Yang Cheng, Trikantzopoulos Elefterios, Jacobs Christopher B, Venton B Jill
Department of Chemistry, University of Virginia, Charlottesville, VA, 22904, United States.
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, TN, 37831, United States.
Anal Chim Acta. 2017 May 1;965:1-8. doi: 10.1016/j.aca.2017.01.039. Epub 2017 Jan 31.
Fibers made of CNTs are attractive microelectrode sensors because they can be directly fabricated into microelectrodes. Different protocols for making CNT fibers have been developed, but differences in surface structure and therefore electrochemical properties that result have not been studied. In this study, we correlated the surface and electrochemical properties for neurochemical detection at 3 types of materials: CNT fibers produced by wet spinning with (1) polyethylenimine (PEI/CNT) or (2) chlorosulfonic acid (CA/CNT), and (3) CNT yarns made by solid-based CNT drawing. CNT yarns had well-aligned, high purity CNTs, abundant oxygen functional groups, and moderate surface roughness which led to the highest dopamine current density (290 ± 65 pA/cm) and fastest electron transfer kinetics. The crevices of the CNT yarn and PEI/CNT fiber microelectrodes allow dopamine to be momentarily trapped during fast-scan cyclic voltammetry detection, leading to thin-layer cell conditions and a response that was independent of applied waveform frequency. The larger crevices on the PEI/CNT fibers led to a slower time response, showing too much roughness is detrimental to fast detection. CA/CNT fibers have a smoother surface and lower currents, but their negative surface charge results in high selectivity for dopamine over uric acid or ascorbic acid. Overall, small crevices, high conductivity, and abundant oxygen groups led to high sensitivity for amine neurotransmitters, such as dopamine and serotonin. Thus, different surfaces of CNT fibers result in altered electrochemical properties and could be used in the future to predict and control electrochemical performance.
由碳纳米管制成的纤维是极具吸引力的微电极传感器,因为它们可以直接制成微电极。目前已开发出不同的制备碳纳米管纤维的方法,但尚未对由此产生的表面结构差异以及电化学性质差异进行研究。在本研究中,我们关联了三种材料用于神经化学检测时的表面性质和电化学性质:通过湿法纺丝制备的碳纳米管纤维,其中(1)使用聚乙烯亚胺(PEI/CNT)或(2)氯磺酸(CA/CNT),以及(3)通过基于固体的碳纳米管拉伸制成的碳纳米管纱线。碳纳米管纱线具有排列良好、高纯度的碳纳米管、丰富的氧官能团以及适度的表面粗糙度,这导致其具有最高的多巴胺电流密度(290±65 pA/cm)和最快的电子转移动力学。碳纳米管纱线和PEI/CNT纤维微电极的缝隙使得多巴胺在快速扫描循环伏安法检测过程中能够瞬间捕获,从而形成薄层电池条件,且响应与施加的波形频率无关。PEI/CNT纤维上较大的缝隙导致时间响应较慢,这表明粗糙度太大不利于快速检测。CA/CNT纤维表面更光滑且电流较低,但其负表面电荷导致对多巴胺的选择性高于尿酸或抗坏血酸。总体而言,小缝隙、高导电性和丰富的氧基团导致对多巴胺和血清素等胺类神经递质具有高灵敏度。因此,碳纳米管纤维的不同表面会导致电化学性质改变,未来可用于预测和控制电化学性能。