Engineering the Local Electronic Microenvironment via Interfacial Chelation for Efficient CO₂ Photoreduction Toward...

Area of Science:

• Materials Science
• Photocatalysis
• Renewable Energy

Background:

• Photocatalytic conversion of CO2 into hydrocarbons using solar energy is key for energy crisis and carbon neutrality.
• Conventional p-block photocatalysts show inefficient electron transfer, limiting CO2 reduction to CO and hindering high-value hydrocarbon formation.
• Developing efficient photocatalysts is crucial for selective CO2 reduction to valuable products like methane.

Purpose of the Study:

• To design and synthesize a novel BiOCl-BiO(HCOO) heterostructure (BiOCH) for efficient photocatalytic CO2 reduction to CH4.
• To investigate the role of interfacial chelating interactions and electronic modulation in enhancing photocatalytic activity.
• To explore the potential of organic-inorganic hybrid layered structures for selective CO2 conversion.

Main Methods:

• Synthesis of a novel BiOCl-BiO(HCOO) heterostructure (BiOCH).
• Characterization of the heterostructure's properties, including light absorption and charge separation.
• Mechanistic studies to understand the role of interfacial Bi-O chelation in the CO2 reduction pathway.
• Evaluation of photocatalytic performance for CO2 to CH4 conversion, including production rate and electron selectivity.

Main Results:

• The BiOCH heterostructure exhibits broadened light absorption and enhanced photoinduced charge separation.
• Interfacial Bi-O chelation in BiO(HCOO) modulates the electronic structure, facilitating the *CO to *CHO conversion step.
• The optimized BiOCH catalyst achieved a CH4 production rate of 42.95 µmol·g−1·h−1 with 95.38% electron selectivity.
• Demonstrated efficient photocatalytic CO2 reduction to methane, a high-value hydrocarbon.

Conclusions:

• The novel BiOCH organic-inorganic hybrid layered structure effectively promotes photocatalytic CO2 reduction to CH4.
• Interfacial chelating interactions and electronic modulation are critical for enhancing catalytic activity and selectivity.
• This work presents a promising strategy for designing advanced photocatalysts for sustainable energy applications and carbon neutrality.