期刊
ACS SENSORS
卷 3, 期 2, 页码 360-366出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssensors.7b00787
关键词
aptamer; chronoamperometry; in vivo; E-AB; electrochemical sensors; precision medicine
资金
- Natural Sciences and Engineering Research Council of Canada
- Postdoctoral Program of the Basque Government
- Institute for Collaborative Biotechnologies through U.S. Army Research Office [W911NF-09- 0001]
- Defense Advanced Research Projects Agency (DARPA) Biological Technologies Office (BTO) Electrical Prescriptions (ElectRx) program through the DARPA Contracts Management Office [HR001117C0122]
- Otis Williams Postdoctoral Fellowship of the Santa Barbara Foundation
Electrochemical, aptamer-based (E-AB) sensors support the continuous, real-time measurement of specific small molecules directly in situ in the living body over the course of many hours. They achieve this by employing binding-induced conformational changes to alter electron transfer from a redox-reporter-modified, electrode-attached aptamer. Previously we have used voltammetry (cyclic, alternating current, and square wave) to monitor this binding-induced change in transfer kinetics indirectly. Here, however, we demonstrate the potential advantages of employing chronoamperometry to measure the change in kinetics directly. In this approach target concentration is reported via changes in the lifetime of the exponential current decay seen when the sensor is subjected to a potential step. Because the lifetime of this decay is independent of its amplitude (e.g., insensitive to variations in the number of aptamer probes on the electrode), chronoamperometrically interrogated E-AB sensors are calibration free and resistant to drift. Chronoamperometric measurements can also be performed in a few hundred milliseconds, improving the previous few-second time resolution of E-AB sensing by an order of magnitude. To illustrate the potential value of the approach we demonstrate here the calibration-free measurement of the drug tobramycin in situ in the living body with 300 ms time resolution and unprecedented, few-percent precision in the determination of its pharmacokinetic phases.
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