A covalent organic framework with asymmetric coordination for the oxygen reduction reaction: a computational study

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• The oxygen reduction reaction (ORR) is crucial for energy conversion technologies.
• Developing efficient electrocatalysts for ORR remains a significant challenge.

Purpose of the Study:

• To identify novel materials for efficient oxygen reduction.
• To investigate the catalytic activity of covalent organic frameworks (COFs) for ORR.

Main Methods:

• First-principles calculations using density functional theory (DFT).
• Microkinetic modeling.
• Electronic structure analysis.

Main Results:

• A covalent organic framework with an asymmetric CoN2O2 active site was identified.
• The material exhibits remarkable ORR activity with a theoretical half-wave potential of 0.98 V.
• Electronic structure analysis revealed that the asymmetric coordination modulates charge redistribution, enhancing oxygen species activation.

Conclusions:

• Asymmetric coordination environments in COFs can significantly boost ORR performance.
• The identified COF is a promising candidate for ORR electrocatalysis.
• Computational methods are effective for designing high-performance electrocatalysts.