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一种集成有抗菌微针阵列的可穿戴防污电化学传感器,用于检测组织间液中的尿酸。

A wearable antifouling electrochemical sensor integrated with an antimicrobial microneedle array for uric acid detection in interstitial fluid.

作者信息

Lv Mingrui, Wang Lei, Hou Yiting, Qiao Xiujuan, Luo Xiliang

机构信息

Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, Shandong Key Laboratory of Biochemical Analysis, College of Chemistry and Molecular Engineering, Qingdao University of Science & Technology, Qingdao, 266042, China.

Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, Shandong Key Laboratory of Biochemical Analysis, College of Chemistry and Molecular Engineering, Qingdao University of Science & Technology, Qingdao, 266042, China.

出版信息

Anal Chim Acta. 2025 Feb 15;1339:343610. doi: 10.1016/j.aca.2025.343610. Epub 2025 Jan 3.

DOI:10.1016/j.aca.2025.343610
PMID:39832880
Abstract

Wearable microneedle array (MNA) based electrochemical sensors have gained increasing attention for their capability to analyze biomarkers in the interstitial fluid (ISF), enabling noninvasive, continuous monitoring of health parameters. However, challenges such as nonspecific adsorption of biomolecules on the sensor surfaces and the risk of infection at the microneedle penetration sites hinder their practical application. Herein, a wearable dual-layer microneedle patch was prepared to overcome these issues by integrating an antimicrobial microneedle layer with an antifouling sensing layer. The microneedle layer was prepared from polyvinyl alcohol, carboxylated nanocellulose, quaternary ammonium chitosan and carbon nanotubes, and it possessed antimicrobial and mechanical properties necessary for skin penetration, ISF collection and effective transmission to the sensing layer. The sensing layer was prepared from bacterial cellulose, epoxy propyl dimethyl dodecyl ammonium chloride, carbon nanotubes and gold nanoparticles, and it was capable of preventing biofouling and sensing uric acid (UA) in ISF. The wearable MNA based sensor exhibited a linear range of 0.5 μM - 2.5 μM and 9.6 μM - 2.15 mM for UA detection, with a limit of detection of 0.17 μM. Moreover, it was capable of accurately monitoring UA levels in ISF of mice without significant biofouling, as verified by the ELISA method. This innovative wearable sensor based on the MNA effectively balances the antifouling and antimicrobial functions, offering a reliable strategy for the assay of ISF, and making it a promising tool for personalized and decentralized health monitoring.

摘要

基于可穿戴微针阵列(MNA)的电化学传感器因其能够分析间质液(ISF)中的生物标志物,实现对健康参数的无创、连续监测而受到越来越多的关注。然而,诸如生物分子在传感器表面的非特异性吸附以及微针穿刺部位的感染风险等挑战阻碍了它们的实际应用。在此,通过将抗菌微针层与防污传感层相结合,制备了一种可穿戴双层微针贴片以克服这些问题。微针层由聚乙烯醇、羧化纳米纤维素、季铵壳聚糖和碳纳米管制成,它具有皮肤穿透、ISF采集以及有效传输至传感层所需的抗菌和机械性能。传感层由细菌纤维素、环氧丙基二甲基十二烷基氯化铵、碳纳米管和金纳米颗粒制成,它能够防止生物污染并传感ISF中的尿酸(UA)。基于可穿戴MNA的传感器对UA检测的线性范围为0.5 μM - 2.5 μM和9.6 μM - 2.15 mM,检测限为0.17 μM。此外,正如酶联免疫吸附测定法所验证的那样,它能够在无明显生物污染的情况下准确监测小鼠ISF中的UA水平。这种基于MNA的创新型可穿戴传感器有效地平衡了防污和抗菌功能,为ISF检测提供了一种可靠的策略,使其成为个性化和去中心化健康监测的有前途的工具。

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