Aqueous Processable Two-Dimensional Triazine Polymers with Superior Photocatalytic Properties

Area of Science:

• Materials Science
• Polymer Chemistry
• Nanotechnology

Background:

• Scalable production of processable two-dimensional (2D) polymers remains a significant challenge.
• Existing methods often lack efficiency and control over polymer quality and processability.

Purpose of the Study:

• To develop a convenient noncovalent functionalization strategy for producing uniform, aqueous-processable, and semiconducting 2D triazine polymers.
• To investigate the mechanism of exfoliation and the impact of functionalization on material properties and photocatalytic activity.

Main Methods:

• Noncovalent functionalization of bulk crystalline covalent triazine framework (CTF) using aromatic amphiphilic 1-pyrenebutyrate.
• Exfoliation in water facilitated by π-π stacking interactions.
• Characterization of 2D triazine polymer nanosheets and their assembly into aerogels and films.
• Evaluation of photocatalytic hydrogen evolution performance.

Main Results:

• Achieved large-scale exfoliation of CTF into highly water-dispersible single-layer/few-layer 2D triazine polymer nanosheets.
• Demonstrated facile processing into ultralight aerogels and mechanically strong films.
• Observed enhanced photogenerated carrier separation and optimized band structure due to surface molecule doping.
• Reported a remarkable photocatalytic hydrogen evolution rate (1249 μmol h⁻¹) and high apparent quantum efficiency (27.2% at 420 nm).

Conclusions:

• The noncovalent functionalization strategy offers an efficient route to high-quality, processable 2D triazine polymers.
• The developed materials exhibit excellent performance as metal-free photocatalysts for hydrogen evolution.
• This approach significantly advances the potential applications of 2D polymers in sustainable energy technologies.