Nanogap Electrochemistry and Sensor Technology at the Molecular Limit

分子极限的纳米间隙电化学和传感器技术

• 批准号: EP/I028706/1
• 负责人: Frank Marken
• 金额: $ 38.65万
• 依托单位: University of Bath
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2011
• 资助国家: 英国
• 起止时间: 2011 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FI028706%2F1
• 关键词: Nanogap; Electrochemistry; Sensor; Technology; Molecular

Sensors with electrochemical stimulus and read-out have found wide-spread use in gas, environmental, and medical trace analysis. Low cost and reliability as well as miniaturisation are major factors in commercialisation and mass production and in particular cheap screen printed sensors have dominated for example in the medical glucose sensing field. The low cost of these devices has been the secret to their commercial success and wide distribution. More powerful generator-collector electrode systems have been initially developed by Nekrasov and Frumkin and then further developed for rotating ring-disc systems, dual and interdigitated band electrode systems, in SECM and in STM, as well as in dual flow channel systems. Work with microelectrode arrays has been reported for electroanalysis and for patterning in DNA synthesisers. However, in these devices the inter-electrode gap has always been relatively large and the potential benefits of sub-micron gaps have not been exploited. In this project we propose (i) to develop extremely small gap systems to reach the limit of single molecule detection and (ii) to device novel bipotentiostat junction technology for powerful sensors for a wide range of applications.Our project hypothesis is that junction electrodes with 100 nm or less inter-electrode gap allow novel (electro-)chemical sensor processes to be exploited and investigated which have not been considered/realised in previous studies e.g. using conventional SECM and STM or in studies employing single-electrode electrochemical processes. The junction electrode formation is based on a robust (cheap, fast, & reproducible) electro-deposition approach which will need refinement and optimisation for particular applications. New experimental protocols will be developed to control surface roughness, improve growth & geometry, to introduce new junction materials, and to coat/fill sensor junctions. Diffusion within the junction will be investigated and short lived intermediates generated (for example HS., O2., O3., and other radical species) and modulator-sensor experiments conducted where pulses of reagents are generated at one (or more) modulator electrodes. Multi-dimensional pulse voltammetry with specifically optimised pulse sequences will provide higher sensitivity and higher selectivity and allow unusual detection modes (e.g. based on hydroxide pulses, see glucose detection in neutral solution aided by hydroxide pulses). The numerical simulation (based on new GPU methods ) of dual disc or band electrode systems and for junction electrodes is challenging and will provide important insight into physical phenomena, chemical mechanisms, and sensor optimisation.

具有电化学激励和读出的传感器已在气体、环境和医学痕量分析中得到广泛应用。低成本和可靠性以及小型化是商业化和大规模生产的主要因素，特别是廉价的丝网印刷传感器在例如医疗葡萄糖感测领域中占主导地位。这些设备的低成本一直是其商业成功和广泛销售的秘诀。Nekrasov和Frumkin最初开发了更强大的发生器-集电极系统，然后进一步开发用于旋转环-盘系统、双和交叉指状带电极系统、SECM和STM以及双流道系统。微电极阵列的工作已被报道用于电分析和DNA合成器中的图案化。然而，在这些装置中，电极间间隙一直相对较大，并且亚微米间隙的潜在益处尚未被利用。在这个项目中，我们提出（i）开发极小的间隙系统，以达到单分子检测的极限，（ii）装置新型双恒电位结技术，用于广泛应用的强大传感器。我们的项目假设是，具有100 nm或更小电极间间隙的结电极允许新型双恒电位结技术。这是有待开发和研究的（电）化学传感器过程，其在先前的研究中没有被考虑/实现，例如使用常规的SECM和STM或在采用单电极电化学过程的研究中。结电极的形成是基于一个强大的（廉价，快速，可重复）电沉积方法，这将需要细化和优化特定的应用。将开发新的实验方案来控制表面粗糙度，改善生长和几何形状，引入新的结材料，并涂覆/填充传感器结。将研究结内的扩散并产生短寿命的中间体（例如HS.，氧气，氧气，和其它自由基种类）和在一个（或多个）调制器电极处产生试剂脉冲的情况下进行的调制器-传感器实验。具有特别优化的脉冲序列的多维脉冲伏安法将提供更高的灵敏度和更高的选择性，并允许不寻常的检测模式（例如，基于氢氧化物脉冲，参见氢氧化物脉冲辅助的中性溶液中的葡萄糖检测）。双圆盘或带状电极系统和结电极的数值模拟（基于新的GPU方法）具有挑战性，将为物理现象，化学机制和传感器优化提供重要的见解。

项目成果

Pulse electroanalysis at gold-gold micro-trench electrodes: chemical signal filtering.

金-金微沟槽电极的脉冲电解分析：化学信号过滤。

• DOI: 10.1039/c3fd00022b
• 发表时间: 2013
• 期刊: Faraday discussions
• 影响因子: 3.4
• 作者: Dale SE

A gold-gold oil microtrench electrode for liquid-liquid anion transfer voltammetry.

用于液-液阴离子转移伏安法的金-金油微沟槽电极。

• DOI: 10.1002/elps.201300071
• 发表时间: 2013
• 期刊: Electrophoresis
• 影响因子: 2.9
• 作者: Dale SE

Boron-doped diamond dual-plate microtrench electrode for generator-collector chloride/chlorine sensing

• DOI: 10.1016/j.elecom.2014.06.025
• 发表时间: 2014-09-01
• 期刊: ELECTROCHEMISTRY COMMUNICATIONS
• 影响因子: 5.4
• 作者: Gross, Andrew J.;Marken, Frank
• 通讯作者: Marken, Frank

Interdigitated ring electrodes: Theory and experiment

• DOI: 10.1016/j.jelechem.2013.10.009
• 发表时间: 2013-11-15
• 期刊: JOURNAL OF ELECTROANALYTICAL CHEMISTRY
• 影响因子: 4.5
• 作者: Barnes, Edward O.;Fernandez-la-Villa, Ana;Compton, Richard G.
• 通讯作者: Compton, Richard G.

Gold-gold junction electrodes:the disconnection method.

金-金连接电极：断开法。

• DOI: 10.1002/tcr.201100008
• 发表时间: 2012
• 期刊: Chemical record (New York, N.Y.)
• 作者: Dale SE