Journal
SMALL METHODS
Volume 5, Issue 12, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smtd.202101072
Keywords
electrochemical nanosensors; gatekeeper DNA; host-guest assemblies; porous redox particles; ratiometric detection
Funding
- National Natural Science Foundation of China (NSFC) [51773022, 21734002]
- Graduate Research and Innovation Foundation of Chongqing [CYB21071]
- 100 Talents Program of Chongqing University
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This study developed a host-guest assembly strategy to build redox nanosensors for immobilization-free and ratiometric electrochemical detection system. By utilizing miRNA triggering and NIR irradiation, the system achieved highly repeatable detection of miRNA, providing a new direction for the design of advanced electrochemical biosensors.
Electrochemical nanosensors by integrating functional nucleic acids and nanomaterials hold a great promise in the fast detection of biomarkers, yet the current systems possess limitations on the accessibility of target-probe and probe-electrode interactions and the repeatability of detection. Herein, a host-guest assembly strategy is developed to build redox nanosensors for an immobilization-free and ratiometric electrochemical detection system. Specifically, electroactive molecule (E-m) guests are loaded in porous hosts of polydopamine nanoparticles (MPDA) to act as dual-signal redox reporters. Hybrid DNA probes of G-quadruplex and a single-stranded anchor DNA are installed as gatekeepers for sealing the mesopores. Thereby, miRNA triggered E-m release by strand displacement reactions and the homogeneous transportation of the hosts/guests to the electrode facilitate the generation of reference signal/response signal at different potentials. Concomitantly applied NIR irradiation boosts the electron transfer from MPDA to the electrode and results in a tenfold increase in the reference signal. Finally, the sensing system through the differential pulse voltammetry method achieves a highly repeatable detection (relative standard deviation 3.8%) of miRNA with a lower detection limit (362 x 10(-15) m). This attractive system paves the way for rational designs of advanced electrochemical biosensors and smart diagnosis.
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