Oxygen-Molecule Adsorption and Dissociation on BCN Graphene: A First-Principles Study

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Boron and nitrogen co-doped (BCN) graphene is a promising metal-free electrocatalyst.
• Its unique structure and electronic properties are key to its catalytic activity.

Purpose of the Study:

• To determine the structure of the active oxygen dissociation site in BCN graphene.
• To investigate the influence of different boron-nitrogen (BN) cluster types on catalytic activity.

Main Methods:

• Density functional theory (DFT) calculations were employed.
• Analysis of electronic structure and energy barriers for O2 dissociation.

Main Results:

• The edge termination and shape of BN clusters significantly impact BCN graphene's catalytic activity.
• N-terminated triangular BN clusters are more effective than B-terminated or quadrangular clusters.
• A B atom adjacent to an N-terminated triangular BN cluster exhibits the lowest O2 dissociation energy barrier (0.08 eV).

Conclusions:

• The B atom next to an N-terminated triangular BN cluster is the most active site for O2 dissociation.
• Enhanced catalytic activity is linked to positive charge density and increased density of π* states near the Fermi level.