Active Sites Engineering toward Superior Carbon-Based Oxygen Reduction Catalysts via Confinement Pyrolysis

Developing efficient and low-cost defective carbon-based catalysts for the oxygen reduction reaction (ORR) is essential to metal-air batteries and fuel cells. Active sites engineering toward these catalysts is highly desirable but challenging to realize boosted catalytic performance. Herein, a sandwich-like confinement route to achieve the controllable regulation of active sites for carbon-based catalysts is reported. In particular, three distinct catalysts including metal-free N-doped carbon (NC), single Co atoms dispersed NC (Co-N-C), and Co nanoparticles-contained Co-N-C (Co/Co-N-C) are controllably realized and clearly identified by synchrotron radiation-based X-ray spectroscopy. Electrochemical measurements suggest that the Co/Co-N-C catalyst delivers optimized ORR performance due to the rich Co-N_x active sites and their synergistic effect with metallic Co nanoparticles. This work provides deep insight for rationally designing efficient ORR catalyst based on active sites engineering.