF-RGO杂化物。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、原子力显微镜(AFM)、X射线衍射(XRD)、X射线光电子能谱(XPS)、傅里叶变换红外光谱(FT-IR)、热重分析(TGA)、拉曼光谱和磁力测定对制备的杂化物进行表征。所得的M-DF-RGO杂化物具有独特的磁性,并应用于从水溶液中去除4-氯苯酚(4-CP)和2,4-二氯苯酚(2,4-DCP)。在各种条件下,针对初始氯苯酚浓度、pH值和接触时间,对4-CP和2,4-DCP在M-DF-RGO杂化物上的吸附进行了研究。结果表明,4-CP和2,4-DCP在M-DF-RGO杂化物上的吸附强烈依赖于pH值,而对接触时间的依赖性较弱。此外,4-CP和2,4-DCP在M-DF-RGO杂化物上的吸附等温线很好地符合Freundlich模型,在pH值为6和25℃时,4-CP和2,4-DCP在M-DF-RGO上的吸附容量分别达到55.09和127.33 mg/g。在这种情况下,包括π-π相互作用和氢键在内的分子间相互作用起作用。密度泛函理论的计算结果进一步表明,M-DF-RGO杂化物对2,4-DCP分子的吸附比4-CP分子更容易。此外,M-DF-RGO杂化物可以通过磁分离过程轻松分离,并且显示出超过五个循环的良好可回收性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60a9/9078394/f4bf5755f9fc/c8ra00503f-f1.jpg

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