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Electrochromic, Closed-Bipolar Electrodes Employing Aptamer-Based Recognition for Direct Colorimetric Sensing Visualization

Cite this: Anal. Chem. 2019, 91, 17, 11467–11473
Publication Date (Web):August 8, 2019
https://doi.org/10.1021/acs.analchem.9b03013
Copyright © 2019 American Chemical Society

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    Abstract

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    In this paper, we adapt the electrochemical, aptamer-based (E-AB) sensor platform to develop colorimetric aptamer-based sensors using a closed-bipolar electrode (C-BPE) system. The C-BPE E-AB sensors provide quantitative detection of target molecules based on the rate of color change of an electrochromic Prussian blue (PB) thin-film indicator electrode. The C-BPE cathode, or sensing electrode, is modified with a redox-labeled aptamer that binds to a specific target. More specifically, we employed sequences specific for adenosine triphosphate (ATP) and tobramycin as test-bed targets because these sequences are well vetted. The C-BPE anode, or indicator electrode, was coated with an electrochromic thin film comprising Prussian white (PW) that, when reduced to PB, is accompanied by a corresponding color change used for analytical detection. The rate of color change from PW to PB is facilitated by a potassium ferricyanide-catalyzed oxidation of leucomethylene blue (LB) to methylene blue (MB), the redox label conjugated to the aptamer on the sensing electrode. We demonstrate that the rate of color change is quantitatively related to the concentration of target analyte, which provides a means for naked eye determination. When combined with smartphone-based colorimetric detection, these C-BPE E-AB sensors present a user-friendly alternative to traditional E-AB sensors that rely on voltammetric analysis and a potentiostat, opening up the possibility of point-of-use applications.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.analchem.9b03013.

    • Additional information about the reset potential for conversion of PB to PW, the driving voltages of C-BPE E-AB sensors for conversion of PW to PB, the color change using different buffer solutions, photographs of the devices with and without ATP and K3[Fe(CN)6], optimization of the aptamer concentration used in surface modification of the sensing electrode, and photographs of C-BPE E-AB sensors used for titrations for both ATP and tobramycin E-AB sensors (PDF)

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