Enhancement tetracycline adsorption by amino/nitro-functionalized MIL-126(Fe) adsorbent based on the ligand installation method

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-06-21 DOI:10.1016/j.micromeso.2024.113228

Mengting Xu , Zeyu Chen , Yeyang Ni , Wanyong Yang , Xihua Xu , Qing Liu , Zhaoyang Fei , Mifen Cui , Xu Qiao

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Abstract

MIL-126(Fe) shows great potential for aqueous phase drug adsorption due to its permanent porosity and easy modification. Herein, we utilized the ligand installation method to introduce two ligands, 2-amino terephthalic acid (NH₂-BDC) and 2-nitro terephthalic acid (NO₂-BDC), into MIL-126(Fe) to prepare MIL-126(Fe)-NH₂ and MIL-126(Fe)-NO₂, respectively. Various analytical tools were used to confirm the successful installation of the 1, 4-phthalic acid (BDC) series of ligands, as well as the successful introduction of amino (-NH₂) and nitro (-NO₂) groups. The presence of both -NH₂ and -NO₂ groups improved the adsorption of TC by the adsorbent material, with -NH₂ groups having a stronger influence on the enhancement. The experimental results indicated that MIL-126(Fe)-NH₂ had the highest adsorption performance at the optimal pH of 7, achieving a static adsorption capacity of 326.5 mg/g, which was about twice the adsorption capacity of the original MIL-126(Fe). X-ray photoelectron spectroscopy (XPS) determined that the adsorption of TC by MIL-126(Fe)-NH₂ relies mainly on π-π interaction and Fe-N coordination bonds. Furthermore, the higher adsorption capacity of MIL-126(Fe)-NH₂ can be attributed to the O-H⋯N hydrogen bonds interaction between -NH₂ and the phenolic hydroxyl group (Ph-OH) in the TC molecule.

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基于配体安装方法的氨基/硝基功能化 MIL-126(Fe)吸附剂对四环素的吸附增强作用

MIL-126(Fe)因其永久多孔性和易于改性的特点，在水相药物吸附方面具有巨大潜力。在此，我们利用配体安装方法将 2-氨基对苯二甲酸（NH2-BDC）和 2-硝基对苯二甲酸（NO2-BDC）两种配体引入 MIL-126(Fe)，分别制备出 MIL-126(Fe)-NH2 和 MIL-126(Fe)-NO2。使用各种分析工具确认了 1，4-邻苯二甲酸（BDC）系列配体的成功安装，以及氨基（-NH2）和硝基（-NO2）基团的成功引入。-NH2 和 -NO2 基团的存在都提高了吸附材料对 TC 的吸附能力，其中 -NH2 基团对吸附能力的提高影响更大。实验结果表明，在最佳 pH 值为 7 时，MIL-126（Fe）-NH2 的吸附性能最高，静态吸附容量达到 326.5 mg/g，约为原 MIL-126（Fe）吸附容量的两倍。X 射线光电子能谱（XPS）测定，MIL-126（Fe）-NH2 对 TC 的吸附主要依赖于 π-π 相互作用和 Fe-N 配位键。此外，MIL-126(Fe)-NH2 较高的吸附能力可归因于 -NH2 与 TC 分子中的酚羟基（Ph-OH）之间的 O-H⋯N 氢键相互作用。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.