Atomic-Scale Charge Channelling in Poly(triazine imide) With Cooperative Ti-Ru Sites for Efficient Visible-Light CO₂...

Area of Science:

• Materials Science
• Photocatalysis
• Renewable Energy

Background:

• Solar-to-chemical energy conversion via photocatalytic CO2 reduction is promising but limited by inefficient catalysts.
• Existing catalysts struggle with directing charge flow and synchronizing redox kinetics for water splitting and CO2 reduction.

Purpose of the Study:

• To develop an atomic-scale charge-channelling photocatalyst for efficient solar-driven CO2 reduction.
• To investigate a spatially cooperative strategy using Ti single atoms and Ru species on poly(triazine imide) (PTI).

Main Methods:

• Fabrication of a composite photocatalyst with lattice-substituted Ti and anchored Ru species on crystalline PTI.
• Utilizing spectroscopic investigations and theoretical calculations to elucidate reaction mechanisms.
• Evaluating catalytic performance for CO2 reduction to CO using H2O as the electron donor.

Main Results:

• The optimized Ti-Ru/PTI catalyst achieved a CO evolution rate of 281.0 µmol g⁻¹ h⁻¹ with high stability.
• Ti species facilitated visible-light absorption and hole extraction for water oxidation.
• Photogenerated electrons were channeled to Ru sites for CO2 reduction, establishing vectorial charge separation.

Conclusions:

• The developed photocatalyst effectively suppresses charge recombination through spatially coupled charge transport.
• This strategy provides mechanistic insights into artificial photosynthesis and offers a pathway for designing high-performance catalysts.
• The complementary roles of Ti and Ru sites are crucial for efficient carrier utilization and reaction energetics.