Porous Aluminum-Based Metal–Organic Framework–Aminoclay\nNanocomposite: Sustainable Synthesis and Ultrahigh Sorption of Cephalosporin\nAntibiotics

Javad Imanipoor (9634976), Mohsen Mohammadi (5593175)
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Abstract

A novel\nsorbent was synthesized based on MIL-53­(Al) MOF grown over\nan aminoclay (AC) platform, called MIL-53­(Al)@AC nanocomposite, via\na green and facile hydrothermal method. The nanocomposite was characterized\nusing FT-IR, PXRD, BET, TEM, FESEM, EDS, XPS, TGA, DLS, and zeta potential\nanalyses. BET analysis represented the porous nature and great surface\narea of MIL-53­(Al)@AC. The high crystalline structure for the synthesized\nnanocomposite was verified using the PXRD pattern. FESEM, EDS, TEM,\nand XPS analysis proved the successful decoration of MIL-53­(Al) over\nthe AC platform. Cephalosporin antibiotics cefixime (CFX) and cephalexin\n(CPX), which are often present in wastewaters, were utilized to examine\nthe sorption capacity of the nanocomposite. The significant influential\nfactors such as pH, temperature, sorbent amount, ionic strength, and\nimpurity were discussed. At an initial pH of 7.0 ± 0.1, the highest\nsorption capacities of CFX and CPX on MIL-53­(Al)@AC were 784.14 and\n747.91 mg g<sup>–1</sup> (<i>T</i> = 298 K, and sorbent\namount = 0.1 g L<sup>–1</sup>), which were 1.43 and 1.47 times\ngreater compared to that of MIL-53­(Al), respectively. The evaluation\nof experimental results was implemented through the Langmuir and Freundlich\nisotherm equations. The isothermal data were described nobly by the\nFreundlich isotherm, which confirmed multilayer adsorption on heterogeneous\nsurfaces (<i>R</i><sup>2</sup> > 0.970). A kinetic study\nindicated that the nanocomposite could adsorb the majority of cephalosporin\nantibiotics within 30 min. In addition, the experimental data were\nevaluated via pseudo-first-order, pseudo-second-order, and intraparticle\ndiffusion models. The results indicated that the pseudo-second-order\nequation agreed more closely with the kinetic data (<i>R</i><sup>2</sup> > 0.990). Furthermore, the processes of adsorption\nwere\nexothermic and spontaneous. The electrostatic attraction, hydrophobic\ninteraction, π–π electron donor–acceptor\neffect, H-bond, and π–π stacking constituted the\nmain sorption mechanisms. Finally, MIL-53­(Al)@AC presented an excellent\nregeneration performance. Thus, the results revealed the potential\napplication of the MIL-53­(Al)@AC nanocomposite for water remediation.
多孔铝基金属-有机骨架-氨基clay纳米复合材料:头孢菌素纳米抗生素的可持续合成和超高吸附
以在\nan氨基clay (AC)平台上生长的MIL-53 - (Al) MOF为基础,通过\na绿色水热法合成了新型的\nsorbent纳米复合材料MIL-53 - (Al)@AC。对纳米复合材料进行了表征\nusing FT-IR, PXRD, BET, TEM, FESEM, EDS, XPS, TGA, DLS和zeta电位\nanalyses。BET分析表征了MIL-53 - (Al)@AC的多孔性和巨大的表面\narea。通过PXRD谱图验证了合成的\nnanocomposite具有较高的晶体结构。FESEM, EDS, TEM, \nand XPS分析证明MIL-53 - (Al)在\nthe AC平台上修饰成功。利用常存在于废水中的头孢菌素类抗生素头孢克肟(CFX)和头孢氨苄\n (CPX)来检测纳米复合材料\nthe的吸附能力。讨论了pH、温度、吸附剂用量、离子强度和\nimpurity等因素对吸附性能的显著影响\nfactors。在初始pH为7.0±0.1时,CFX和CPX对MIL-53 - (Al)@AC的最高\nsorption容量分别为784.14和\n 747.91 mg g&lt;sup&gt; - 1&lt;/sup&gt; (&lt;i&gt;T&lt;/i&gt; = 298 K,吸附剂\namount = 0.1 g L&lt;sup&gt; - 1&lt;/sup&gt;),分别是MIL-53 - (Al)的1.43和1.47倍\ngreater。评价\nof实验结果通过Langmuir和Freundlich \nisotherm方程实现。等温数据用\nFreundlich等温线描述,证实了多相吸附\nsurfaces (&lt;i&gt;R&lt;/i&gt;&lt;sup&gt;2&lt;/sup&gt; &gt; 0.970)上的多层吸附。动力学研究\nindicated表明纳米复合材料可以在30分钟内吸附大部分头孢菌素\nantibiotics。此外,实验数据通过伪一阶、伪二阶和粒子内\ndiffusion模型\nevaluated。结果表明,伪二阶方程\nequation与动力学数据更为吻合(&lt;i&gt;R&lt;/i&gt;&lt;sup&gt;2&lt;/sup&gt; &gt; 0.990)。此外,吸附过程\nwere\nexothermic和自发。静电吸引、疏水\ninteraction、π -π电子供体-受体\neffect、氢键和π -π堆积构成了\nmain吸附机制。最后,MIL-53 - (Al)@AC表现出优异的\nregeneration性能。因此,研究结果揭示了MIL-53 - (Al)@AC纳米复合材料在水修复方面的潜力\napplication。
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