Accelerated Electron Transfer in Nanostructured Electrodes Improves the Sensitivity of Electrochemical Biosensors.
Accelerated Electron Transfer in Nanostructured Electrodes Improves the Sensitivity of Electrochemical Biosensors.
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DOI：
10.1002/advs.202102495
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发表时间：
2021-12
期刊：
影响因子：
--
通讯作者：
Soh HT
中科院分区：
文献类型：
--
作者：
Fu K;Seo JW;Kesler V;Maganzini N;Wilson BD;Eisenstein M;Murmann B;Soh HT
电化学生物传感器将分子检测、信号处理和无线通信集成在一个小型化、低成本的系统中，具有令人兴奋的潜力。然而，随着电化学生物传感器小型化到微米级，它们的信噪比下降，降低了它们在分子诊断中的效用。已有研究报道，纳米结构电极可以改善电化学生物传感器信号，但由于其潜在机制尚不清楚，因此很难充分利用这一现象来提高生物传感器的性能。本文对纳米孔电极上的电化学适体生物传感器进行了优化，通过调整孔径、探针密度和电化学测量参数来提高灵敏度。此外，研究人员还提出了一种新的机制，即由于减少了电荷筛选，电子转移在纳米结构电极内被物理加速，从而提高了灵敏度，并进行了实验验证。与该平台增加的表面积相一致，这种新发现的效应可以产生高达24倍的信号电平增加，并且相对于具有相同足迹的平面电极，检测下限接近4倍。重要的是，这种策略可以推广到几乎任何电化学适体传感器，在需要小型化的应用中实现灵敏的检测，并且同样应该广泛适用于提高电化学生物传感器的总体性能。在这项工作中，具有可调孔隙度的纳米结构电极用于电化学生物传感，比传统的平面电极提供更高的信号水平和更低的检测极限。重要的是，提出了一种新的机制，在纳米结构电极内，由于减少电荷筛选，电子转移被物理加速，从而提高灵敏度，并通过实验验证。
Electrochemical biosensors hold the exciting potential to integrate molecular detection with signal processing and wireless communication in a miniaturized, low‐cost system. However, as electrochemical biosensors are miniaturized to the micrometer scale, their signal‐to‐noise ratio degrades and reduces their utility for molecular diagnostics. Studies have reported that nanostructured electrodes can improve electrochemical biosensor signals, but since the underlying mechanism remains poorly understood, it remains difficult to fully exploit this phenomenon to improve biosensor performance. In this work, electrochemical aptamer biosensors on nanoporous electrode are optimized to achieve improved sensitivity by tuning pore size, probe density, and electrochemical measurement parameters. Further, a novel mechanism in which electron transfer is physically accelerated within nanostructured electrodes due to reduced charge screening, resulting in enhanced sensitivity is proposed and experimentally validated. In concert with the increased surface areas achieved with this platform, this newly identified effect can yield an up to 24‐fold increase in signal level and nearly fourfold lower limit of detection relative to planar electrodes with the same footprint. Importantly, this strategy can be generalized to virtually any electrochemical aptamer sensor, enabling sensitive detection in applications where miniaturization is a necessity, and should likewise prove broadly applicable for improving electrochemical biosensor performance in general. In this work, nanostructured electrodes with tunable porosity for electrochemical biosensing that offer increased signal level and lower limit of detection than conventional planar electrodes are reported. Importantly, a novel mechanism in which electron transfer is physically accelerated within nanostructured electrodes due to reduced charge screening, resulting in enhanced sensitivity is proposed and experimentally validated.
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