Facultad de Posgrado, Universidad Técnica de Manabí, S/N, Avenida Urbina y Che Guevara, Portoviejo, 130104, Ecuador; Departamento de Química Orgánica, Universidad de Córdoba, Edificio Marie Curie (C-3), Campus de Rabanales, Ctra. Nnal. IV-A, Km 396, E14014, Córdoba, Spain.
Departamento de Química Orgánica, Universidad de Córdoba, Edificio Marie Curie (C-3), Campus de Rabanales, Ctra. Nnal. IV-A, Km 396, E14014, Córdoba, Spain; Laboratorio de Análisis Químicos y Biotecnológicos, Instituto de Investigación, Universidad Técnica de Manabí, S/N, Avenida Urbina y Che Guevara, Portoviejo, 130104, Ecuador.
Environ Res. 2024 Jan 1;240(Pt 1):117492. doi: 10.1016/j.envres.2023.117492. Epub 2023 Nov 8.
In this work, a hybrid was synthesized by hydrothermal treatment, metal-organic framework functionalized with hydrochar (MIL-53(Al)@HC) for the adsorption of two organic molecules Ibuprofen sodium salt and Metsulfuron-methyl, in binary system. The hybrid is composed of 71 wt% biomass and 29 wt% MOF. TGA, BET, FTIR, XRD and XPS characterization techniques were used to verify the hybridization of MIL-53(Al)@HC. The MIL-53(Al)@HC hybrid showed in situ MIL-53(Al) crystal growth capability. Batch adsorption experiments were carried out to study the effect of pH, adsorbent dosage, adsorbate concentration, contact time and temperature effect. The results obtained under extreme conditions demonstrate that MIL-53(Al)@HC is an adsorbent capable of removing >98% of IBU and MTM in mixture at a concentration of 0.3 mM (68 ppm IBU and 115 ppm MTM). The pseudo-second order model adequately described the adsorption kinetics and equilibrium using the Sips and Freundlich models. The physico-statistical microscopic model (2-layer) corroborated the hypothesis of a multilayer adsorption proposed by the macroscopic Freundlich model. In the competition study between IBU and MTM, both antagonistic and synergistic effects were observed. In the thermodynamic study, positive values of (ΔH°) indicate that adsorption is endothermic in nature and that the dominant mechanism is physisorption. A mechanism of adsorption by hydrogen bridging and non-covalent π*-π adsorbate-adsorbate and adsorbate-adsorbate-adsorbate interactions was proposed. The desorption study shows that in 5 washing cycles MIL-53(Al)@HC is a recoverable material.
在这项工作中，通过水热处理合成了一种杂化物，该杂化物用水热炭功能化的金属有机骨架（MIL-53(Al)@HC）用于在二元体系中吸附两种有机分子布洛芬钠盐和甲磺隆甲酯。该杂化物由 71wt%生物质和 29wt% MOF 组成。使用 TGA、BET、FTIR、XRD 和 XPS 表征技术验证了 MIL-53(Al)@HC 的杂化。MIL-53(Al)@HC 杂化物表现出原位 MIL-53(Al)晶体生长能力。进行了批量吸附实验，以研究 pH、吸附剂用量、吸附物浓度、接触时间和温度效应的影响。在极端条件下获得的结果表明，MIL-53(Al)@HC 是一种能够在 0.3mM 浓度下（68ppm IBU 和 115ppm MTM）去除混合物中 >98%IBU 和 MTM 的吸附剂。准二级模型使用 Sips 和 Freundlich 模型充分描述了吸附动力学和平衡。物理统计微观模型（2 层）证实了宏观 Freundlich 模型提出的多层吸附假设。在 IBU 和 MTM 之间的竞争研究中，观察到了拮抗和协同作用。在热力学研究中，（ΔH°）的正值表明吸附本质上是吸热的，并且主要机制是物理吸附。提出了一种通过氢键和非共价π*-π吸附物-吸附物和吸附物-吸附物-吸附物相互作用进行吸附的机制。解吸研究表明，在 5 次洗涤循环中，MIL-53(Al)@HC 是一种可回收材料。
