Facile construction of a stable core-shell spherically magnetic polyimide covalent organic framework for efficient extraction of phenylurea herbicides

IF 6.1 1区 化学 Q1 CHEMISTRY, ANALYTICAL
Xiaoxia Zhang , Jinchang Liu , Han Zhang , Qinming Zhang , Jiwei Shen , Yinmao Wei , Chaozhan Wang
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Abstract

Efficient enrichment is crucial for the highly sensitive monitoring of phenylurea herbicides (PUHs) in various environmental waters. In this work, a stable core-shell spherically magnetic polyimide covalent organic framework (COF) was synthesized via a simple template-mediated precipitation polymerization method under mild conditions using tri(4-aminophenyl)amine (TAPA) and 3,3′,4,4′-biphenyltetracarboxylic dianhydride (BPDA) as the building units (denoted as Fe3O4@TAPA-BPDA). The Fe3O4@TAPA-BPDA exhibits remarkable adsorption performance for PUHs with an optimized adsorption time of only 10 min. The adsorption of PUHs by Fe3O4@TAPA-BPDA followed the pseudo-second-order kinetic model and the Langmuir model. Furthermore, hydrogen bonding, halogen bonding, hydrophobic interaction, electro donor-acceptor interaction and π-π interactions are identified as the dominant mechanisms contributing to excellent adsorption performance. It was demonstrated that halogen bonds play an important role in the adsorption of substances containing chlorine atoms. The Fe3O4@TAPA-BPDA is easy to operate and highly regenerable. A simple magnetic solid-phase extraction (MSPE) method based on the Fe3O4@TAPA-BPDA was then developed for the rapid extraction of five PUHs in real samples, coupled with high-performance liquid chromatography (HPLC) determination. The analytical method developed has a linear range of 0.5–50 ng/mL, and the limit of detection (LOD) ranges from 0.06 to 0.10 ng/mL. The method exhibits good accuracy with recoveries ranged from 74.5 % to 111.4 %. The analytical method was successfully applied to the highly sensitive detection of PUHs in environmental water samples, which highlighting the potential application of the Fe3O4@TAPA-BPDA in the sample pretreatment.

Abstract Image

简便构建稳定的核壳球形磁性聚酰亚胺共价有机框架,用于高效萃取苯基脲类除草剂
高效富集对于高灵敏度监测各种环境水体中的苯基脲类除草剂(PUHs)至关重要。本研究以三(4-氨基苯基)胺(TAPA)和 3,3′,4,4′-联苯四羧酸二酐(BPDA)为构建单元,通过简单的模板介导沉淀聚合法,在温和条件下合成了稳定的核壳球形磁性聚酰亚胺共价有机框架(COF)(简称 Fe3O4@TAPA-BPDA)。Fe3O4@TAPA-BPDA对聚氨酯具有显著的吸附性能,最佳吸附时间仅为10分钟。Fe3O4@TAPA-BPDA 对 PUHs 的吸附遵循伪秒阶动力学模型和 Langmuir 模型。此外,氢键、卤素键、疏水作用、电供体-受体作用和 π-π 相互作用被认为是促成优异吸附性能的主要机制。研究表明,卤素键在吸附含氯原子的物质时发挥了重要作用。Fe3O4@TAPA-BPDA 操作简便,可再生性强。基于Fe3O4@TAPA-BPDA开发了一种简单的磁性固相萃取(MSPE)方法,用于快速萃取实际样品中的五种聚氨酯,并结合高效液相色谱法(HPLC)进行测定。所建立的分析方法的线性范围为0.5-50 ng/mL,检出限(LOD)为0.06-0.10 ng/mL。该方法准确度高,回收率在 74.5 % 至 111.4 % 之间。该分析方法成功地应用于环境水样中PUHs的高灵敏度检测,凸显了Fe3O4@TAPA-BPDA在样品前处理中的应用潜力。
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来源期刊
Talanta
Talanta 化学-分析化学
CiteScore
12.30
自引率
4.90%
发文量
861
审稿时长
29 days
期刊介绍: Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.
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麦克林
3,3′,4,4′-Biphenyltetracarboxylic dianhydride (BPDA)
阿拉丁
linuron
阿拉丁
isoproturon
阿拉丁
monolinuron
阿拉丁
chlortoluron
阿拉丁
monuron
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