Microstructure and Microenvironment Regulation of Covalent Organic Frameworks for Electrochemical CO₂ Reduction...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Growing energy crisis and environmental concerns drive research into electrochemical CO2 reduction (eCO2RR).
• Covalent organic frameworks (COFs) show promise for CO2 conversion due to tunable structures.
• Current COF research for eCO2RR focuses on macroscopic properties, neglecting microstructural influences.

Purpose of the Study:

• To review advances in optimizing COF-based materials for eCO2RR through microstructure and microenvironment engineering.
• To highlight strategies for tuning active sites, including charge distribution and adsorbed species concentration.
• To provide insights for designing next-generation COF electrocatalysts.

Main Methods:

• Ligand engineering to tune local electron density and charge distribution.
• Linkage engineering to modify COF structures.
• Substituent effects to enhance catalytic activity.
• Analysis of anion and cation adsorption on active sites to steer reaction pathways.

Main Results:

• Microstructure and microenvironment engineering significantly impact COF performance in eCO2RR.
• Precise control over charge distribution and adsorbed species concentration enhances catalytic activity.
• Selective ion adsorption influences intermediate adsorption energy and reaction pathways.

Conclusions:

• Engineering the microstructure and microenvironment of COFs is crucial for efficient eCO2RR.
• Strategies like ligand and linkage engineering offer pathways to improved COF electrocatalysts.
• Further research into ion effects and rational design is needed for advanced COF catalysts.