Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 7, Issue 9, Pages 5020-5030Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8ta11785c
Keywords
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Funding
- National Key Research and Development Program of China [2017YFB0102900, 2016YFB0101201]
- National Natural Science Foundation of China (NSFC) [21476088, 21776105, 21805034]
- Guangdong Provincial Department of Science and Technology [2015B010106012]
- Guangzhou Science Technology and Innovation Committee [201504281614372, 2016GJ006]
- NSLS-II, Brookhaven National Laboratory, under U.S. DOE Contract [DE-SC0012704]
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We report a hollow carbon nanopolyhedron catalyst doped with N and single Fe atoms, prepared by pyrolyzing hollow ZIF-8 with ferric acetylacetonate and g-C3N4. The catalyst retains the polyhedral morphology of its precursor and possesses exclusively Fe-N-4 moieties promoted by g-C3N4 nitriding, evidenced by multipronged microscopic and spectroscopic analyses. In rotating disk measurements, the catalyst exhibits superior ORR activity in both acidic and alkaline media, with a half-wave potential of 0.78 V in the former and 0.845 V in the latter. In addition, its ORR stability surpasses that of commercial Pt/C in acidic and alkaline media. Most notably, the catalyst exhibits ultra-high performance in a H-2/O-2 proton exchange membrane fuel cell (PEMFC), with a current density of 400 mA cm(-2) at 0.7 V and 133 mA cm(-2) at 0.8 V, and a maximum power density of 628 mW cm(-2). This is among the best PEMFC performances reported for cathodes free of platinum-group metals. We attribute this excellent-ORR activity to the integration of the high density Fe(ii)-N-4-H2O moiety (4.51956 x 10(13) sites cm(-2)) embedded in the carbon framework, identified by in situ X-ray absorption spectroscopy, and the well-balanced micro/meso/macroporous structure.
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