A novel pH-responsive aptamer-molecularly imprinted hydrogel for efficient identification and separation of ampicillin in complex matrices.

IF 6.1 1区 化学 Q1 CHEMISTRY, ANALYTICAL
Talanta Pub Date : 2025-12-01 Epub Date: 2025-06-10 DOI:10.1016/j.talanta.2025.128425
Liyu Qiu, Xixiang Yang, Nan Zhao, Anqi Luo, Li Wang, Xiaogang Hu
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引用次数: 0

Abstract

Hybrids of molecular imprinting-aptamers have been used for environmental analysis; however, the weak selectivity and stability inhibited their applications in complex matrices. In this paper, the nano-scale pH-responsive aptamer-molecularly imprinted interpenetrating hydrogels (Fe3O4@Apt-MIH) were prepared in one step by the modified sol-gel method based on the preparation principle of interpenetrating network hydrogels, with Fe3O4 as the carrier, aminopropyltriethoxysilane and methyltrimethoxysilane as functional monomers, polyethyleneimine (PEI) as the pH-responsive components, and tetraethoxysilane (TEOS) and glutaraldehyde (GA) as dual cross-linking agents. After optimizing the polymerization and extraction conditions, the pH response performance, extraction capacity and reusability of the material with highly magnetism were investigated, which could achieve magnetic separation within 5 s. The SiO2 coating hydrolyzed by TEOS provided a rigid backbone for interpenetrating hydrogels, which could improve the acid resistance of PEI by adjusting the isoelectric point of Fe3O4@Apt-MIH and assist in target identification. Selectivity research showed that aptamers and functional monomers have a highly effective synergistic recognition effect on ampicillin, with the imprinting factor of 6.90 and the synergistic recognition factor of 1.48. This solid-phase microextraction material coupled to high-performance liquid chromatography with the linear range of 10-1000 μg/L and the detection limit of 7.67 μg/L enabled the selective separation and detection of ampicillin in milk and honey, with minimal sample matrix interference and recovery between 95.2 and 102 %.

一种新型ph响应适体-分子印迹水凝胶,用于复杂基质中氨苄西林的有效鉴定和分离。
分子印迹适体杂交已被用于环境分析;然而,选择性和稳定性较弱,限制了它们在复杂矩阵中的应用。本文基于互穿网络水凝胶的制备原理,以Fe3O4为载体,氨基丙基三乙氧基硅烷和甲基三甲氧基硅烷为功能单体,聚乙烯亚胺(PEI)为ph响应组分,四乙氧基硅烷(TEOS)和戊二醛(GA)为双交联剂,采用改进的溶胶-凝胶法一步制备了纳米级ph响应分子印迹互穿水凝胶(Fe3O4@Apt-MIH)。通过优化聚合和提取条件,考察了高磁性材料的pH响应性能、提取能力和可重复使用性,在5 s内实现了磁性分离。TEOS水解的SiO2涂层为互穿水凝胶提供了刚性骨架,通过调节Fe3O4@Apt-MIH等电点提高PEI的耐酸性能,有助于目标识别。选择性研究表明,适体和功能单体对氨苄西林具有高效的协同识别作用,印迹因子为6.90,协同识别因子为1.48。该固相微萃取材料耦合高效液相色谱法,线性范围为10 ~ 1000 μg/L,检出限为7.67 μg/L,可选择性分离检测牛奶和蜂蜜中的氨苄西林,样品基质干扰最小,回收率在95.2% ~ 102%之间。
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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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