Single-Atom-like B-N3 Sites in Ordered Macroporous Carbon for Efficient Oxygen Reduction Reaction

On the premise of cleanliness and stability, improving the catalytic efficiency for the oxygen reduction reaction in the electrode reaction of fuel cells and metal-air batteries is of vital importance. Studies have shown that heteroatom doping and structural optimization are efficient strategies. Herein, a single-atom-like B-N₃ configuration in carbon is designed for efficient oxygen reduction reaction catalysis inspired by the extensively studied transition metal M-N_x sites, which is supported on the ordered macroporous carbon prepared by utilizing a hydrogen-bonded organic framework as carbon and nitrogen sources and SiO₂ spheres as a template. The co-doping of B/N and ordered macroporous structures promote the metal-free material high oxygen reduction catalytic performance in alkaline media. DFT calculations reveal that the B-N₃ structure played a key role in enhancing the oxygen reduction activity by providing rich favorable *OOH and *OH adsorption sites on the B center. The promoted formation of *OH/*OOH intermediates accelerated the electrocatalyst reaction. This study provides new insights into the design of single-atom-like nonmetallic ORR electrocatalysts and synthesis of ordered macroporous carbons based on hydrogen-bonded organic frameworks.