Donor-Acceptor MOF Enabling Efficient Electrochemiluminescence Based on TSCT-TADF

Area of Science:

• Materials Science
• Chemistry
• Physical Chemistry

Background:

• Electrochemiluminescence (ECL) is vital for studying surface energy states and charge transfer mechanisms.
• Developing novel luminescent materials with efficient ECL is crucial for advanced applications.

Purpose of the Study:

• To demonstrate thermally activated delayed fluorescence (TADF) via spatial charge transfer in donor-acceptor metal-organic frameworks (D-A MOFs).
• To investigate the synthesis and enhanced ECL properties of these hybrid materials.

Main Methods:

• Precise synthesis of luminescent materials by incorporating phenyl-carbazole derivatives as donor guests within acceptor-hosted MOFs.
• Utilizing Density Functional Theory (DFT) calculations to elucidate charge transfer mechanisms.
• Tuning guest molecule dihedral angles to optimize π-π interactions.

Main Results:

• Hybrid D-A MOF structures exhibited significantly higher ECL intensities than monomeric counterparts.
• DFT calculations confirmed efficient intermolecular through-spatial charge transfer (TSCT) due to the spatially proximate D-A configuration.
• Modulation of guest molecule structure enhanced π-π interactions and ECL performance.

Conclusions:

• The study presents a novel strategy for modulating spatial charge transfer at the molecular level.
• Programmable synthesis of D-A MOFs offers a pathway to design highly efficient ECL luminophores.
• This approach enhances ECL performance through controlled intermolecular interactions.