Solar-Driven CO₂ and H₂O Conversion Over a High-Density Nickel Single-Site Catalyst With Unprecedented CO Evolution...

Area of Science:

• Materials Science
• Catalysis
• Renewable Energy

Background:

• Photothermal catalysis for carbon dioxide (CO2) reduction using water (H2O) is challenging.
• Developing efficient catalysts for solar fuel production is crucial for sustainable energy.

Purpose of the Study:

• To develop a high-density Ni single-site catalyst on a porous aromatic framework (Ni-PAF) for efficient CO2 reduction.
• To investigate the synergistic effects of photothermal conversion and catalysis in the Ni-PAF system.

Main Methods:

• Synthesis of a high-density Ni single-site catalyst anchored on a porous aromatic framework (PAF).
• Photocatalytic CO2 reduction experiments using pure H2O under Xe light and concentrated sunlight.
• Characterization using calculations and experimental data to understand reaction mechanisms.

Main Results:

• Ni-PAF achieved high CO production rates: 25.64 mmol·g-1·h-1 (Xe light) and 229.04 mmol·g-1·h-1 (concentrated sunlight).
• Nitrogen-rich groups facilitated uniform Ni single-site anchoring, acting as active centers for CO2 and H2O activation.
• Synergistic effects of UV-Vis light-driven charge transfer and IR-induced localized heating enhanced CO2 conversion.

Conclusions:

• Ni-PAF demonstrates superior performance for solar-driven CO2 reduction in H2O.
• The catalyst's design offers a new strategy for developing efficient photothermal catalysts.
• This work opens avenues for advanced solar fuel production technologies.