Calibration-Free, Seconds-Resolved In Vivo Molecular Measurements using Fourier-Transform Impedance Spectroscopy Interrogation of Electrochemical Aptamer Sensors.
Calibration-Free, Seconds-Resolved In Vivo Molecular Measurements using Fourier-Transform Impedance Spectroscopy Interrogation of Electrochemical Aptamer Sensors.
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DOI：
10.1021/acssensors.3c00632
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发表时间：
2023-08-25
期刊：
影响因子：
8.9
通讯作者：
Sepunaru, Lior
中科院分区：
文献类型：
--
作者：
Roehrich, Brian;Leung, Kaylyn K.;Gerson, Julian;Kippin, Tod E.;Plaxco, Kevin W.;Sepunaru, Lior
基于电化学适体 (EAB) 的传感器能够以几秒的时间分辨率实时测量体内特定分子的浓度。对于其信号转导机制，这些传感器利用其目标识别、氧化还原报告基因修饰适体中结合诱导的构象变化来改变报告基因和支持电极之间的电子转移速率。虽然多种伏安技术已用于监测动力学的这种变化，但它们存在各种缺点，包括时间分辨率仅限于几秒以及需要校准才能消除的传感器与传感器之间的变化。然而，我们在这里表明，使用快速傅里叶变换电化学阻抗谱 (FFT-EIS) 来询问 EAB 传感器可以提高时间分辨率（此处优于 2 秒）和免校准操作，即使此类传感器部署在体内也是如此。为了展示这些好处，我们展示了该方法在活体大鼠静脉中进行实时分子测量的能力。
Electrochemical aptamer-based (EAB) sensors are capable of measuring the concentrations of specific molecules in vivo, in real time, and with a few-second time resolution. For their signal transduction mechanism, these sensors utilize a binding-induced conformational change in their target-recognizing, redox-reporter-modified aptamer to alter the rate of electron transfer between the reporter and the supporting electrode. While a variety of voltammetric techniques have been used to monitor this change in kinetics, they suffer from various drawbacks, including time resolution limited to several seconds and sensor-to-sensor variation that requires calibration to remove. Here, however, we show that the use of fast Fourier transform electrochemical impedance spectroscopy (FFT-EIS) to interrogate EAB sensors leads to improved (here better than 2 s) time resolution and calibration-free operation, even when such sensors are deployed in vivo. To showcase these benefits, we demonstrate the approach’s ability to perform real-time molecular measurements in the veins of living rats.
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