Development of a Photoelectrochemical Microelectrode Using an Organic Probe for Monitoring Hydrogen Sulfide in Living Brains

IF 6.7 1区化学 Q1 CHEMISTRY, ANALYTICAL

Analytical Chemistry Pub Date : 2024-11-22 DOI:10.1021/acs.analchem.4c05336

Yuanqiang Hao, Yewen Yang, Wenhui Wang, Hui Gu, Wansong Chen, Chunlan Li, Peisheng Zhang, Rongjin Zeng, Maotian Xu, Shu Chen

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引用次数: 0

Abstract

Hydrogen sulfide (H₂S) is an important bioactive molecule that plays a significant role in various functions, particularly in the living brain, where it is closely linked to cognition, memory, and several neurological diseases. Consequently, developing effective detection methods for H₂S is essential for studying brain functions and the underlying mechanisms of these diseases. This study aims to construct a novel photoelectrochemical (PEC) microelectrode Ti/TiO₂@HSP for the quantitative monitoring of H₂S levels in the living brain. The PEC microelectrode Ti/TiO₂@HSP is formed by covalently bonding a specifically designed organic PEC probe HSP, which possesses a D-π–A structure, to the surface of TiO₂ nanotubes generated via in situ anodic oxidation of titanium wire. The PEC probe HSP can effectively react with H₂S and generate significant photocurrent response under long-wavelength excitation light (560 nm), thereby achieving quantitative detection of H₂S. The sensor demonstrates high sensitivity and good selectivity. In vivo experiments utilizing the PEC microelectrode Ti/TiO₂@HSP enable the monitoring of dynamic changes in H₂S levels across various regions of the mouse brain. The findings reveal that in normal mice, the concentration of H₂S in the hippocampus is significantly higher than in the striatum and cerebral cortex. Additionally, following propargylglycine drug stimulation, H₂S concentrations in different brain regions were observed to decrease, with the most substantial reduction noted in the hippocampus. This suggests that cystathionine γ-lyase (CSE) is the primary enzyme responsible for H₂S production in this area, while the striatum exhibits a less pronounced decrease in H₂S concentration, indicating a reliance on alternative enzymatic pathways for H₂S production. Therefore, this study not only successfully develops a high-performance H₂S detection sensor but also provides new experimental tools and theoretical foundations for further exploring the roles of H₂S in neurophysiological and pathological processes.

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利用有机探针开发用于监测活体大脑中硫化氢的光电化学微电极

硫化氢（H2S）是一种重要的生物活性分子，在各种功能中发挥着重要作用，特别是在活体大脑中，它与认知、记忆和多种神经系统疾病密切相关。因此，开发有效的 H2S 检测方法对于研究大脑功能和这些疾病的潜在机制至关重要。本研究旨在构建一种新型光电化学（PEC）微电极 Ti/TiO2@HSP，用于定量监测活体大脑中的 H2S 水平。PEC微电极Ti/TiO2@HSP是通过将具有D-π-A结构的特殊设计的有机PEC探针HSP共价键合到钛丝原位阳极氧化生成的TiO2纳米管表面而形成的。PEC 探针 HSP 能有效地与 H2S 发生反应，并在长波长激发光（560 纳米）下产生显著的光电流响应，从而实现对 H2S 的定量检测。该传感器具有高灵敏度和良好的选择性。利用 PEC 微电极 Ti/TiO2@HSP 进行的体内实验能够监测小鼠大脑各区域 H2S 水平的动态变化。研究结果表明，正常小鼠海马区的 H2S 浓度明显高于纹状体和大脑皮层。此外，在丙炔甘氨酸药物刺激下，不同脑区的 H2S 浓度都会下降，其中海马区的下降幅度最大。这表明胱硫醚γ-赖氨酸酶（CSE）是该区域产生 H2S 的主要酶，而纹状体的 H2S 浓度下降不明显，表明 H2S 的产生依赖于其他酶的途径。因此，本研究不仅成功开发了一种高性能 H2S 检测传感器，还为进一步探索 H2S 在神经生理和病理过程中的作用提供了新的实验工具和理论基础。

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来源期刊

Analytical Chemistry 化学-分析化学

CiteScore

12.10

自引率

12.20%

发文量

1949

审稿时长

1.4 months

期刊介绍： Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.