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DOI10.1039/c9ee03027a
High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst
Zhang N.; Zhou T.; Chen M.; Feng H.; Yuan R.; Zhong C.; Yan W.; Tian Y.; Wu X.; Chu W.; Wu C.; Xie Y.
发表日期2020
ISSN1754-5692
起始页码111
结束页码118
卷号13期号:1
英文摘要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. © 2020 The Royal Society of Chemistry.
语种英语
scopus关键词Aromatic compounds; Catalyst activity; Coordination reactions; Electrocatalysts; Electrolysis; Electrolytic reduction; Electronic structure; Iron; Iron compounds; Nitrogen; Open circuit voltage; Oxygen; Adsorption energies; Coordination catalysts; Coordination structures; High-purity iron; ORR electrocatalysts; Peak power densities; Proton exchange membrane fuel cell (PEMFCs); Reaction selectivity; Proton exchange membrane fuel cells (PEMFC); catalyst; electrokinesis; experimental study; fuel cell; oxygen; reduction
来源期刊Energy and Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/162924
作者单位National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei Anhui, 230029, China; Hefei National Laboratory for Physical Science at the Microscale, IChEM (Collaborative Innovation Center of Chemistry for Energy Materials), CAS Key Laboratory of Mechanical Behavior and Design of Materials, University of Science and Technology of China, Hefei, Anhui, 230026, China; CAS Key Laboratory of Materials for Energy Conversion, Department of Material Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China
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GB/T 7714
Zhang N.,Zhou T.,Chen M.,et al. High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst[J],2020,13(1).
APA Zhang N..,Zhou T..,Chen M..,Feng H..,Yuan R..,...&Xie Y..(2020).High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst.Energy and Environmental Science,13(1).
MLA Zhang N.,et al."High-purity pyrrole-type FeN4 sites as a superior oxygen reduction electrocatalyst".Energy and Environmental Science 13.1(2020).
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