Rational Generation of Fe-Nx Active Sites in Fe- and N-Doped Carbon Electrocatalysts Facilitated by Fe-N Coordinated Precursors for the Oxygen Reduction Reaction
- Rational Generation of Fe-Nx Active Sites in Fe- and N-Doped Carbon Electrocatalysts Facilitated by Fe-N Coordinated Precursors for the Oxygen Reduction Reaction
- 유성종; 장주혁; 김민형; 유지문; 손윤준; 신희종; 강지호; 강윤식; 이국승; 성영은; 안치영
- Issue Date
- VOL 11, NO 24-5988
- Fe？N？C catalysts synthesized by pyrolysis of Fe and N precursors have been intensively studied due to their remarkable activities for the electrochemical oxygen reduction reaction (ORR). Although Fe？N4 coordinated structures have been suggested as active sites by recent spectroscopic studies, the influence of precursor coordination on the generation of the active sites during hightemperature pyrolysis is not well understood. In this work, phenanthroline isomers were used as systematic model precursors to reveal the correlation between precursor coordination and active site formation in Fe？N？C catalysts. Coordination between Fe and each phenanthroline isomer was effectively controlled by the molecular structure: monodentate (1,7 and 4,7phenanthroline) and bidentate coordination (1,10phenanthroline). Through Xray absorption spectroscopy and Xray photoelectron spectroscopy study, large difference in atomic distribution of both Fe and N was revealed; the preferential formation of FeNx active sites was featured only in Fe(1,10phenanthroline)/KB with homogeneously distributed Fe and highly retained pyridinic N. With FeNx active site moieties, Fe(1,10phenanthroline)/KB exhibited superior ORR activity and stability in alkaline halfcell and fullcell tests. These results highlight the importance of the use of precursors with multiple coordination (i.？e. bidentate) for the effective derivation of FeNx active sites for highly active and stable ORR electrocatalysts.
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