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- Energy; Materials Science; Engineering; C2N; Fe electrocatalyst; Fe@C2N; Encapsulation; Indirect-contact; ORR; Stability
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Converting unstable earth-abundant group VIIIB transition metals into stable catalysts with high oxygen reduction reaction (ORR) performances remains a critical challenge for electrochemical technologies. Iron (Fe)-nitrogen (N)-carbon (C)-based electrocatalysts have recently demonstrated ORR performances comparable to platinum (Pt)-based catalysts. However, as their poor stability remains a critical issue, which needs to be resolved to satisfy commercial requirements. Here, we describe a methodology for preparing a high-performance and stable Fe-based ORR catalyst. The catalyst was obtained by the in-situ sandwiching of a Fe 3+ precursor in a nitrogenated holey two-dimensional network (denoted as C 2 N). Reduction of the sandwiched Fe 3+ results in the formation of Fe oxide (Fe x O y ) nanoparticles, which are simultaneously transformed into highly crystalline Fe 0 nanoparticle cores, while the C 2 N is catalysed into well-defined, encapsulating, nitrogenated graphitic shells (Fe@C 2 N nanoparticles) during heat-treatment. The resultant Fe 0 @C 2 N nanoparticles are uniformly distributed on the C 2 N substrate, becoming the Fe@C 2 N catalyst, which displayed ORR activities superior to commercial Pt/C in both acidic and alkaline media. Furthermore, the Fe@C 2 N catalyst remained rust-free during harsh electrochemical testing even after 650 h, suggesting that its unusual durability originates from indirect-contact electrocatalysis.