Department of Biomedical Engineering, Northwestern University, Evanston, IL, 60208, USA.
Simpson Querrey Institute, Northwestern University, Chicago, IL, 60611, USA.
Nat Commun. 2023 Mar 25;14(1):1665. doi: 10.1038/s41467-023-37402-2.
Electrochemical aptamer-based sensors are typically deployed as individual, passive, surface-functionalized electrodes, but they exhibit limited sensitivity especially when the area of the electrode is reduced for miniaturization purposes. We demonstrate that organic electrochemical transistors (electrolyte gated transistors with volumetric gating) can serve as on-site amplifiers to improve the sensitivity of electrochemical aptamer-based sensors. By monolithically integrating an Au working/sensing electrode, on-chip Ag/AgCl reference electrode, and Poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) counter electrode - also serving as the channel of an organic electrochemical transistor- we can simultaneously perform testing of organic electrochemical transistors and traditional electroanalytical measurement on electrochemical aptamer-based sensors including cyclic voltammetry and square-wave voltammetry. This device can directly amplify the current from the electrochemical aptamer-based sensor via the in-plane current modulation in the counter electrode/transistor channel. The integrated sensor can sense transforming growth factor beta 1 with 3 to 4 orders of magnitude enhancement in sensitivity compared to that in an electrochemical aptamer-based sensor (292 μA/dec vs. 85 nA/dec). This approach is believed to be universal, and can be applied to a wide range of tethered electrochemical reporter-based sensors to enhance sensitivity, aiding in sensor miniaturization and easing the burden on backend signal processing.
基于电化学适体的传感器通常被部署为单个、无源、表面功能化的电极,但它们的灵敏度有限,特别是当为了小型化目的而减小电极面积时。我们证明,有机电化学晶体管(具有体积门控的电解质门控晶体管)可以作为现场放大器,以提高基于电化学适体的传感器的灵敏度。通过将 Au 工作/传感电极、片上 Ag/AgCl 参比电极和聚(3,4-亚乙基二氧噻吩)-聚(苯乙烯磺酸盐)对电极(也用作有机电化学晶体管的通道)单片集成,我们可以同时对有机电化学晶体管和传统电化学分析测量进行测试,包括循环伏安法和方波伏安法。该器件可以通过在对电极/晶体管通道中的平面电流调制直接放大来自基于电化学适体的传感器的电流。与基于电化学适体的传感器(292 μA/dec 对 85 nA/dec)相比,集成传感器可以以 3 到 4 个数量级的灵敏度增强来检测转化生长因子 β1。这种方法被认为是通用的,可以应用于广泛的基于连接的电化学报告器传感器,以提高灵敏度,有助于传感器小型化并减轻后端信号处理的负担。