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High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst

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Abstract

Atomically dispersed iron–nitrogen (FeN4) catalysts have emerged as the most promising alternative to costly Pt-based counterparts in proton exchange membrane fuel cells (PEMFCs), but often they suffer from high overpotential and poor stability due to the diverse iron–nitrogen coordination structure. Herein, we demonstrate high-purity pyrrole-type FeN4 sites for the first time, as a superior ORR electrocatalyst for PEMFCs. The high-purity pyrrole-type FeN4 catalyst exhibited extremely outstanding ORR activity with an ultra-high active area current density of 6.89 mA m−2 in acid medium, which exceeds that of most reported metal–nitrogen coordination catalysts. Experimental and theoretical analyses reveal that high-purity pyrrole-type coordination significantly modifies the atomic and electronic structures of FeN4 sites, bringing with it high intrinsic catalytic activity, preferable O2 adsorption energy and full four-electron reaction selectivity for ORR catalysis. Therefore, PEMFCs built with this high-purity FeN4 catalyst achieve a high open-circuit voltage (1.01 V) and a large peak power density (over 700 mW cm−2). High-purity iron–nitrogen coordination would give new insights into highly efficient electrocatalysts for PEMFCs.

Graphical abstract: High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst

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Publication details

The article was received on 18 Sep 2019, accepted on 22 Nov 2019 and first published on 23 Nov 2019


Article type: Communication
DOI: 10.1039/C9EE03027A
Energy Environ. Sci., 2020, Advance Article

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    High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst

    N. Zhang, T. Zhou, M. Chen, H. Feng, R. Yuan, C. Zhong, W. Yan, Y. Tian, X. Wu, W. Chu, C. Wu and Y. Xie, Energy Environ. Sci., 2020, Advance Article , DOI: 10.1039/C9EE03027A

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