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Dual-Reporter Drift Correction To Enhance the Performance of Electrochemical Aptamer-Based Sensors in Whole Blood

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Department of Chemistry and Biochemistry, University of California—Santa Barbara, Santa Barbara, California 93106, United States
Center for Bioengineering, University of California—Santa Barbara, Santa Barbara, California 93106, United States
§ Department of Chemistry, University of Rome, Tor Vergata, Via della Ricerca Scientifica, 00133, Rome, Italy
Consorzio Interuniversitario Biostrutture e Biosistemi “INBB”, Rome 00136, Italy
Cite this: J. Am. Chem. Soc. 2016, 138, 49, 15809–15812
Publication Date (Web):November 6, 2016
Copyright © 2016 American Chemical Society

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    The continuous, real-time monitoring of specific molecular targets in unprocessed clinical samples would enable many transformative medical applications. Electrochemical aptamer-based (E-AB) sensors appear to be a promising approach to this end because of their selectivity (performance in complex samples, such as serum) and reversible, single-step operation. E-AB sensors suffer, however, from often-severe baseline drift when challenged in undiluted whole blood. In response we report here a dual-reporter approach to performing E-AB baseline drift correction. The approach incorporates two redox reporters on the aptamer, one of which serves as the target-responsive sensor and the other, which reports at a distinct, nonoverlapping redox potential, serving as a drift-correcting reference. Taking the difference in their relative signals largely eliminates the drift observed for these sensors in flowing, undiluted whole blood, reducing drift of up to 50% to less than 2% over many hours of continuous operation under these challenging conditions.

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