Journal
ANALYTICAL CHEMISTRY
Volume 90, Issue 3, Pages 1506-1510Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.7b04852
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Funding
- National Basic Research Program of China (973 Program) [2015CB932600]
- National Natural Science Foundation of China [21722507, 21605053, 21525523, 21574048]
- National Key R&D Program of China [2017YFA0208000, 2016YFF0100800]
- Fok Ying-Tong Education Foundation of China [151011]
- National Sciences and Engineering Research Council of Canada [2014-06403]
- Canada Research Chair in Bioengineering and Bionanotechnology, Tier II
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Although extensively used in all fields of chemistry, molecular recognition still suffers from a significant limitation: host guest binding displays a fixed, hyperbolic dose response curve, which limits its usefulness in many applications. Here we take advantage of the high programmability of 8) DNA chemistry and propose a universal strategy to engineer biorecognition-based sensors with dual programmable dynamic ranges. Using DNA aptamers as our model recognition element and electrochemistry as our readout signal, we first designed a dual signaling signal-on and signal-off adenosine triphosphate (ATP) sensor composed of a ferrocene-labeled ATP aptamer in complex to a complementary, electrode-bound, methylene-blue labeled DNA. Using this simple dimeric sensor, we show that we can easily (1) tune the dynamic range of this dual-signaling sensor through base mutations on the electrode-bound DNA, (2) extend the dynamic range of this sensor by 2 orders of magnitude by using a combination of electrode-bound strands with varying affinity for the aptamers, (3) create an ultrasensitive dual signaling sensor by employing a sequestration strategy in which a nonsignaling, high affinity depletant DNA aptamer is added to the sensor surface, and (4) engineer a sensor that simultaneously provides extended and ultrasensitive readouts. These strategies, applicable to a wide range of biosensors and chemical systems, should broaden the application of molecular recognition in various fields of chemistry.
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