Electrochemical reduction for modulating spin state of nickel: A pathway to improved water and seawater oxidation

IF 3.5 2区物理与天体物理 Q2 PHYSICS, APPLIED

Applied Physics Letters Pub Date : 2025-01-28 DOI:10.1063/5.0250893

Yu Shuai, Shucheng Liu, Tao Zhang, Yi Liu

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引用次数: 0

Abstract

Understanding the electronic structure of catalysts is crucial for analyzing electrocatalyst behavior. Here, we present a straightforward method to modify the electronic configuration of active sites in nickel-iron-niobium layered double hydroxides (NiFeNb-LDHs) via electrochemical reduction (ER), uncovering key factors that enhance oxygen evolution reaction (OER) activity. The results indicate that ER-NiFeNb-LDHs display excellent OER performance and long-term stability over 60 h in various electrolytes (271.99 mV@50 mA cm−2 in 1M KOH and 280.56 mV@50 mA cm−2 in 1M KOH +0.5M NaCl). Furthermore, the cell voltage of the two-electrode electrolyzer ER-NiFeNb-LDHs ǁ Pt/C achieves a current density of 50 mA cm−2 at an ultra-low voltage of 1.58 V, significantly outperforming the commercial RuO2ǁPt/C. X-ray absorption spectroscopy, magnetic characterization, and density functional theory calculations reveal that the unsaturated coordination environment created by ER modifies the electronic state distribution between eg and t2g orbitals, effectively lowering the spin state of nickel and enhancing its OER activity.

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来源期刊

Applied Physics Letters 物理-物理：应用

CiteScore

6.40

自引率

10.00%

发文量

1821

审稿时长

1.6 months

期刊介绍： Applied Physics Letters (APL) features concise, up-to-date reports on significant new findings in applied physics. Emphasizing rapid dissemination of key data and new physical insights, APL offers prompt publication of new experimental and theoretical papers reporting applications of physics phenomena to all branches of science, engineering, and modern technology. In addition to regular articles, the journal also publishes invited Fast Track, Perspectives, and in-depth Editorials which report on cutting-edge areas in applied physics. APL Perspectives are forward-looking invited letters which highlight recent developments or discoveries. Emphasis is placed on very recent developments, potentially disruptive technologies, open questions and possible solutions. They also include a mini-roadmap detailing where the community should direct efforts in order for the phenomena to be viable for application and the challenges associated with meeting that performance threshold. Perspectives are characterized by personal viewpoints and opinions of recognized experts in the field. Fast Track articles are invited original research articles that report results that are particularly novel and important or provide a significant advancement in an emerging field. Because of the urgency and scientific importance of the work, the peer review process is accelerated. If, during the review process, it becomes apparent that the paper does not meet the Fast Track criterion, it is returned to a normal track.