Bimetal Leaching Induced Reconstruction of Water Oxidation Electrocatalyst for Enhanced Activity and Stability

IF 13.5 2区化学 Q1 CHEMISTRY, PHYSICAL 物理化学学报 Pub Date : 2024-08-01 DOI:10.3866/PKU.WHXB202308003

Wentao Xu , Xuyan Mo , Yang Zhou , Zuxian Weng , Kunling Mo , Yanhua Wu , Xinlin Jiang , Dan Li , Tangqi Lan , Huan Wen , Fuqin Zheng , Youjun Fan , Wei Chen

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Abstract

Surface reconstruction inevitably occurs during pre-catalysis for the oxygen evolution reaction (OER); however, obtaining OER electrocatalysts with high performance and stability remains a challenge. In this study, we have developed a bimetallic leaching-induced surface reconstruction strategy to fabricate efficient electrocatalysts for water oxidation. Microcolumn arrays consisting of α-CoMoO₄, K₂Co₂(MoO₄)₃, Co₃O₄, and CoFe₂O₄ four-phase oxides were integrated as pre-catalyst by a hydrothermal, ion-exchange, and subsequent annealing process. In situ Raman spectroelectrochemical and ex situ X-ray diffraction (XRD) studies revealed that the rapid dissolution of the unstable component K₂Co₂(MoO₄)₃ triggered the adaptive leaching of Mo and K, which accelerated the transformation of the surface-enriched α-Co(OH)₂ to the active phase of CoOOH at low voltage. Furthermore, the stable CoFe₂O₄ component couples the reconfigured new phase CoO with the amorphous layer CoOOH to form a compact hierarchical structure of CoFe₂O₄@CoO@CoOOH, which plays the role of a nanofence and effectively prevents the catalyst from over-reconstruction, thus achieving excellent catalytic stability. This work provides a novel idea for designing OER catalysts with excellent activity and stability at high current densities.

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双金属浸出诱导水氧化电催化剂活性和稳定性增强的重构

摘要在析氧反应（OER）的预催化过程中，表面重构是不可避免的；然而，获得高性能稳定的OER电催化剂仍然是一个挑战。在这项研究中，我们开发了一种双金属浸出诱导表面重建策略来制造高效的水氧化电催化剂。由α-CoMoO4、K2Co2(MoO4)3、Co3O4和CoFe2O4四相氧化物组成的微柱阵列通过水热、离子交换和随后的退火工艺作为预催化剂进行集成。原位拉曼光谱电化学和非原位x射线衍射（XRD）研究表明，不稳定组分K2Co2(MoO4)3的快速溶解引发了Mo和K的自适应浸出，加速了表面富集的α-Co(OH)2在低压下向CoOOH的活性相转变。此外，稳定的CoFe2O4组分将重新配置的新相CoO与非晶层CoOOH偶联，形成致密的层次化结构CoFe2O4@CoO@CoOOH，起到纳米屏障的作用，有效地防止了催化剂的过度重构，从而获得了优异的催化稳定性。本研究为设计在高电流密度下具有良好活性和稳定性的OER催化剂提供了新的思路。

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