Rational Design of Fe1−xS/Fe3O4/Nitrogen and Sulfur‐Doped Porous Carbon with Enhanced Oxygen Reduction Reaction Catalytic Activity

Abstract In this paper, the rational design of Fe‐N‐, Fe‐S‐, and Fe‐N‐S‐based model catalysts for oxygen reduction reaction (ORR), developed using task‐specific hypercrosslinked polymers as precursors is presented. Based on the model catalysts, atom‐induced differences in ORR performance are carefully examined. In the S‐doped carbons, Fe 1− x S forms the metal nanoparticles, while the N sourced together with FeCl 3 ensures the uniform distribution of Fe 3 O 4 . Obtained results indicate that N/Fe 3 O 4 acts as the higher catalytic active site, whereas the S/Fe 1− x S deteriorates the ORR catalytic activity. However, due to the synergistic effect between Fe 1− x S /Fe 3 O 4 and N, the S‐doped carbons can substantially enhance the ORR performance. Hence, this work provides guidance for the efficient design of Fe‐N‐S‐based catalysts for ORR.