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Adsorption of pharmaceuticals and personal care products by deep eutectic solvents-regulated magnetic metal-organic framework adsorbents: performance and mechanism
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-03-20 , DOI: 10.1016/j.cej.2020.124808
Xiaoxiao Wei , Yuzhi Wang , Jing Chen , Fangting Xu , Ziwei Liu , Xiyan He , Heqiong Li , Yigang Zhou

The ecological and human health threats brought by emerging pollutants are increasingly serious. Development of efficient removal methods is urgent. Herein, seven deep eutectic solvents (DESs) composed by quaternary ammonium salts and lactic acid or glycolic acid were synthesized and used to regulate magnetic (Fe3O4) metal organic framework (MUiO-66-NH2) composites. The obtained nanoparticles (named as DES-MUiO-66-NH2) were used as adsorbents to adsorb pharmaceuticals and personal care products (PPCPs). Langmuir isotherm model and pseudo-second-order kinetics model were suitable to analyze the adsorption process of DES-MUiO-66-NH2 to PPCPs, indicated that the adsorption of PPCPs was chemisorption on homogeneous surface of DES-MUiO-66-NH2 adsorbents. Under the optimal conditions, the adsorption capacity of DES-MUiO-66-NH2 toward ofloxacin and mefenamic acid reached up to 97.60 and 79.22 mg/g, respectively. Mechanism exploration indicated that DES-MUiO-66-NH2 selectively adsorbed PPCPs through electrostatic interaction, chelation, π-π stacking, hydrophobic interactions and hydrogen bonding. Density functional theory proved the chelation through theoretical calculation. Selective experiments manifested that the structures of DESs directly determined the specificity of DES-MUiO-66-NH2 for different PPCPs, and the investigation of structure-activity relationship provided new ideas for designing efficient tailor-made adsorbents for PPCPs. The proposed PPCPs removal approach focused on the guiding role of DESs in selective adsorption. And this green DESs regulation idea provided more options for the synthesis of high-efficiency and functional adsorbents for emerging pollutants.



中文翻译:

深共熔溶剂调节的磁性金属-有机骨架吸附剂对药物和个人护理产品的吸附:性能和机理

新兴污染物带来的生态和人类健康威胁日益严重。迫切需要开发有效的清除方法。在此,合成了由季铵盐和乳酸或乙醇酸组成的七种深共晶溶剂(DES),并用于调节磁性(Fe 3 O 4)金属有机骨架(MUiO-66-NH 2)复合材料。所获得的纳米颗粒(命名为DES-MUiO-66-NH 2)用作吸附剂以吸附药物和个人护理产品(PPCP)。Langmuir等温线模型和拟二级动力学模型适用于分析DES-MUiO-66-NH 2的吸附过程对PPCPs的吸附表明PPPPs的吸附是在DES-MUiO-66-NH 2吸附剂的均相表面上的化学吸附。在最佳条件下,DES-MUiO-66-NH 2对氧氟沙星和甲芬那酸的吸附量分别达到97.60和79.22 mg / g。机理探索表明,DES-MUiO-66-NH 2通过静电相互作用,螯合,π-π堆积,疏水相互作用和氢键选择性吸附PPCP 。密度泛函理论通过理论计算证明了螯合。选择性实验表明,DES的结构直接决定了DES-MUiO-66-NH 2的特异性对于不同的PPCP,结构-活性关系的研究为设计高效的PPCP量身定制的吸附剂提供了新思路。提出的PPCPs去除方法侧重于DES在选择性吸附中的指导作用。这种绿色的DESs监管理念为合成新兴污染物的高效和功能性吸附剂提供了更多选择。

更新日期:2020-03-21
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