Single‐Nanoparticle Collision Revealing High‐Entropy Suppression of Elemental Segregation in Multi‐Element Alloys During Oxygen Evolution Reaction

五元 合金 材料科学 高熵合金 密度泛函理论 组态熵 化学物理 析氧 拉曼光谱 金属间化合物 电流密度 元素分析 纳米颗粒 结构稳定性 熵(时间箭头) 扫描透射电子显微镜 透射电子显微镜 分子动力学 扫描电子显微镜
作者
Jianan Xu,Han Sun,Furong Cai,Hongyuan Liu,MingLi Hu,Wei Liu,Xiangyi Shan,Wei Yan,Han Gao,Fangyuan Zhao,Min Zhou
出处
期刊:Angewandte Chemie [Wiley]
卷期号:65 (14): e22707-e22707
标识
DOI:10.1002/anie.202522707
摘要

In the oxygen evolution reaction (OER), the structural reconstruction and elemental segregation of alloy catalysts are key factors influencing their activity and stability, while the irreversible structural evolution induced by high current density is the primary issue leading to performance degradation. Herein, we designed a multi-element alloy nanoparticle (MEA-NP) model electrocatalyst from binary (FeIr) to quinary alloy (FeCoNiIrRu), modulating the configuration entropy to explore its influence on structural stability. The single-nanoparticle collision (SNC) based on scanning electrochemical cell microscopy (SECCM) was employed to facilitate efficient mass transfer and ultrahigh current density, thereby accelerating structural evolution during OER. By combining multidimensional feature extraction and clustering analysis of transient signals, it was found that increasing the number of constituent elements improves the structural stability under OER conditions, and high entropy effectively suppresses elemental segregation. Transmission electron microscopy (TEM), in situ Raman spectroscopy, and density functional theory (DFT) calculations further confirmed the advantages of the quinary alloy in terms of structural homogeneity and stability. This study established a statistical correlation between elemental segregation and single-particle transient OER signals, proposed a strategy similar to "accelerated testing under extreme conditions", providing new insights for the mechanistic study and rational design of OER catalysts.
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