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一种基于氮掺杂石墨烯量子点和分子印迹聚合物的荧光传感器,用于环境和临床基质中美罗培南的选择性和灵敏检测。

A fluorescent sensor based on nitrogen-doped graphene quantum dots and molecularly imprinted polymers for selective and sensitive detection of meropenem in environmental and clinical matrices.

作者信息

Serag Ahmed, Abdelazim Ahmed H, Ramzy Sherif, Alnemari Reem M, Alzhrani Rami M, Abduljabbar Maram H, Althobaiti Yusuf S, Alosaimi Manal E, Alaqel Saleh I, Almalki Atiah H

机构信息

Pharmaceutical Analytical Chemistry Department, Faculty of Pharmacy, Al-Azhar University, Nasr City, 11751, Cairo, Egypt.

Pharmaceutical Analytical Chemistry Department, Faculty of Pharmacy, Al-Azhar University, Nasr City, 11751, Cairo, Egypt.

出版信息

Talanta. 2026 Jan 1;296:128442. doi: 10.1016/j.talanta.2025.128442. Epub 2025 Jun 7.

DOI:10.1016/j.talanta.2025.128442
PMID:40527076
Abstract

Meropenem, a broad-spectrum carbapenem antibiotic, is widely used in the treatment of severe bacterial infections. However, the accurate determination of meropenem in complex biological and environmental matrices remains a significant analytical challenge. In this study, we report the development of a highly sensitive and selective fluorescence sensor for the determination of meropenem using nitrogen-doped graphene quantum dots capped with a surface molecular imprinting polymer (N-GQDs@MIP). Characterization and optical properties of the N-GQDs@MIP nanocomposite were thoroughly investigated using various analytical techniques. Upon excitation at 365 nm, the sensor exhibited strong fluorescence emission at 450 nm which quenched upon meropenem binding. Mechanistic studies revealed a static quenching process driven by strong host-guest interactions between meropenem and the imprinted polymer recognition sites, as confirmed by Stern-Volmer analysis and thermodynamic calculations. Density functional theory calculations also revealed specific molecular interactions between meropenem and the N-GQDs@MIP. Central composite design optimization was employed to systematically investigate the effect of key experimental parameters, such as pH, reaction time, and N-GQDs@MIP concentration, on the sensor's performance. A significant quadratic regression model was obtained, with a high coefficient of determination (R = 0.956) and excellent predictive capability that was further employed to maximize the sensor's sensitivity. Validation of the analytical method demonstrated a wide linear range of 25-1500 ng/mL, a low limit of detection of 7.42 ng/mL, and excellent selectivity against structurally similar antibiotics as well as good stability and reusability. The developed N-GQDs@MIP sensor was successfully applied to the determination of meropenem in pharmaceutical formulations, spiked human serum, urine, and environmental water samples with satisfactory recoveries and precision. Hence, this facile and robust fluorescence sensor offers a promising analytical platform for the sensitive, selective, and reliable quantification of meropenem in various clinical and environmental applications posing the current approach as a valuable alternative to existing analytical methods.

摘要

美罗培南是一种广谱碳青霉烯类抗生素,广泛用于治疗严重细菌感染。然而,在复杂的生物和环境基质中准确测定美罗培南仍然是一项重大的分析挑战。在本研究中,我们报告了一种高灵敏度和选择性的荧光传感器的开发,该传感器使用表面分子印迹聚合物包覆的氮掺杂石墨烯量子点(N-GQDs@MIP)来测定美罗培南。使用各种分析技术对N-GQDs@MIP纳米复合材料的表征和光学性质进行了深入研究。在365 nm激发下,该传感器在450 nm处表现出强烈的荧光发射,美罗培南结合后荧光猝灭。机理研究揭示了由美罗培南与印迹聚合物识别位点之间的强主客体相互作用驱动的静态猝灭过程,这通过Stern-Volmer分析和热力学计算得到证实。密度泛函理论计算还揭示了美罗培南与N-GQDs@MIP之间的特定分子相互作用。采用中心复合设计优化系统研究了pH、反应时间和N-GQDs@MIP浓度等关键实验参数对传感器性能的影响。获得了一个显著的二次回归模型,其决定系数高(R = 0.956)且具有出色的预测能力,进一步用于最大化传感器的灵敏度。分析方法的验证表明线性范围宽,为25 - 1500 ng/mL,检测限低至7.42 ng/mL,对结构相似的抗生素具有出色的选择性,以及良好的稳定性和可重复使用性。所开发的N-GQDs@MIP传感器成功应用于药物制剂、加标人血清、尿液和环境水样中美罗培南的测定,回收率和精密度令人满意。因此,这种简便且稳健的荧光传感器为在各种临床和环境应用中灵敏、选择性和可靠地定量美罗培南提供了一个有前景的分析平台,使当前方法成为现有分析方法的有价值替代方案。

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