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Free keywords:
NITROGEN-DOPED CARBON; IRON-BASED CATALYSTS; FE-57
MOSSBAUER-SPECTROSCOPY; PEM FUEL-CELL; OXYGEN REDUCTION; METAL
ELECTROCATALYST; IDENTIFICATION; COORDINATION; NANOPARTICLES; CHEMISTRY
Abstract:
Fe-N-C catalysts with high O-2 reduction performance are crucial for displacing Pt in low-temperature fuel cells. However, insufficient understanding of which reaction steps are catalyzed by what sites limits their progress. The nature of sites were investigated that are active toward H2O2 reduction, a key intermediate during indirect O-2 reduction and a source of deactivation in fuel cells. Catalysts comprising different relative contents of FeNxCy moieties and Fe particles encapsulated in N-doped carbon layers (0-100%) show that both types of sites are active, although moderately, toward H2O2 reduction. In contrast, N-doped carbons free of Fe and Fe particles exposed to the electrolyte are inactive. When catalyzing the ORR, FeNxCy moieties are more selective than Fe particles encapsulated in N-doped carbon. These novel insights offer rational approaches for more selective and therefore more durable Fe-N-C catalysts.
