Carbon Black‐Supported Single‐Atom CoNC as an Efficient Oxygen Reduction Electrocatalyst for H2O2 Production in Acidic Media and Microbial Fuel Cell in Neutral Media

Abstract Single metal atom isolated in nitrogen‐doped carbon materials (MNC) are effective electrocatalysts for oxygen reduction reaction (ORR), which produces H 2 O 2 or H 2 O via 2‐electron or 4‐electron process. However, most of MNC catalysts can only present high selectivity for one product, and the selectivity is usually regulated by complicated structure design. Herein, a carbon black‐supported CoNC catalyst (CB@CoNC) is synthesized. Tunable 2‐electron/4‐electron behavior is realized on CB@Co‐N‐C by utilizing its H 2 O 2 yield dependence on electrolyte pH and catalyst loading. In acidic media with low catalyst loading, CB@CoNC presents excellent mass activity and high selectivity for H 2 O 2 production. In flow cell with gas diffusion electrode, a H 2 O 2 production rate of 5.04 mol h −1 g −1 is achieved by CB@CoNC on electrolyte circulation mode, and a long‐term H 2 O 2 production of 200 h is demonstrated on electrolyte non‐circulation mode. Meanwhile, CB@CoNC exhibits a dominant 4‐electron ORR pathway with high activity and durability in pH neutral media with high catalyst loading. The microbial fuel cell using CB@CoNC as the cathode catalyst shows a peak power density close to that of benchmark Pt/C catalyst.