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Unraveling the high-activity nature of Fe-N-C electrocatalysts for oxygen reduction reaction: the extraordinary synergy between Fe-N4 and Fe4N

Abstract

The scarcity and weak durability of precious metal catalysts are among the biggest obstacles to achieving cost-effective electrocatalysts in fuel cells and metal-air batteries. Hence, it is imperative to develop low-cost non-precious metal catalysts with comparable oxygen reduction reaction (ORR) activity to the precious metal catalysts. Herein, we report a highly effective strategy for the facile synthesis of Fe/N-functionalized 3D porous carbon networks. A major advantage of the newly designed catalyst is that ultrafine Fe4N nanoparticles are grown and uniformly mounted on the carbon framework upon pyrolysis treatment at 800 oC, and co-existing with numerous in-situ formed Fe-N4 moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. The new electrocatalysts yield high ORR activity, comparable/superior to that of the state-of-the-art Fe/N-carbon based catalysts reported to date. Specifically, the catalysts show a half-wave potential of 0.890 V (vs. RHE) and a limited current density of 6.18 mA cm-2. By resorting to the experimental measurements and density-functional theory (DFT) calculations, the synergistic effects between Fe-N4 moieties and the Fe4N support are identified for the first time, which play a key role in boosting the catalytic performance of the Fe/N-functionalized porous carbon networks.

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Publication details

The article was received on 03 Mar 2019, accepted on 15 Apr 2019 and first published on 16 Apr 2019


Article type: Paper
DOI: 10.1039/C9TA02338K
Citation: J. Mater. Chem. A, 2019, Accepted Manuscript

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    Unraveling the high-activity nature of Fe-N-C electrocatalysts for oxygen reduction reaction: the extraordinary synergy between Fe-N4 and Fe4N

    X. Ao, W. Zhang, Z. Li, L. Lv, Y. Ruan, H. Wu, W. Chiang, C. Wang, M. Liu and X. C. Zeng, J. Mater. Chem. A, 2019, Accepted Manuscript , DOI: 10.1039/C9TA02338K

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