Multispatially Localized DNA Walker Coupling Covalent Organic Framework for Dual-Mode Detection of Nucleocapsid Protein Using the Walking-Recycling-Conversion Strategy

Anal Chem. 2024 Nov 19;96(46):18464-18473. doi: 10.1021/acs.analchem.4c03846. Epub 2024 Nov 5.

Abstract

DNA walkers have emerged as a powerful tool in bioanalysis; however, many existing approaches are still restricted by low reaction kinetics and inaccurate single-mode detection. Herein, a fluorescence (FL) and electrochemical (EC) dual-mode biosensor was proposed based on a multispatially localized DNA walker (m-DNA walker) coupling covalent organic framework (COF) using the walking-recycling-conversion strategy. Specifically, the functionalized COF not only served as a three-dimensional nanocarrier but also acted as an effective quencher of the walking tracks. In the presence of the target, the activated m-DNA walker moved fast along the numerous quenching tracks, leading to the cleavage of Cy3-H1 and the recovery of the FL signal. To further improve the detection sensitivity, the Cy3-H1 fragments' recycling process was implemented with the generation of a large amount of S1 and S2, which caused the assembly of DNA-Fe3+-polydopamine network amplifiers on the electrode. The rapid electrochemical conversion was introduced to convert DNA-Fe3+-polydopamine into electroactive Prussian Blue, providing a significant EC signal output. Using nucleocapsid protein (N-protein) as the model target, the designed biosensing platform produced a FL/EC dual-mode readout with the detection limits of 65.0 fg/mL for FL mode and 2.3 fg/mL for EC mode, which could eliminate the interference from different reactive pathways and improve the detection accuracy, holding potential application in early disease diagnosis and treatment.

MeSH terms

  • Biosensing Techniques* / methods
  • Carbocyanines / chemistry
  • DNA* / chemistry
  • Electrochemical Techniques* / methods
  • Electrodes
  • Ferrocyanides / chemistry
  • Indoles
  • Limit of Detection
  • Metal-Organic Frameworks* / chemistry
  • Polymers / chemistry

Substances

  • DNA
  • Metal-Organic Frameworks
  • Polymers
  • polydopamine
  • Carbocyanines
  • Ferrocyanides
  • ferric ferrocyanide
  • cyanine dye 3
  • Indoles