Department of Chemistry, University of North Carolina at Chapel Hill, CB 3290, Chapel Hill, NC, 27599, United States.
Department of Chemistry, University of North Carolina at Chapel Hill, CB 3290, Chapel Hill, NC, 27599, United States.
Anal Chim Acta. 2019 Jan 3;1045:67-76. doi: 10.1016/j.aca.2018.08.054. Epub 2018 Sep 1.
Continuous, in situ detection of hydrogen sulfide (HS) in biological milieu is made possible with electrochemical methods, but direct amperometry is constrained by the generation of elemental sulfur as an oxidative byproduct. Deposition of a sulfur layer passivates the working electrode, reducing sensitivity and causing performance variability. Herein, we report on the use of a surface preconditioning procedure to deposit elemental sulfur on a glassy carbon electrode prior to measurement and evaluate performance with common analytical metrics. The lack of traditional anti-poisoning techniques (e.g. redox mediators, cleaning pulses) also allowed for facile surface modification with electropolymerized films. For the first time, a series of electropolymerized films were characterized for their HS permselective behavior against common biological interferents. Highly selective, film-modified electrodes were then evaluated for their anti-biofouling ability in simulated wound fluid. The final optimized electrode was capable of measuring HS with a low detection limit (i.e., <100 nM) and ∼80% of its initial sensitivity in proteinaceous media.
电化学方法可实现生物环境中硫化氢(HS)的连续原位检测,但直接电流法受到元素硫作为氧化副产物生成的限制。硫层的沉积会使工作电极钝化,降低灵敏度并导致性能变化。在此,我们报告了在测量前使用表面预处理程序在玻碳电极上沉积元素硫的方法,并使用常见的分析指标评估性能。缺乏传统的抗中毒技术(例如氧化还原介质、清洗脉冲)也允许用电化学聚合膜进行简单的表面改性。首次对一系列电化学聚合膜的 HS 选择透过性能进行了表征,以对抗常见的生物干扰物。然后,评估了具有高选择性的膜修饰电极在模拟伤口液中的抗生物污染能力。最终优化的电极能够在蛋白质介质中以低检测限(即 <100 nM)和初始灵敏度的约 80%测量 HS。