Abstract：
Herein we introduce a novel water-based graphite ink modified with multiwalled carbon nanotubes, designed for the development of the first wearable self-powered biosensor enabling alcohol abuse detection through sweat analysis. The stencil-printed graphite (SPG) electrodes, printed onto a flexible substrate, were modified by casting multiwalled carbon nanotubes (MWCNTs), electrodepositing polymethylene blue (pMB) at the anode to serve as a catalyst for nicotinamide adenine dinucleotide (NADH) oxidation, and hemin at the cathode as a selective catalyst for H2O2 reduction. Notably, alcohol dehydrogenase (ADH) was additionally physisorbed onto the anodic electrode, and alcohol oxidase (AOx) onto the cathodic electrode. The self-powered biosensor was assembled using the ADH/pMB-MWCNTs/SPG||AOx/Hemin-MWCNTs/SPG configuration, enabling the detection of ethanol as an analytical target, both at the anodic and cathodic electrodes. Its performance was assessed by measuring polarization curves with gradually increasing ethanol concentrations ranging from 0 to 50 mM. The biosensor demonstrated a linear detection range from 0.01 to 0.3 mM, with a detection limit (LOD) of 3 ± 1 µM and a sensitivity of 64 ± 2 μW mM-1, with a correlation coefficient of 0.98 (RSD 8.1%, n = 10 electrode pairs). It exhibited robust operational stability (over 2800 s with continuous ethanol turnover) and excellent storage stability (approximately 93% of initial signal retained after 90 days). Finally, the biosensor array was integrated into a wristband and successfully evaluated for continuous alcohol abuse monitoring. This proposed system displays promising attributes for use as a flexible and wearable biosensor employing biocompatible water-based inks, offering potential applications in forensic contexts.
摘要：
本文介绍了一种新型的多壁碳纳米管改性的水基石墨油墨,设计用于开发第一个可穿戴式自供电生物传感器，通过汗液分析实现酒精滥用检测。模版印刷石墨（SPG）电极，印刷到柔性基板上，通过铸造多壁碳纳米管（MWCNTs）进行改性，在阳极电沉积聚亚甲基蓝（pMB），以作为烟酰胺腺嘌呤二核苷酸（NADH）氧化的催化剂，和氯化血红素在阴极作为H2O2还原的选择性催化剂。值得注意的是,醇脱氢酶(ADH)被另外物理吸附到阳极电极上，和醇氧化酶(AOx)到阴极电极上。使用ADH/pMB-MWCNT/SPG||AOx/Hemin-MWCNT/SPG配置组装自供电生物传感器，能够检测乙醇作为分析目标，在阳极和阴极电极。通过测量0至50mM范围内逐渐增加的乙醇浓度的极化曲线来评估其性能。生物传感器显示出0.01至0.3mM的线性检测范围，检出限（LOD）为3±1µM，灵敏度为64±2μWmM-1，相关系数为0.98（RSD为8.1％，n=10个电极对)。它表现出强大的操作稳定性（超过2800秒，连续乙醇周转）和出色的储存稳定性（90天后保留了约93％的初始信号）。最后,将生物传感器阵列集成到腕带中,并成功进行了连续酒精滥用监测评估.该提出的系统显示出有希望的属性，可用作采用生物相容性水基墨水的柔性和可穿戴生物传感器。在法医环境中提供潜在的应用。
