Conductive Metal–Organic Framework Microelectrodes Regulated by Conjugated Molecular Wires for Monitoring of Dopamine in the Mouse Brain

化学 电极 多巴胺 共轭体系 微电极 导电体 纳米技术 金属 神经科学 有机化学 聚合物 物理化学 量子力学 生物 物理 材料科学
作者
Yue Wang,Yinjie Qian,Limin Zhang,Zhihui Zhang,Shiwei Chen,Jinfeng Liu,Xiao He,Yang Tian
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (4): 2118-2126 被引量:81
标识
DOI:10.1021/jacs.2c07053
摘要

Herein, we demonstrated a strategy to regulate the conductive metal-organic framework (MOF) surface, by the conjugated molecule wires for selective and sensitive determination of dopamine (DA) in the live brain. The MOFs were decorated at the carbon fiber electrode deposited by Au nanoleaves as the upper electric transducer to provide rich electrocatalytic sites for electron transfer of neurochemicals at the electrode surface, leading to greatly enhanced sensitivity for detection of neurochemicals. On the other hand, the conjugated molecular wire, 4-(thiophen-3-ylethynyl)-benzaldehyde (RP1), was synthesized and assembled as an underlying bridge to regulate the electrochemical processes at the MOF-based electrode, specifically decreasing the reaction Gibbs free energy of DA oxidation, thus selectively promoting the heterogeneous electron transfer of DA from the MOF layer to the electrode surface. Owing to the electrocatalytic activity for DA oxidation, the present microsensor exhibited high selectivity for real-time tracking of DA in a good linear relationship in the range of 0.004-0.4 μM with a detection limit of 1 nM. Eventually, this functionalized electrode was successfully applied for in vivo monitoring of DA in mouse brains with Parkinson's disease (PD) model. The results indicated that the levels of DA were obviously decreased in both acute and subacute PD models. Moreover, the level of DA strongly depended on the amount of uric acid (UA), a physiological antioxidant, which rose as the UA amount was lower than 200 mg kg-1 but was downregulated again after treatment by a higher amount of UA.
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