Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) modified metal-organic frameworks boosting carbon dots electrochemiluminescence emission for sensitive miRNA detection

Abstract

Highly efficient luminescent materials play an important role in electrochemiluminescence (ECL) biosensing systems. Herein, the poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) modified carbon dots (CDs)/zeolitic imidazolate framework-8 (ZIF-8) compositing metal-organic frameworks (MOFs) materials with excellent luminescence performance were prepared as the ECL emitters for biosensing application. In this novel ternary composites, CDs were used as emitters, ZIF-8 was used as a carrier, and the luminescent performance was finally improved by introducing PEDOT:PSS to improve the conductivity of the nanomaterials. As a result, CDs/PEDOT:PSS/ZIF-8 exhibited an approximately 8 times ECL intensity compared to CDs alone. By further modifying with AuNPs, the enhancement factor reached ≈10 in reference to the individual CDs. After combining with a DNAzyme-based two-cycle target amplification principle, an ECL biosensor was constructed to achieve high-sensitivity detection of miRNA-21 with a detection limit of 50 aM. The biosensor also demonstrated desirable selectivity, excellent stability, and quantitative ability for human serum target detection. Overall, these findings not only provide a promising pathway for high luminous efficiency ECL emitters synthesis, but also provide a platform for ultrasensitive miRNA sensing.