Abstract
The development of efficient non-noble metal catalysts is critical for advancing sustainable fuel-cell technologies. This study investigates the effect of carbon support microstructure on the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts. By precisely tuning the pyrolysis temperature of activated carbon (AC) between 600 and 1000 °C, we elucidate the mechanistic influence of the physicochemical characteristics of the carbon support on the ORR activity of the supported catalyst. Increasing the pyrolysis temperature enhanced the electrical conductivity of the carbon support, thereby improving the ORR performance of the catalyst. However, while the defect density and specific surface area of the carbon support initially increased with increasing pyrolysis temperature, they declined when elevated temperatures were used (e.g., 1000 °C), leading to reduced ORR activity. The AC-900 support, pyrolyzed at 900 °C, exhibited an optimal balance of a high surface area, abundant defects, and superior conductivity. An Fe phthalocyanine/AC-900 catalyst synthesized using the AC-900 support exhibited excellent ORR activity (E(1/2): 0.89 V and E(on): 0.95 V vs. reversible hydrogen electrode (RHE)) in 0.1 M KOH. This work highlights the pivotal role of carbon support microstructure in governing the ORR activity of the supported catalyst and provides a rational strategy for designing high-performance non-noble metal electrocatalysts.