Journal
SMALL
Volume 19, Issue 22, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202300758
Keywords
electrocatalysis; Fe-N-C; graphitization; oxygen reduction reaction; stability
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An effective phase-transition strategy is reported to enhance the stability of Fe-N-C catalysts, while preserving their activity, by increasing the graphitization degree and incorporating Fe nanoparticles encapsulated by a graphitic carbon layer. The resulting Fe@Fe-N-C catalysts exhibit excellent oxygen reduction reaction (ORR) activity and stability, making them promising alternatives to platinum group metals.
Fe single atoms and N co-doped carbon nanomaterials (Fe-N-C) are the most promising oxygen reduction reaction (ORR) catalysts to replace platinum group metals. However, high-activity Fe single-atom catalysts suffer from poor stability owing to the low graphitization degree. Here, an effective phase-transition strategy is reported to enhance the stability of Fe-N-C catalysts by inducing increased degree of graphitization and incorporation of Fe nanoparticles encapsulated by graphitic carbon layer without sacrificing activity. Remarkably, the resulted Fe@Fe-N-C catalysts achieved excellent ORR activity (E-1/2 = 0.829 V) and stability (19 mV loss after 30K cycles) in acid media. Density functional theory (DFT) calculations agree with experimental phenomena that additional Fe nanoparticles not only favor to the activation of O-2 by tailoring d-band center position but also inhibit the demetallization of Fe active center from FeN4 sites. This work provides a new insight into the rational design of highly efficient and durable Fe-N-C catalysts for ORR.
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