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Bio-inspired FeN5 moieties anchored on a three-dimensional graphene aerogel to improve oxygen reduction catalytic performance

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Abstract

Transition-metal-coordinated nitrogen-doped carbon (M-N-C) materials have been regarded as the most promising oxygen reduction reaction (ORR) catalysts. However, the ambiguity of the exact active sites seriously hampered the understanding of the structure–performance correlation and the further activity improvement of M-N-C catalysts. Herein, we designed and synthesized a three-dimensional graphene aerogel (GA) supported FeN5 composite with an explicit five-coordinated Fe–N bond. In this composite, pyridine groups were covalently grafted on the graphene surface to anchor iron phthalocyanine (FePc) molecules (FePc/AP-GA). The ORR performance of this catalyst showed a half-wave potential of −0.035 V (vs. Hg/HgO) in an alkaline electrolyte, which surpassed those of the benchmark Pt/C and most pyrolyzed or non-pyrolyzed nonprecious metal catalysts. Additionally, the FePc/AP-GA composite also exhibited a high kinetic current density of 20.01 mA cm−2 at −0.1 V, good durability, and high tolerance to methanol poisoning effects. X-ray absorption spectroscopy results revealed that the five-coordinated Fe–N bond dominated in the FePc/AP-GA composite with an elongated bond length. This geometric and electronic structure of the iron atom in the FePc/AP-GA composite is believed to facilitate the adsorption of O2 and intermediates and thus to enhance ORR activity and durability. Our results provided a promising target active site for the rational design of highly efficient M-N-C catalysts for fuel cells and metal–air batteries.

Graphical abstract: Bio-inspired FeN5 moieties anchored on a three-dimensional graphene aerogel to improve oxygen reduction catalytic performance

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Publication details

The article was received on 05 Jul 2018, accepted on 04 Sep 2018 and first published on 04 Sep 2018


Article type: Paper
DOI: 10.1039/C8TA06455E
Citation: J. Mater. Chem. A, 2018, Advance Article
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    Bio-inspired FeN5 moieties anchored on a three-dimensional graphene aerogel to improve oxygen reduction catalytic performance

    J. Huang, Q. Lu, X. Ma and X. Yang, J. Mater. Chem. A, 2018, Advance Article , DOI: 10.1039/C8TA06455E

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