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通过在铁磁氢氧化镍铁催化剂中预磁化诱导活性位点加速析氧活性

Accelerating Oxygen Evolution Activity via Premagnetization-Induced Active Sites in Ferromagnetic Nickel-Iron Hydroxide Catalysts.

作者信息

Du Xiangbowen, Tan Mingwu, Shi Jichao, Zhang Lili, Qin Xiaojun, Duan Yu, Mao Shanjun, Mushina Selvi, Liu Wen, Wang Yong, Li Renhong

机构信息

School of Materials Science & Engineering, Zhejiang Sci-Tech University, Hangzhou 310018, China.

Department of Chemistry, Zhejiang University, Hangzhou 310013, China.

出版信息

JACS Au. 2025 Jun 2;5(6):2500-2512. doi: 10.1021/jacsau.5c00118. eCollection 2025 Jun 23.

Abstract

Magnetization induced by an external magnetic field has emerged as a potential strategy to enhance the catalytic performance of the oxygen evolution reaction (OER). However, the underlying mechanism, particularly its impact on surface adsorbates, reaction intermediates, and surface reconfiguration, remains unclear. Here we delve into the adsorbate evolution mechanism during the OER catalyzed by ferromagnetic NiFe-hydroxide (LDH-FeOOH) after temporary exposure to a magnetic field (premagnetization, PM). The heterojunction induces crucial interfacial electronic modulation, specifically altering the electronic structure and Ni-O bonding configuration of interfacial Ni sites in the LDH phase, which potentially enhances the magnetic field sensitivity of Ni sites during the premagnetization processes. Following PM treatment, the Tafel slope of LDH-FeOOH significantly decreases from 111.7 to 44.6 mV/dec, indicating the enhancement of catalytic activity. Our investigation reveals that PM improved deprotonation ability induces surface reconstruction, forming highly active high-valenced nickle (oxy)-hydroxide that serves as more possible active sites. Additionally, the PM process promotes to establish a spin conduction channel that optimizes the adsorption energy of key intermediates and enhances spin-oriented electron transfer processes. Furthermore, enhancement of OER kinetics via PM treatment has been validated with both laboratory-scale anion-exchange membrane (AME) eletrcolyzer and industrial-scale commercial alkaline water electrolyzer. This study not only offers new insights into the role of PM in catalyst performance but also highlights its substantial potential for industrial hydrogen production applications.

摘要

由外部磁场诱导的磁化已成为提高析氧反应(OER)催化性能的一种潜在策略。然而,其潜在机制,特别是对表面吸附物、反应中间体和表面重构的影响仍不清楚。在此,我们深入研究了铁磁性氢氧化镍铁(LDH-FeOOH)在临时暴露于磁场(预磁化,PM)后催化OER过程中的吸附物演化机制。异质结引发了关键的界面电子调制,特别是改变了LDH相中界面镍位点的电子结构和Ni-O键构型,这可能增强了预磁化过程中镍位点对磁场的敏感性。经过PM处理后,LDH-FeOOH的塔菲尔斜率从111.7显著降低至44.6 mV/dec,表明催化活性增强。我们的研究表明,PM改善的去质子化能力诱导表面重构,形成高活性的高价镍(氧)氢氧化物,作为更可能的活性位点。此外,PM过程促进建立自旋传导通道,优化关键中间体的吸附能并增强自旋取向的电子转移过程。此外,通过PM处理提高OER动力学已在实验室规模的阴离子交换膜(AME)电解槽和工业规模的商业碱性水电解槽中得到验证。这项研究不仅为PM在催化剂性能中的作用提供了新的见解,还突出了其在工业制氢应用中的巨大潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/fdee/12188396/8733b472b9cd/au5c00118_0001.jpg

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