Three-dimensional porous nitrogen-doped carbon nanosheets with ultra-high surface area for high-performance oxygen reduction reaction electrocatalysts

A series of three-dimensional (3D) porous nitrogen-doped carbon nanosheets (PNCNs) have been successfully fabricated via a high-pressure carbonization followed by high-temperature thermal treatment. With the prolonging of thermal treatment time, the 3D PNCNs demonstrate several remarkable advantages for oxygen reduction reaction (ORR) electrocatalysts, including ultra-high specific surface area (more than 2100 m2/g-1), unique 3D porous structure, abundant defects, and suitable configuration of nitrogen. With these merits, the N-C2 h based electrocatalyst exhibits outstanding ORR activities with a comparable onset potential of -40 mV (vs. Ag/AgCl), half-wave potential of -120 mV (vs. Ag/AgCl), satisfactory electron transfer number (4) and superior stability to those of commercial 20% Pt/C. The excellent electrochemical behaviors of 3D PNCNs are confirmed to be dominated by structural characteristics, which can be optimized by varying thermal treatment time. Our work offers a promising way for controllably constructing carbon-based materials with optimized ORR performance.