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Title: The effect of tuning the coordination sphere of iron complexes for the oxygen reduction reaction in acidic media
Authors: Wang, Xiaojiang
Zheng, Tianlong
Tang, Yizhao
Li, Xiaoyu
Rykov, Alexandre I.
Li, Xuning
Wang, Junhu
He, Qinggang
Cheng, Jun
Zhang, Xue
Keywords: Engineering::Chemical engineering
Issue Date: 2021
Source: Wang, X., Zheng, T., Tang, Y., Li, X., Rykov, A. I., Li, X., Wang, J., He, Q., Cheng, J. & Zhang, X. (2021). The effect of tuning the coordination sphere of iron complexes for the oxygen reduction reaction in acidic media. Journal of the Electrochemical Society, 168(4), 044506-.
Journal: Journal of the Electrochemical Society
Abstract: As a type of important non-precious catalyst for the oxygen reduction reaction (ORR), the regulating role of a metal centre in metal-macrocycles and other complexes for activity has been extensively studied. However, a common guideline to explain the effect of peripheral coordinated-ligands has not been reached. Herein, a series of organic iron complexes (denoted as FeL, L = TAA, Pc, TPP, Corrole, Tim and Salen) were synthesized as ORR catalysts and an explicit relationship of structure-activity was constructed. The kinetic current density for these compounds was identified to follow the order of FeTAA > FePc > FeTPP > FeCorrole > FeTim > FeSalen. An electron-transfer number close to 4 was derived for all these complexes except for FeTim and FeSalen, implying a near complete reduction of oxygen to water. X-ray absorption near edge structure spectroscopy (XANES) and Mössbauer spectroscopy were used to probe the nature of the distinct activities by investigating the iron-centre electron structures. Density function theory (DFT) calculations were carried out to study the charge redistribution across the iron complexes. Novel activity descriptors including the charge and spin densities on the Fe site were proposed and validated by available experimental data, presenting a strategy to design highly-active nonprecious metal complex catalysts with specific supporting ligands.
ISSN: 0013-4651
DOI: 10.1149/1945-7111/abf21b
Rights: © The Electrochemical Society, Inc. 2021. All rights reserved. Except as provided under U.S. copyright law, this work may not be reproduced, resold, distributed, or modified without the express permission of The Electrochemical Society (ECS). The archival version of this work was published in Journal of The Electrochemical Society, 168(4), 044506-..
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:SCBE Journal Articles

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