化工进展 ›› 2022, Vol. 41 ›› Issue (2): 881-891.DOI: 10.16085/j.issn.1000-6613.2021-0109

• 材料科学与技术 • 上一篇    下一篇

Fe3O4@PGMA-Arg磁性吸附剂的制备及对亚铁离子的吸附性能

田忠宇(), 杨敬一(), 王怿兴, 徐心茹   

  1. 华东理工大学化工学院, 绿色能源化工国际联合研究中心,上海 200237
  • 收稿日期:2021-01-16 修回日期:2021-04-07 出版日期:2022-02-05 发布日期:2022-02-23
  • 通讯作者: 杨敬一
  • 作者简介:田忠宇(1992—),男,硕士研究生,研究方向为石油化学。E-mail:tianzysl@163.com

Preparation of Fe3O4@PGMA-Arg magnetic adsorbents and its adsorption performance for ferrous ion

TIAN Zhongyu(), YANG Jingyi(), WANG Yixing, XU Xinru   

  1. International Joint Research Center of Green Energy Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
  • Received:2021-01-16 Revised:2021-04-07 Online:2022-02-05 Published:2022-02-23
  • Contact: YANG Jingyi

摘要:

为脱除油田采出水中的Fe(Ⅱ)合成磁性吸附剂,本文以溶剂热法制得亲水性Fe3O4纳米颗粒,使用盐酸多巴胺(DA)进行包覆得到Fe3O4@PDA,再以甲基丙烯酸缩水甘油酯(GMA)在其表面聚合接枝得到Fe3O4@PGMA,后经精氨酸(Arg)修饰后得到功能化的Fe3O4@PGMA-Arg。通过红外光谱、X射线光电子能谱、X射线衍射和磁化强度对制备的纳米颗粒进行表征,结果表明Fe3O4@PGMA-Arg中具有伯胺、亚胺双键、羟基和羧基官能团,其中伯胺基团和亚胺双键上的N可与Fe(Ⅱ)形成配位键,羟基和羧基的O可与Fe(Ⅱ)形成配位键,从而达到吸附Fe(Ⅱ)的目的。合成产物仍保持了Fe3O4的反尖晶石结构,具有好的磁响应性能。通过静态吸附实验探究吸附条件对Fe3O4@PGMA-Arg吸附Fe(Ⅱ)的影响因素,结果表明,Fe(Ⅱ)的吸附量随着温度和初始浓度的增加而增加,适宜的pH为4。动力学和热力学研究表明,吸附Fe(Ⅱ)过程符合准二级反应动力学模型,吸附等温线符合Langmuir模型,吸附过程活化能为45.60kJ/mol,为化学吸附。Fe3O4@PGMA-Arg经5次再生后,对亚铁离子仍保持较高的脱除率。

关键词: 亚铁离子, 磁性, 吸附, 聚合物接枝

Abstract:

Magnetic adsorbents were synthesized to remove the ferrous ion form oilfield. The hydrophilic Fe3O4 nanoparticles were prepared by solvothermal method and Fe3O4@PDA was obtained by coating with dopamine hydrochloride. Glycidyl methacrylate was also grafted onto Fe3O4@PDA to obtain Fe3O4@PGMA. Fe3O4@PGMA-Arg was obtained by modifying Fe3O4@PGMA with arginine. Infrared spectrometer, X-ray photoelectron spectrometer, X-ray diffractometer and vibrating sample magnetometer were used to characterize these adsorbents. Fe3O4@PGMA-Arg had primary amine, imine double bond, hydroxyl and carboxyl functional groups. The N on the primary amine group and imine double bond could form coordination bonds with Fe(Ⅱ), and the O on the hydroxyl and carboxyl groups could also form coordination bond with Fe(Ⅱ), which made Fe3O4@PGMA-Arg could adsorb Fe(Ⅱ). These synthesized adsorbents maintained the inverse spinel structure of Fe3O4 and the magnetic response properties were good. The static adsorption experiment was carried out to explore the influencing factors of adsorption conditions on Fe(Ⅱ) adsorption by Fe3O4@PGMA-Arg. The results indicated that the adsorption capacity of Fe(Ⅱ) increased with the increase of temperature and initial concentration, and the suitable pH was 4. Kinetic and thermodynamic studies showed that the process of Fe(Ⅱ) adsorption conformed to the quasi-second-order reaction kinetic model. The adsorption isotherms conformed to the Langmuir model. The activation energy was 45.60kJ/mol, which was chemical adsorption. Fe3O4@PGMA-Arg maintained a high removal rate of ferrous ions after 5 times regeneration.

Key words: ferrous ion, magnetic, adsorption, polymer grafting

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