Fabrication of electron-acceptor staggered AB Covalent triazine-based frameworks for enhanced visible-light-driven H₂...

Area of Science:

• Materials Science
• Photocatalysis
• Renewable Energy

Background:

• Covalent triazine-based frameworks (CTFs) show potential for photocatalytic water splitting.
• Existing CTFs primarily utilize an AA stacking model for water splitting.
• The influence of stacking models on CTF performance remains underexplored.

Purpose of the Study:

• To synthesize CTF-1 isomers with distinct stacking models (AA and AB).
• To investigate the impact of stacking models on photocatalytic water splitting activity.
• To explore the structure-property relationship between CTF stacking and hydrogen evolution.

Main Methods:

• Synthesis of CTF-1 isomers by controlling reaction temperature.
• Experimental evaluation of photocatalytic hydrogen evolution rates.
• Theoretical calculations to understand electronic structure and reaction mechanisms.
• Photoelectrochemical measurements for water reduction.

Main Results:

• CTF-1 with staggered AB stacking demonstrated significantly higher hydrogen evolution (362 μmol g⁻¹ h⁻¹) compared to AA stacking (70 μmol h⁻¹ g⁻¹).
• AB stacking CTF-1 exhibited superior photocurrent density (77 μA cm⁻²) as a PEC cathode material.
• Theoretical analysis revealed that AB stacking facilitates greater N atom participation in water reduction.

Conclusions:

• Stacking models critically influence the photocatalytic performance of CTFs.
• Staggered AB stacking in CTF-1 enhances hydrogen evolution efficiency.
• This research provides a pathway for designing advanced CTF photocatalysts for water splitting.