One-Dimensional Covalent Organic Framework with Improved Charge Transfer for Enhanced Electrochemiluminescence

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• Electrochemical luminescence (ECL) is a powerful analytical technique.
• Developing novel materials to enhance ECL performance is crucial for advanced sensing applications.
• Covalent organic frameworks (COFs) offer tunable properties for various applications.

Purpose of the Study:

• To design and synthesize a one-dimensional pyrene-based covalent organic framework (1D-COF).
• To investigate the effect of the 1D-COF structure on electrochemiluminescence (ECL) properties.
• To explore the application of 1D-COF in ECL biosensing.

Main Methods:

• Synthesis of a 1D-COF with a dual-chain-like edge architecture.
• Characterization of the 1D-COF's structural and electronic properties.
• Electrochemical and ECL measurements using tripropylamine (TPrA) and K2S2O8 as coreactants.
• Density Functional Theory (DFT) calculations to understand the mechanism of ECL enhancement.
• Fabrication of an ECL biosensor for dopamine detection.

Main Results:

• The 1D-COF exhibits enhanced anodic (92.5-fold) and cathodic (3.2-fold) ECL signals compared to 2D-COF.
• Anodic and cathodic ECL efficiencies of 1D-COF are 2.08- and 3.08-fold higher than 2D-COF, respectively.
• DFT analysis indicates that the 1D-COF structure restrains intramolecular spin, reducing nonradiative transitions and enhancing ECL.
• The 1D-COF demonstrates sensitive detection of dopamine in an ECL biosensor.

Conclusions:

• The dimensional regulating charge transfer strategy using 1D-COF effectively enhances ECL.
• The unique architecture of 1D-COF plays a key role in improving ECL performance.
• 1D-COF holds great promise for developing highly sensitive ECL biosensors.