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g-C3N4 promoted MOF derived hollow carbon nanopolyhedra doped with high density/fraction of single Fe atoms as an ultra-high performance non-precious catalyst towards acidic ORR and PEM fuel cells

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Abstract

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–N4 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 H2/O2 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)–N4–H2O moiety (4.51956 × 1013 sites cm−2) embedded in the carbon framework, identified by in situ X-ray absorption spectroscopy, and the well-balanced micro/meso/macroporous structure.

Graphical abstract: g-C3N4 promoted MOF derived hollow carbon nanopolyhedra doped with high density/fraction of single Fe atoms as an ultra-high performance non-precious catalyst towards acidic ORR and PEM fuel cells

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Publication details

The article was received on 07 Dec 2018, accepted on 31 Jan 2019 and first published on 31 Jan 2019


Article type: Paper
DOI: 10.1039/C8TA11785C
Citation: J. Mater. Chem. A, 2019, Advance Article

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    g-C3N4 promoted MOF derived hollow carbon nanopolyhedra doped with high density/fraction of single Fe atoms as an ultra-high performance non-precious catalyst towards acidic ORR and PEM fuel cells

    Y. Deng, B. Chi, X. Tian, Z. Cui, E. Liu, Q. Jia, W. Fan, G. Wang, D. Dang, M. Li, K. Zang, J. Luo, Y. Hu, S. Liao, X. Sun and S. Mukerjee, J. Mater. Chem. A, 2019, Advance Article , DOI: 10.1039/C8TA11785C

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