Journal of the American Chemical Society · 2014 · 624 citations · 31 references
Natural SciencesChemical EngineeringChemistryCatalysisElectrochemistryInorganic ChemistryCatalyst CharacterizationCatalyst DesignCatalytic MaterialsOxidation-reduction ReactionsRedox CatalysisRedox-active MaterialsActive Site StructureActive SitesCatalyst Active SitesCatalyst Structure - Activity RelationshipsCatalytic ActivityElectrocatalystsOxygen Reduction CatalystsOxygen Reduction Reaction
High-temperature pyrolyzed FeN(x)/C catalyst is one of the most promising nonprecious metal electrocatalysts for oxygen reduction reaction (ORR). However, it suffers from two challenging problems: insufficient ORR activity and unclear active site structure. Herein, we report a FeN(x)/C catalyst derived from poly-m-phenylenediamine (PmPDA-FeN(x)/C) that possesses high ORR activity (11.5 A g(-1) at 0.80 V vs RHE) and low H2O2 yield (<1%) in acid medium. The PmPDA-FeN(x)/C also exhibits high catalytic activity for both reduction and oxidation of H2O2. We further find that the ORR activity of PmPDA-FeN(x)/C is not sensitive to CO and NO(x) but can be suppressed significantly by halide ions (e.g., Cl(-), F(-), and Br(-)) and low valence state sulfur-containing species (e.g., SCN(-), SO2, and H2S). This result reveals that the active sites of the FeN(x)/C catalyst contains Fe element (mainly as Fe(III) at high potentials) in acid medium.
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An oxygen reduction electrocatalyst based on carbon nanotube–graphene complexes
Yanguang Li, Wu Zhou, Hailiang Wang et al. · Nature Nanotechnology · 2012 · 1.6K citations