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New insights into the selective adsorption mechanism of cationic and anionic dyes using MIL-101(Fe) metal-organic framework: Modeling and interpretation of physicochemical parameters
Journal of Contaminant Hydrology ( IF 3.6 ) Pub Date : 2022-02-14 , DOI: 10.1016/j.jconhyd.2022.103977
Mohamed Shakly 1 , Laila Saad 2 , Moaaz K Seliem 3 , Adrián Bonilla-Petriciolet 4 , Nabila Shehata 1
Affiliation  

In the current study, iron-based metal organic framework (MOF) MIL-101(Fe) was successfully prepared via a facile solvothermal method. The as–synthesized MIL-101(Fe) was characterized by XRD, FE-SEM, FTIR, TGA and zeta potential techniques, and then employed as an adsorbent for methyl orange (MO) and methylene blue (MB) dyes. The adsorbed quantities of MO (1067 to 831 mg/g) were higher than those of MB (402 to 353 mg/g) indicating the high selectivity of MIL-101(Fe) towards the anionic dye at all temperatures (20–60 °C). Adsorption processes of MO and MB followed the pseudo-second order kinetics and the Langmuir equilibrium model. The interaction mechanism at a molecular level was analyzed and deeply interpreted via the advanced multilayer adsorption model. Steric parameters indicated that MO molecular aggregation (n) was 0.95–1.33 thus signifying the presence of multi–docking and multi–interactions mechanisms. The aggregated number of MB was superior to unity (i.e., n = 1.17–1.78) suggesting a vertical adsorption position and a multi-interactions mechanism at all operating temperatures. The density of MIL-101(Fe) active sites (DM = 77.33–52.38 mg/g for MB and 149.91–107.07 for MO) and the total adsorbed dye layers (Nt = 3.12–2.49 for MB and 5.36–3.67 for MO) resulted in improving the adsorption capacities of MO dye. The adsorption energies ranged from 8.89 to 33.73 kJ/mol and they displayed that MO and MB uptake processes were exothermic controlled by physical interactions at all temperatures. Regeneration results indicated that this adsorbent can be reutilized without a significant loss in its removal efficiency after five adsorption-desorption cycles. Overall, the adsorption capacity, chemical stability, and regeneration performance of MIL-101(Fe) support its application as a very promising adsorbent for the removal of organic hazardous pollutants from water.



中文翻译:

使用 MIL-101(Fe) 金属有机框架对阳离子和阴离子染料的选择性吸附机制的新见解:物理化学参数的建模和解释

在目前的研究中,铁基金属有机骨架 (MOF) MIL-101(Fe) 通过简便的溶剂热法成功制备。合成后的 MIL-101(Fe) 通过 XRD、FE-SEM、FTIR、 TGA和 zeta 电位技术表征,然后用作甲基橙 (MO) 和亚甲蓝 (MB) 染料的吸附剂。MO 的吸附量(1067 至 831 mg/g)高于 MB 的吸附量(402 至 353 mg/g),表明高MIL-101(Fe) 在所有温度 (20–60 °C) 下对阴离子染料的选择性。MO和MB的吸附过程遵循准二级动力学和Langmuir平衡模型。通过先进的多层吸附模型对分子水平的相互作用机理进行了深入的分析和解释。立体参数表明MO分子聚集( n)为0.95-1.33,因此表明存在多对接和多相互作用机制。MB 的总数量优于统一(即n  = 1.17-1.78),表明在所有操作温度下都有垂直吸附位置和多相互作用机制。MIL-101(Fe) 活性位点的密度 ( D M =MB 为 77.33-52.38 mg/g,MO 为 149.91-107.07)和总吸附染料层( MB 为N t  = 3.12-2.49,MO 为 5.36-3.67)导致 MO 染料的吸附能力提高。吸附能范围为 8.89 至 33.73 kJ/mol,它们表明 MO 和 MB 的吸收过程在所有温度下都是由物理相互作用控制的放热过程。再生结果表明,该吸附剂在经过五次吸附-解吸循环后可以重复利用,而其去除效率不会显着降低。总体而言,MIL-101(Fe) 的吸附能力、化学稳定性和再生性能支持其作为一种非常有前途的吸附剂,用于去除水中的有机有害污染物。

更新日期:2022-02-16
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