Abstract

Understanding the origin of high activity of Fe–N–C electrocatalysts in oxygen reduction reaction (ORR) is critical but still challenging for developing efficient non-precious metal catalysts in fuel cells and metal-air batteries. Herein, we developed Fe-based ORR catalysts containing highly dispersed interfaces of Fe2N/Fe3C and revealed the origin of its activity by intensively investigating the structure of the catalysts and their correlations with the electrochemical performance. It was found that the Fe2N/Fe3C with a well-matched interface displays a half-wave potential of 0.764 V (vs. RHE) and high current density in acidic electrolytes. In addition, the H2–O2 fuel cell assembled using Fe2N/Fe3C as the cathode exhibits excellent performance with a peak power density of 713 mW/cm−1. The experimental and computational results reveal that the interface of the Fe2N/Fe3C heterojunction is essential for the ORR in acidic electrolytes because it provides a remarkable decrease in the maximum free energy change of O∗ protonation to OH∗.

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