Fathi Fatemeh, Sueoka Brandon, Zhao Feng, Zeng Xiangqun
Department of Chemistry, Oakland University, Rochester, Michigan 48309, United States.
Micro/Nanoelectronics and Energy Laboratory, School of Engineering and Computer Science, Washington State University, Vancouver, Washington 98686, United States.
Anal Chem. 2023 Mar 21;95(11):4855-4862. doi: 10.1021/acs.analchem.2c03609. Epub 2023 Mar 9.
In this work, we designed, fabricated, and characterized the first nitrogen (N)-doped single-crystalline 4H silicon carbide (4H-SiC) electrode for sensing the neurotransmitter dopamine. This N-doped 4H-SiC electrode showed good selectivity for redox reactions of dopamine in comparison with uric acid (UA), ascorbic acid (AA), and common cationic ([Ru(NH)]), anionic ([Fe(CN)]), and organic (methylene blue) redox molecules. The mechanisms of this unique selectivity are rationalized by the unique negative Si valency and adsorption properties of the analytes on the N-doped 4H-SiC surface. Quantitative electrochemical detection of dopamine by the 4H-SiC electrode was achieved in the linear range from 50 nM to 10 μM with a detection limit of 0.05 μM and a sensitivity of 3.2 nA.μM in a pH = 7.4 phosphate buffer solution. In addition, the N-doped 4H-SiC electrode demonstrated excellent electrochemical stability. This work forms the foundation for developing 4H-SiC as the next-generation robust and biocompatible neurointerface material for a broad range of applications such as the in vivo sensing of neurotransmitters.
在这项工作中,我们设计、制备并表征了首个用于检测神经递质多巴胺的氮(N)掺杂单晶4H碳化硅(4H-SiC)电极。与尿酸(UA)、抗坏血酸(AA)以及常见的阳离子([Ru(NH)])、阴离子([Fe(CN)])和有机(亚甲基蓝)氧化还原分子相比,这种N掺杂的4H-SiC电极对多巴胺的氧化还原反应表现出良好的选择性。这种独特选择性的机制可通过N掺杂4H-SiC表面上独特的负硅价态以及分析物的吸附特性来解释。在pH = 7.4的磷酸盐缓冲溶液中,4H-SiC电极对多巴胺进行定量电化学检测的线性范围为50 nM至10 μM,检测限为0.05 μM,灵敏度为3.2 nA·μM。此外,N掺杂的4H-SiC电极表现出优异的电化学稳定性。这项工作为将4H-SiC开发成为下一代坚固且具有生物相容性的神经界面材料奠定了基础,可用于广泛的应用,如神经递质的体内传感。