Prussian Blue Analogue-Derived p-n Junction Heterostructure for Photothermal Reverse Water-Gas Shift: Enhanced...

Area of Science:

• Materials Science
• Catalysis
• Renewable Energy

Background:

• Photothermal catalytic conversion of carbon dioxide (CO2) is crucial for sustainable energy, but efficient catalysts are challenging to develop.
• Developing stable and selective catalysts for CO2 valorization remains a significant hurdle in renewable energy research.

Purpose of the Study:

• To design and synthesize a novel p-n junction heterostructure catalyst for enhanced photothermal CO2 conversion.
• To investigate the catalytic performance, stability, and reaction mechanisms of the engineered heterostructure.

Main Methods:

• Synthesis of a p-n junction heterostructure (T-CZ-PBA (SC)) via controlled pyrolysis of Prussian blue analogues (PBA).
• Integration of CuCo alloy, ZnO, N-doped carbon (NC), and ZnII-CoIII PBA into a synergistic architecture.
• Characterization using in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) to elucidate reaction mechanisms.

Main Results:

• The optimized T-C3Z1-PBA (SC) catalyst achieved a CO2 conversion rate of 126.0 mmol gcat⁻¹ h⁻¹ with 98.8% CO selectivity under light irradiation.
• The catalyst exhibited robust stability, operating continuously for over 50 hours.
• Identification of COOH* as a key intermediate and elucidation of photoexcitation's role in accelerating charge carrier dynamics.

Conclusions:

• The rationally designed p-n junction heterostructure effectively enhances CO2 adsorption, activation, and conversion through optimized interfacial and electronic properties.
• This work provides valuable insights into engineering high-performance catalysts for photothermal CO2 conversion, advancing sustainable energy technologies.