具有尿素功能性覆盖孔的互穿坚固金属有机框架，用于抗生素和含氧阴离子的选择性和超灵敏检测,Crystal Growth & Design

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具有尿素功能性覆盖孔的互穿坚固金属有机框架，用于抗生素和含氧阴离子的选择性和超灵敏检测
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2023-10-09 , DOI: 10.1021/acs.cgd.3c00979
Partha Pratim Mondal ₁ , Devaraj Muthukumar ₂ , Shifna K. P. Fathima ₁ , Renjith S. Pillai _{2,

3} , Subhadip Neogi _{1,

4}

Affiliation

结合结构多样性和在多孔通道内故意植入特定任务位点的优点，金属有机框架（MOF）不仅可以通过敏锐检测有机和无机污染物来确保环境修复，还可以合理化结构与性能的协同作用，以设计出具有先进性能的更智能材料。在此，我们报告了一种基于混合配体方法的脲官能团接枝Co(II)-框架(UMOF)。含有3重互穿和[Co ₂ (COO) ₄ N ₄ ]构建单元的结构表现出高稳定性和游离羧酰胺位点装饰的微孔通道。高密度氢键供体基团加上富含 π 电子的芳香配体的同化有利于 UMOF 通过显着的猝灭作用作为三种有毒抗生素的选择性荧光传感器，包括呋喃西林 (NFT, K sv : 3.2 _× 10 ⁴ M ^–1 )、呋喃妥因 (NFZ, K _sv : 3.0 × 10 ⁴ M ^–1 ) 和磺胺二甲嗪 (SMZ, K _sv : 3.3 × 10 ⁴ M ^–1 ) 检测限为 ppb 级 (LOD, NFT: 110.42, NFZ ：97.89，SMZ：78.77）。发光猝灭的机制见解得到了密度泛函理论计算的支持，除了验证分析物-连接体非共价相互作用之外，密度泛函理论计算还通过描绘单个有机毒素的脲基固定连接体能级的变化来支持电子转移路线。该框架进一步展示了对具有极低LOD（Cr ₂ O ₇^2–：73.35；CrO ₄^2–：189；和MnO ₄^–：49.96 ppb）的含氧阴离子的高度辨别性关闭检测。值得注意的是，除了快速响应检测之外，UMOF 对所有有机和无机分析物的多循环传感的可重复使用性，其中不同大小的能量转移贡献明确地验证了关闭事件。

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Interpenetrated Robust Metal–Organic Framework with Urea-Functionality-Decked Pores for Selective and Ultrasensitive Detection of Antibiotics and Oxo-anions

Conjoining the benefits of structural diversity and deliberate implantation of task-specific sites inside the porous channels, metal–organic frameworks (MOFs) not only ensure environmental remediation via acute detection of organic as well as inorganic pollutants but also rationalize structure–performance synergies to devise smarter materials with advanced performances. Herein, we report a urea-functionality-grafted Co(II)-framework (UMOF) based on a mixed ligand approach. The 3-fold interpenetrated and [Co₂(COO)₄N₄] building unit-containing structure exhibits high stability and free-carboxamide-site-decorated microporous channels. Assimilation of high-density hydrogen-bond donor groups plus the π-electron-rich aromatic ligand benefits the UMOF acting as a selective fluoro-sensor for three noxious antibiotics through remarkable quenching, including nitrofurazone (NFT, K_sv: 3.2 × 10⁴ M^–1), nitrofurantoin (NFZ, K_sv: 3.0 × 10⁴ M^–1), and sulfamethazine (SMZ, K_sv: 3.3 × 10⁴ M^–1) with ppb level limits of detection (LODs, NFT: 110.42, NFZ: 97.89, and SMZ: 78.77). The mechanistic insight of luminescence quenching is supported from density functional theory calculations, which endorse the electron-transfer route via portraying variation in the energy levels of the urea group-affixed linker by individual organo-toxins, besides verifying analyte–linker noncovalent interactions. The framework further demonstrates highly discriminative turn-off detection of oxo-anions with extreme low LODs (Cr₂O₇^2–: 73.35; CrO₄^2–: 189; and MnO₄^–: 49.96 ppb). Of note is the reusability of the UMOF toward multicyclic sensing of all the organic and inorganic analytes besides their fast-responsive detection, where variable magnitudes of energy-transfer contributions unequivocally authenticate the turn-off event.

更新日期：2023-10-09

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