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DOI | 10.1039/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 |
ISSN | 1754-5692 |
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 |
推荐引用方式 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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