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基于导电金属有机框架(Cu(苯六硫醇))纳米片修饰电极的抗坏血酸电化学传感

Electrochemistry sensing of ascorbic acid based on conductive metal-organic framework (Cu(benzenehexathiol)) nanosheets modified electrode.

作者信息

Yuan Runhao, Zhong Xiaolong, Sun Weiming, Wang Jian, Huang Chuanhui, Lin Zhenyu, Zheng Jianping

机构信息

Ministry of Education Key Laboratory for Analytical Science of Food Safety and Biology, Fujian Provincial Key Laboratory of Analysis and Detection for Food Safety, College of Chemistry, Fuzhou University, Fuzhou, Fujian, 350116, China.

The Department of Basic Chemistry, The School of Pharmacy, Fujian Medical University, Fuzhou, Fujian, 350108, China.

出版信息

Anal Chim Acta. 2025 Jun 1;1353:343980. doi: 10.1016/j.aca.2025.343980. Epub 2025 Mar 28.

Abstract

BACKGROUND

Bulk-type conductive metal-organic frameworks (c-MOFs) had been applied to modify the electrode and used in electrochemical sensing because of the high conductive properties. But which still suffer from low mass permeability, restricted active site exposure, and poor accessibility due to the coordination saturation at metal sites in the bulk-type c-MOF. Recent studies have demonstrated that transforming bulk-type MOFs into MOFs nanosheets (NSs) can maximize the exposure of active sites and mass transfer. However, c-MOF NSs have rarely been applied in electrochemical sensing.

RESULTS

This study presents NSs type c-MOF Cu(benzenehexathiol) (CuBHT), synthesized using a simple sacrificial template method. CuBHT NSs were modified onto a glassy carbon electrode (GCE) to prepare CuBHT NSs/GCE, which was then applied to sense the model target ascorbic acid (AA), the system exhibits high sensitivity of 1.521 mA mM cm and a wide linear range of 1-789 μM, low detection limit of 0.46 μM. The sensitivity is 1.90 times higher than that of bulk-type CuBHT nanoparticles (NPs) modified GCE, which can be attributed to the CuBHT NSs having more exposed Cu sites on their surfaces. CuBHT NSs/GCE was then used to monitor AA levels in human sweat during daily activities or exercise, and the results indicated high reliability compared to the vitamin C ASA kit method.

SIGNIFICANCE

The design of c-MOF CuBHT NSs/GCE lead to better performance in terms of sensitivity and low detection limit in AA sensing compared to bulk-type nanoparticles. The AA sensing mechanism based on CuBHT was investigated, and the sensing system was demonstrated by detecting AA in sweat. This work advances both the fundamental understanding and practical applications of c-MOF NSs in AA sensing.

摘要

背景

块状导电金属有机框架(c-MOFs)因其高导电性能已被应用于修饰电极并用于电化学传感。但由于块状c-MOF中金属位点的配位饱和,其仍存在质量渗透率低、活性位点暴露受限和可及性差等问题。最近的研究表明,将块状MOF转化为MOF纳米片(NSs)可以最大程度地暴露活性位点并实现传质。然而,c-MOF NSs很少应用于电化学传感。

结果

本研究展示了通过简单的牺牲模板法合成的NSs型c-MOF Cu(苯六硫醇)(CuBHT)。将CuBHT NSs修饰在玻碳电极(GCE)上制备CuBHT NSs/GCE,然后将其用于检测模型目标物抗坏血酸(AA),该体系表现出1.521 mA mM cm的高灵敏度、1 - 789 μM的宽线性范围以及0.46 μM的低检测限。该灵敏度比块状CuBHT纳米颗粒(NPs)修饰的GCE高1.90倍,这可归因于CuBHT NSs表面有更多暴露的Cu位点。然后将CuBHT NSs/GCE用于监测日常活动或运动期间人体汗液中的AA水平,结果表明与维生素C ASA试剂盒法相比具有高可靠性。

意义

与块状纳米颗粒相比,c-MOF CuBHT NSs/GCE的设计在AA传感的灵敏度和低检测限方面表现出更好的性能。研究了基于CuBHT的AA传感机制,并通过检测汗液中的AA证明了该传感系统。这项工作推进了c-MOF NSs在AA传感方面的基础理解和实际应用。

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