Covalently Tethering Atomically Precise Au₂₅ Nanoclusters onto Covalent Organic Framework for Visible-Light-Driven...

Area of Science:

• Materials Science
• Photocatalysis
• Renewable Energy

Background:

• Solar-driven CO2 reduction is key for sustainable fuels but faces challenges like charge recombination and slow kinetics.
• Existing methods often require external photosensitizers and cocatalysts, adding complexity and cost.

Purpose of the Study:

• To develop an integrated photocatalyst for efficient CO2 reduction without external additives.
• To investigate the synergistic effects of atomically precise gold nanoclusters (Au25 NCs) and cobalt complexes within a covalent organic framework (COF).

Main Methods:

• Fabrication of an integrated photocatalyst (TF-COF-CONH-Au25-Co) by immobilizing Au25 NCs onto a COF containing [Co(bpy)3]2+ (Co-N6 coordination).
• Testing the photocatalyst's performance in CO2 conversion to syngas under visible-light illumination.

Main Results:

• Achieved a high CO formation rate of 2,321.9 μmol·g-1·h-1 without external photosensitizers or cocatalysts.
• Demonstrated enhanced light responsiveness and charge transfer efficiency due to Au25 NCs.
• Observed modulation of cobalt sites by Au25 NCs, lowering the energy barrier for CO2 reduction.

Conclusions:

• The integrated TF-COF-CONH-Au25-Co photocatalyst shows high performance for solar CO2 conversion.
• Synergistic integration of metal NCs, COFs, and cobalt complexes offers a promising platform for efficient photocatalysis.