Fe3O4@PANI-PG硼吸附剂的制备、表征及其吸附性能

Preparation, characterization, adsorption performance and mechanism of Fe3O4@PANI-PG boron adsorbent

  • 摘要: 基于磁性分离原理,设计并制备了一种磁性多元醇硼吸附剂,有效解决了传统吸附剂与水相分离困难问题。首先,以苯胺为单体,采用原位聚合反应在自制的磁性Fe3O4纳米颗粒表面包裹了一层聚苯胺(PANI),然后通过缩水甘油与聚苯胺末端活性胺基开环反应,制备了一种核壳结构的多元醇硼吸附剂:丙二醇改性聚苯胺复合四氧化三铁(Fe3O4@PANI-PG);采用SEM、TEM、EDS、XRD、XPS和FTIR等表征方法对材料的微观形貌、结构、组成及官能团进行了表征。其次,通过单因素实验考察了吸附时间、硼酸初始浓度、pH等因素对其硼吸附性能的影响,在此基础上采用响应面法优化得到了吸附最佳条件:时间t=10 h,初始浓度C0=1309 mg/L,pH=9.93和相应最佳吸附量Qe=0.1181 mmol/g。此外,通过吸附动力学及吸附等温式拟合,研究发现该吸附剂对硼吸附过程符合准二级吸附动力学和Langmuir等温吸附模型。最后对其吸附机制进行探究,研究发现:该吸附剂末端邻位羟基与水相中的B(OH)4发生络合反应形成了稳定的五元环螯合物。

     

    Abstract: In this paper, the traditional difficult problem of separation between adsorbent and water phase was effectively solved by a kind of magnetic polyols boron adsorbent, which were designed and prepared based on the principle of magnetic separation. Firstly, the polyaniline compound Fe3O4 (Fe3O4@PANI) composites with core-shell structure were prepared by the in-situ polymerization reaction at the presence of aniline and Fe3O4 nanoparticles, which were prepared by ourselves. Then propylene glycol modified polyaniline compound Fe3O4 (Fe3O4@PANI-PG) boron adsorbent was successfully prepared by the ring-opening reaction between polyaniline terminal active —NH2 and glycidyl. After that, the micro-structure, composition and functional groups were analyzed by the SEM, TEM, EDS, XRD, XPS and FTIR, respectively. The adsorption time, initial concentration of boric acid, pH and other factors of Fe3O4@PANI-PG were investigated by the single factor experiment. On this basis, the optimal adsorption conditions (time t=10 h, initial concentration C0=1309 mg/L, pH=9.93) were obtained by response surface method, and the corresponding optimal adsorption capacity up to Qe=0.1181 mmol/g. In addition, it was found that the adsorption process was in accordance with the quasi-second-order adsorption kinetics and Langmuir adsorption isotherm based on the adsorption kinetics and adsorption isotherm fitting. Finally, the adsorption mechanism of Fe3O4@PANI-PG was explored and the results indicating the complex reaction between the hydroxyl group at the end of the adsorbent and B(OH)4 in the aqueous phase formed a stable five-membered ring chelate.

     

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