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Understanding the surface fouling mechanism of ultrananocrystalline diamond microelectrodes using microfluidics for neurochemical detection

机译：使用微流控技术了解超纳米晶金刚石微电极的表面结垢机理，用于神经化学检测

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摘要

Electrochemical methods are widely used for chronic neurochemical sensing, but thus far, the organic solution redox reactions fouled the electrodes' surface. It caused the reduction of sensitivity and the electrodes' lifetime.;Here, we present the boron-doped nanocrystalline diamond microelectrodes (BDUNCD) as the next generation electrode material for neurochemical sensor development. To aid in long-term chronic monitoring of neurochemicals, they have a wide window of electrochemical potential, extremely low background current, and excellent chemical inertness. The main research goal is to reduce the rate of electrode fouling due to the reaction by-products, and significantly extend their useful lifetime.;We systematically characterize the fouling mechanism at the BDUNCD microelectrode surface by investigating silver particles deposited on BDUNCD surface at different fouling conditions using customized microfluidic device. The fouling rates were carefully studied using two electrochemical techniques Fast Scan Cyclic Voltammetry (FSCV) and Amperometry (AM).;Furthermore, in-situ electrode cleaning methods were developed in PBS buffer solution. Under optimal conditions, the cleaning method extended the electrode sensitivity from ~6.5 hours to ~28 hours.;We developed a droplet based microfluidic platform to characterize three types of microelectrodes BDUNCD, nafion modified BDUNCD, and nafion multi wall carbon nanotube modified. BDUNCD dopamine signals enhance two to three times by Electrophoretic deposition (EPD) of nafion layer (50 nM), and enhance about 10 times in complementary nafion multi wall carbon nanotube modified BDUNCD. Specifically, the sensitivity, response time, and clearance rate of dopamine were determined in 9 hours of monitoring. In the presence of ascorbic acid and serotonin was studied using differential pulse voltammetry method, the selectivity comparison performs the multi-wall carbon nanotube superiority and achieved long-lasting 9 hours monitoring after nafion layer coating, it has the initial sensitivity of oxidation current DA (0.58 nA) and 5-HT (1.03 nA) with a sensitivity value of DA 1.18 microA microM-1 cm-2 and 5-HT 2.09 microA microM-1 cm -2. The other advantage of multi-wall carbon nanotube modified BDUNCD electrode reduces the limit of detection to 5.4 nM (DA) and with nitric acid treatment 1.78 nM (DA).
机译：电化学方法已广泛用于慢性神经化学感应，但到目前为止，有机溶液的氧化还原反应已污染了电极的表面。这导致灵敏度的降低和电极寿命的减少。；在此，我们介绍硼掺杂的纳米晶金刚石微电极（BDUNCD）作为用于神经化学传感器开发的下一代电极材料。为了对神经化学物质进行长期的长期监测，它们具有广阔的电化学势能窗口，极低的背景电流和出色的化学惰性。主要研究目标是降低反应副产物引起的电极结垢率，并显着延长其使用寿命。通过研究沉积在BDUNCD表面上的银颗粒在不同结垢下的系统性，我们系统地表征了BDUNCD微电极表面的结垢机理。条件使用定制的微流控设备。使用两种电化学技术快速扫描循环伏安法（FSCV）和安培法（AM）仔细研究结垢率;此外，在PBS缓冲溶液中开发了原位电极清洗方法。在最佳条件下，清洁方法将电极灵敏度从〜6.5小时扩展到〜28小时。;我们开发了基于液滴的微流体平台，以表征三种类型的微电极BDUNCD，nafion修饰的BDUNCD和nafion多壁碳纳米管修饰的。 BDUNCD多巴胺信号通过nafion层（50 nM）的电泳沉积（EPD）增强了2到3倍，在互补nafion多壁碳纳米管修饰的BDUNCD中增强了约10倍。具体而言，在监测的9小时内确定多巴胺的敏感性，响应时间和清除率。使用差示脉冲伏安法研究了抗坏血酸和5-羟色胺的存在下，选择性比较表现出多壁碳纳米管的优越性，并在nafion涂层涂覆后实现了持续9小时的监测，它具有氧化电流DA（ 0.58 nA）和5-HT（1.03 nA），其灵敏度值为DA 1.18 microA microM-1 cm-2和5-HT 2.09 microA microM-1 cm -2。多壁碳纳米管修饰的BDUNCD电极的另一个优点是将检出限降至5.4 nM（DA），硝酸处理后的检出限为1.78 nM（DA）。

著录项

  • 作者

    Chang, An-Yi.;

  • 作者单位

    Louisiana Tech University.;

  • 授予单位 Louisiana Tech University.;
  • 学科 Electrical engineering.;Chemistry.;Biomedical engineering.
  • 学位 Ph.D.
  • 年度 2017
  • 页码 142 p.
  • 总页数 142
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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