Shao Zijun, Puthongkham Pumidech, Hu KeKe, Jia Rui, Mirkin Michael V, Venton B Jill
Dept. of Chemistry, University of Virginia, Charlottesville, VA 22901.
Department of Chemistry and Biochemistry, Queens College-CUNY, Flushing, New York 11367 and Graduate Center of CUNY, New York, NY 10016, USA.
Electrochim Acta. 2020 Nov 20;361. doi: 10.1016/j.electacta.2020.137032. Epub 2020 Sep 5.
Carbon nanotube yarn microelectrodes (CNTYMEs) are an alternative to carbon-fiber microelectrodes (CFMEs) with interesting electrochemical properties because analyte is momentarily trapped in cavities between the CNTs. Here, we compare fast-scan cyclic voltammetry (FSCV) detection of catecholamines, including dopamine, norepinephrine, and epinephrine, at CNTYMEs, CFMEs, as well as cavity carbon nanopipette electrodes (CNPEs). At CFMEs, current decreases dramatically at high FSCV repetition frequencies. At CNTYMEs, current is almost independent of FSCV repetition frequency because the analytes are trapped in the crevices between CNTs, and thus the electrode acts like a thin-layer cell. At CFMEs, small cyclization product peaks are observed due to an intramolecular cyclization reaction to form leucocatecholamine, which is electroactive, and these peaks are largest for the secondary amine epinephrine. At CNTYMEs, more of the leucocatecholamine cyclization product is detected for all catecholamines because of the enhanced trapping effects, particularly at higher repetition rates where the reaction occurs more frequently and more product is accumulated. For epinephrine, the secondary peaks have larger currents than the primary oxidation peaks at 100 Hz, and similar trends are observed with faster scan rates and 500 Hz repetition frequencies. Finally, we examined CNPEs, which also momentarily trap neurotransmitters. Similar to CNTYMEs, at CNPEs, catecholamines have robust cyclization peaks, particularly at high repetition rates. Thus, CNTYMEs and CNPEs have thin layer cell behavior that facilitates high temporal resolution measurements, but catecholamines CVs are complicated by cyclization reactions. However, those additional peaks could be useful in discriminating the analytes, particularly epinephrine and norepinephrine.
碳纳米管纱线微电极(CNTYMEs)是碳纤维微电极(CFMEs)的一种替代品,具有有趣的电化学特性,因为分析物会瞬间被困在碳纳米管之间的空隙中。在此,我们比较了在CNTYMEs、CFMEs以及腔式碳纳米管电极(CNPEs)上对儿茶酚胺(包括多巴胺、去甲肾上腺素和肾上腺素)的快速扫描循环伏安法(FSCV)检测。在CFMEs上,当FSCV重复频率较高时,电流会急剧下降。在CNTYMEs上,电流几乎与FSCV重复频率无关,因为分析物被困在碳纳米管之间的缝隙中,因此该电极的作用类似于薄层电池。在CFMEs上,由于分子内环化反应形成了具有电活性的白儿茶酚胺,会观察到小的环化产物峰,对于仲胺肾上腺素来说,这些峰最大。在CNTYMEs上,由于捕获效应增强,所有儿茶酚胺都能检测到更多的白儿茶酚胺环化产物,特别是在较高的重复速率下,反应更频繁地发生,积累的产物更多。对于肾上腺素,在100 Hz时,二次峰的电流比一次氧化峰大,在更快的扫描速率和500 Hz重复频率下也观察到类似趋势。最后,我们研究了CNPEs,它也能瞬间捕获神经递质。与CNTYMEs类似,在CNPEs上,儿茶酚胺有很强的环化峰,特别是在高重复速率下。因此,CNTYMEs和CNPEs具有薄层电池行为,便于进行高时间分辨率测量,但儿茶酚胺的循环伏安图因环化反应而变得复杂。然而,这些额外的峰可能有助于区分分析物,特别是肾上腺素和去甲肾上腺素。