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铂纳米颗粒/玉米醇溶蛋白/明胶/葡萄糖氧化酶修饰的激光诱导石墨烯电极用于多种生物流体中的无创葡萄糖传感器。

Laser-induced graphene electrode modified by platinum nanoparticle/zein/gelatin/glucose oxidase for non-invasive glucose sensor in multiple biofluids.

作者信息

Sakdaphetsiri Kittiya, Thaweeskulchai Thana, Sukmas Wiwittawin, Wang Joseph, Schulte Albert, Rodthongkum Nadnudda

机构信息

Metallurgy and Materials Science Research Institute, Chulalongkorn University, Bangkok, Thailand.

School of Biomolecular Science and Engineering (BSE), Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong, Thailand.

出版信息

Anal Chim Acta. 2025 Jun 1;1353:343974. doi: 10.1016/j.aca.2025.343974. Epub 2025 Mar 25.

Abstract

BACKGROUND

A non-invasive glucose biosensor for multiple biofluids based on platinum nanoparticle (Pt-NP)-modified laser-induced graphene (LIG) electrodes coated with a zein/gelatin/glucose oxidase (GOx) for amperometric detection of glucose is created. The biosensor fabrication is cost-effective and scalable, as it combines simple LIG electrode fabrication with direct Pt-NP electrodeposition and a sequence of drop-and-dry steps for zein and gelatin layer then GOx enzyme. The Pt-NP modification on the LIG electrode functions as an electrocatalyst to enhance the anodic HO signal, which is directly proportional to glucose concentration. The zein layer acts as a diffusion barrier to mitigate potential interferences, while the gelatin film provides amine groups for the glutaraldehyde-mediated immobilization of the GOx enzyme.

RESULTS

The key parameters of LIG were optimized, such as power laser, number of Pt-NP cycles, and zein concentration. In addition, LIG was characterized by Raman spectroscopy, SEM, and cyclic voltammetry (CV) to ensure graphitization and electron transfer performance. The as prepared LIG/Pt-NP/Zein/Gel-GOx glucose biosensor was in anodic HO detection mode and tested for glucose measurements in multiple biofluids including sweat, saliva, and urine. At HO detection potential of +0.4 V, a linear detection range from 0 up to 2 mM glucose was obtained with a limit of detection (LOD) of 0.01 mM, making it feasible for glucose determination in various clinically relevant biofluids. By comparing with the commercial SPE, this LIG-based sensor offered much higher detection sensitivity towards both HO and glucose, making it a superior choice for electrochemical analysis.

SIGNIFICANCE

This LIG/Pt-NPs/Zein/Gel-GOx offers a practical and high sensitivity approach to glucose measurement with a wide linearity for multiple biofluids. Given the straightforward and easily scalable process, this high-performance, LIG-based glucose biosensor presents a compelling alternative over commercial screen-printed electrode. Highlighted the novelty using zein as a protective layer to reduce interferences. Owing to the simplicity of fabrication with high potential for up-scaling, this high analytical performance biosensor might be an alternative tool for multiplex glucose biosensors in point-of-care applications.

摘要

背景

制备了一种基于铂纳米颗粒(Pt-NP)修饰的激光诱导石墨烯(LIG)电极的用于多种生物流体的无创葡萄糖生物传感器,该电极涂有玉米醇溶蛋白/明胶/葡萄糖氧化酶(GOx),用于葡萄糖的安培检测。这种生物传感器的制造具有成本效益且可扩展,因为它将简单的LIG电极制造与直接的Pt-NP电沉积以及一系列用于玉米醇溶蛋白和明胶层然后是GOx酶的滴加和干燥步骤相结合。LIG电极上的Pt-NP修饰作为一种电催化剂,可增强与葡萄糖浓度成正比的阳极HO信号。玉米醇溶蛋白层作为扩散屏障,以减轻潜在干扰,而明胶膜为戊二醛介导的GOx酶固定提供胺基。

结果

优化了LIG的关键参数,如激光功率、Pt-NP循环次数和玉米醇溶蛋白浓度。此外,通过拉曼光谱、扫描电子显微镜和循环伏安法(CV)对LIG进行表征,以确保石墨化和电子转移性能。所制备的LIG/Pt-NP/玉米醇溶蛋白/明胶-GOx葡萄糖生物传感器处于阳极HO检测模式,并用于在包括汗液、唾液和尿液在内的多种生物流体中进行葡萄糖测量。在HO检测电位为+0.4 V时,获得了从0到2 mM葡萄糖的线性检测范围,检测限(LOD)为0.01 mM,这使得在各种临床相关生物流体中测定葡萄糖成为可能。通过与商业SPE进行比较,这种基于LIG的传感器对HO和葡萄糖均具有更高的检测灵敏度,使其成为电化学分析的优越选择。

意义

这种LIG/Pt-NPs/玉米醇溶蛋白/明胶-GOx为多种生物流体的葡萄糖测量提供了一种实用且高灵敏度的方法,具有宽线性范围。鉴于其直接且易于扩展的过程,这种基于LIG的高性能葡萄糖生物传感器是商业丝网印刷电极的一个极具吸引力的替代方案。突出了使用玉米醇溶蛋白作为保护层以减少干扰的新颖性。由于制造简单且具有高放大潜力,这种高分析性能的生物传感器可能是即时护理应用中多重葡萄糖生物传感器的替代工具。

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