A Hypothesis on the Function of High-Valent Fe in NiFe (Hydr)oxide in the Oxygen-Evolution Reaction.

IF 16.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Angewandte Chemie International Edition Pub Date : 2024-11-04 DOI:10.1002/anie.202418798

Nader Akbari, Jafar Hussain Shah, Cejun Hu, Subhajit Nandy, Pavlo Aleshkevych, Rile Ge, Sumbal Farid, Changchang Dong, Liang Zhang, Keun Hwa Chae, Wei Xie, Taifeng Liu, Junhu Wang, Mohammad Mahdi Najafpour

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Abstract

This study investigated the dynamic changes in NiFe (hydr)oxide and identified the role of high-valent Fe in the oxygen-evolution reaction (OER) within alkaline media via in-situ techniques. Several high-valent Fe ions were found to remain considerably stable in the absence of potential in NiFe (hydr)oxide, even 96 hours after the OER. For Ni2+ hydroxide treated with 57Fe ions, where Fe sites are introduced onto the surface of Ni2+ hydroxide, no Fe4+ species were detected at the rate-determining step (RDS). The findings of this study suggested that the oxidation of bulk Fe ions, similar to Ni ions, to high valent forms, is charge accumulation without a direct role in OER; these results offered a novel perspective on manipulating Fe states to optimize OER efficacy. The prevailing hypothesis suggested that trace amounts of high-valent Fe ions, notably those on the surface, directly participate in OER.

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关于镍铁（氢）氧化物中高价铁在氧进化反应中的功能的假设

本研究通过原位技术研究了镍铁（水合）氧化物的动态变化，并确定了高价铁在碱性介质中氧进化反应（OER）中的作用。研究发现，即使在 OER 发生 96 小时后，若干高价铁离子在镍铁（氢）氧化物中无电位的情况下仍相当稳定。对于用 57Fe 离子处理的 Ni2+ 氢氧化物（Fe 位点被引入 Ni2+ 氢氧化物表面），在速率决定步骤 (RDS) 中没有检测到 Fe4+ 物种。这项研究的结果表明，与镍离子类似，块状铁离子氧化成高价形式也是电荷积累，在 OER 中没有直接作用；这些结果为操纵铁离子状态以优化 OER 效能提供了一个新的视角。普遍的假设认为，微量的高价铁离子，特别是表面的铁离子，直接参与了 OER。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Angewandte Chemie International Edition 化学-化学综合

CiteScore

26.60

自引率

6.60%

发文量

3549

审稿时长

1.5 months

期刊介绍： Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.