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Issue 19, 2019
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Unraveling the high-activity nature of Fe–N–C electrocatalysts for the oxygen reduction reaction: the extraordinary synergy between Fe–N4 and Fe4N

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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 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 °C, and co-exist 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 exhibit 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 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.

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

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Supplementary files

Article information


Submitted
03 Mar 2019
Accepted
15 Apr 2019
First published
16 Apr 2019

J. Mater. Chem. A, 2019,7, 11792-11801
Article type
Paper

Unraveling the high-activity nature of Fe–N–C electrocatalysts for the 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, 7, 11792
DOI: 10.1039/C9TA02338K

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