Dual-Single-Atom Tailoring with Bifunctional Integration for High-Performance CO₂ Photoreduction

Area of Science:

• Materials Science
• Catalysis
• Photochemistry

Background:

• Single-atom photocatalysis is a promising strategy for heterogeneous reactions.
• Integrating multiple single-atom functionalities into dual-single-atom catalysts presents a significant challenge.
• Optimizing cooperative effects in dual-single-atom systems is crucial for enhanced photocatalytic activity.

Purpose of the Study:

• To develop and investigate dual-single-atom catalysts for efficient photocatalytic CO2 reduction.
• To elucidate the structure-performance correlations and synergistic effects between different single-atom species.
• To demonstrate the potential of rationally designed dual-single-atom catalysts in sustainable energy applications.

Main Methods:

• Synthesis of dual-single-atom catalysts (Cobalt and Ruthenium) supported on conjugated porous carbon nitride polymer.
• In situ characterizations to analyze catalyst structure and intermediates.
• Theoretical calculations to understand reaction mechanisms and electronic properties.
• Photocatalytic CO2 reduction experiments to evaluate performance.

Main Results:

• The developed dual-single-atom catalyst effectively reduces CO2 via photocatalysis.
• Cobalt sites facilitate dynamic charge transfer, while Ruthenium sites enhance CO2 surface interaction.
• Achieved an apparent quantum efficiency (AQE) of 2.8% at 385 nm and a turnover number (TON) > 200 without sacrificial agents.
• Demonstrated synergistic effects between Cobalt and Ruthenium single atoms.

Conclusions:

• Dual-single-atom catalysts can be designed to integrate specific metal functionalities for improved photocatalysis.
• The synergistic interaction between Cobalt and Ruthenium atoms significantly enhances CO2 photoreduction performance.
• This work provides insights into regulating cooperative photocatalysis for efficient CO2 conversion.