Rapid electron transfer via dynamic coordinative interaction boosts quantum efficiency for photocatalytic CO₂...

Area of Science:

• Photocatalysis
• Green Chemistry
• Materials Science

Background:

• Achieving high quantum efficiency in photocatalytic CO2 reduction is a significant challenge.
• Dynamic attachment between photosensitizers and catalysts is crucial for improving efficiency.

Purpose of the Study:

• To develop a strategy for dynamic attachment between photosensitizers and catalysts using coordinate bonds.
• To enhance the quantum efficiency and selectivity of photocatalytic CO2 reduction.

Main Methods:

• Utilized a pyridine-appended iridium photosensitizer and molecular catalysts.
• Employed 1H nuclear magnetic resonance titration, theoretical calculations, and spectroscopic measurements for mechanistic studies.
• Investigated the effect of modified cobalt phthalocyanine on catalytic performance.

Main Results:

• Achieved a quantum efficiency of 10.2% ± 0.5% for CO2 to CO conversion using an unmodified cobalt phthalocyanine catalyst.
• Demonstrated over a 4-fold increase in efficiency compared to systems without dynamic interaction.
• Optimized quantum efficiency to 27.9% ± 0.8% with amino group-decorated cobalt phthalocyanine due to enhanced coordination.
• Confirmed the importance of dynamic coordination for catalyst applicability.

Conclusions:

• Dynamic coordination bonds between photosensitizers and catalysts are effective for enhancing photocatalytic CO2 reduction.
• This approach significantly improves quantum efficiency and selectivity.
• The strategy shows wide applicability for various non-noble-metal catalysts.