Abstract
AbstractIron‐nitrogen‐carbon (Fe‐N‐C) composites have emerged as active and non‐precious‐metal electrocatalysts for the oxygen reduction reaction (ORR). Here, we developed a simple process to synthesize FeOx nanoclusters (NCs) incorporated with iron phthalocyanine (FePc) supported on graphene (FeOx/FePc) as highly active electrocatalysts for the ORR by a self‐assembly method. The electrochemical activity of FeOx/FePc depends on the loading or size of the FeOx NCs. The best results are obtained on FeOx/FePc with 10 wt % FeOx NCs of a size of approximately 2 nm and a thickness of approximately 0.6 nm, which achieves a half‐wave potential of 0.888 V and current density of 37.6 Ag−1 at 0.9 V (vs. the reversible hydrogen electrode). This is 50 mV higher than that of FePc supported on graphene and 64 mV higher than that of Pt/C in 0.1 m KOH solution at a catalyst loading of 0.1 mg cm−2. X‐ray absorption spectroscopy and electrochemical cyclic voltammetry results indicate that the incorporated FeOx NCs interact with the active center of FePc, Fe−N4, to enhance the electron transition and reversibility of the FeIII/FeII redox couple and promote the kinetics of the ORR. We demonstrate that the nature of the active center of FePc (i.e., Fe−N4) is related closely to the activity of the FeIII/FeII redox couple.
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