Application of the flexible polyethylene polyamine-based covalent organic frameworks for fluorescence sensing nitrophenols and iodide ions

IF 4 2区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Molecular Structure Pub Date : 2024-11-09 DOI:10.1016/j.molstruc.2024.140695

Ya-Chen Wang, Feng Zhu, Jun Pan, Tong-Mou Geng

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引用次数: 0

Abstract

Recently, flexible covalent organic frameworks (COFs) prepared with nitrogen-rich building units have become targets for selective detection of pollutants to serve a clean environment. To meet the requirements of the practical applications, a series of novel flexible covalent organic frameworks containing polyethylene polyamine units (the flexible PEPA-based COFs, remember as TEDA, TDETA, TTETA, TTEPA, and TPEHA) were designed and developed to create fluorescence sensors. The flexible PEPA-based COFs were found to be excellently fluorescent properties in presence of some solvents under irradiation with UV light and can sense some nitrophenols with good sensitivity for DNP, o-NP, or TNP by fluorescence quenching with high S-V constants (K_SV) of 5.01 × 10⁴, 6.92 × 10³, 7.42 × 10⁴, 7.37 × 10³, and 1.59 × 10⁴ L mol⁻¹, respectively. Theoretical calculations and experimental studies show that the fluorescence quenching in the presence of nitrophenols is put down to photoinduced electron transfer, energy resonance transfer, and the difference between nitrophenols binding sites to the flexible PEPA-based COFs. In addition, TEDA, TDETA, TTETA, TTEPA, and TPEHA can fluorescently sense iodide ions with high K_SV of 2.28 × 10⁴, 1.09 × 10⁴, 6.88 × 10³, 8.81 × 10³, and 1.82 × 10⁴ L mol⁻¹, which are the most sensitive among POP materials.

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基于柔性聚乙烯多胺的共价有机框架在荧光传感硝基苯酚和碘离子中的应用

近年来，利用富氮结构单元制备的柔性共价有机框架（COFs）已成为选择性检测污染物的目标，为清洁环境服务。为了满足实际应用的要求，我们设计并开发了一系列含有聚乙烯多胺单元的新型柔性共价有机框架（柔性珠光体基 COFs，即 TEDA、TDETA、TTETA、TTEPA 和 TPEHA），用于制造荧光传感器。研究发现，在紫外光照射下，柔性聚对苯二甲酸乙二酯基 COFs 在某些溶剂存在下具有优异的荧光特性，并能通过荧光淬灭对一些硝基苯酚具有良好的灵敏度，如 DNP、o-NP 或 TNP，其 S-V 常数（KSV）分别为 5.01 × 104、6.92 × 103、7.42 × 104、7.37 × 103 和 1.59 × 104 L mol-1。理论计算和实验研究表明，硝基苯酚存在时的荧光淬灭归因于光诱导电子转移、能量共振转移以及硝基苯酚与柔性珠光粉基 COF 结合位点之间的差异。此外，TEDA、TDETA、TTETA、TTEPA 和 TPEHA 可荧光感应碘离子，其 KSV 分别高达 2.28 × 104、1.09 × 104、6.88 × 103、8.81 × 103 和 1.82 × 104 L mol-1，是持久性有机污染物材料中灵敏度最高的。

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来源期刊

Journal of Molecular Structure 化学-物理化学

CiteScore

7.10

自引率

15.80%

发文量

2384

审稿时长

45 days

期刊介绍： The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.