物理化学学报 >> 2024, Vol. 40 >> Issue (8): 2308003.doi: 10.3866/PKU.WHXB202308003

所属专题： 电催化功能材料

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双金属浸出诱导催化剂重构用于高活性和高稳定性电化学水氧化

许文涛1, 莫栩妍1, 周洋1, 翁祖贤1, 莫坤玲1, 吴炎桦1, 蒋欣霖1, 李丹1, 蓝汤淇1, 文欢2, 郑伏琴1,*(), 樊友军1,*(), 陈卫1,*()   

  1. 1 广西师范大学化学与药学学院, 广西 桂林 541004
    2 广西大学化学化工学院, 广西电化学能源材料重点实验室, 南宁 530004
  • 收稿日期:2023-08-01 修回日期:2023-09-22 录用日期:2023-09-22 发布日期:2023-10-09
  • 通讯作者: Email: fqzheng@mailbox.gxnu.edu.cn (郑伏琴)youjunfan@mailbox.gxnu.edu.cn (樊友军)weichen@gxnu.edu.cn (陈卫)
  • 基金资助:
    广西自然科学基金(2019GXNSFGA245003); 广西自然科学基金(2021GXNSFBA220058); 国家自然科学基金(22002026); 国家自然科学基金(22272036); 广西师范大学科研基金(GUIKE AD23026272); 广西师范大学科研基金(2022TD)

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

Wentao Xu1, Xuyan Mo1, Yang Zhou1, Zuxian Weng1, Kunling Mo1, Yanhua Wu1, Xinlin Jiang1, Dan Li1, Tangqi Lan1, Huan Wen2, Fuqin Zheng1,*(), Youjun Fan1,*(), Wei Chen1,*()   

  1. 1 School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University, Guilin 541004, Guangxi, China
    2 Guangxi Key Laboratory of Electrochemical Energy Materials, School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China
  • Received:2023-08-01 Revised:2023-09-22 Accepted:2023-09-22 Published:2023-10-09
  • Contact: Email: fqzheng@mailbox.gxnu.edu.cn (Fuqin Zheng)youjunfan@mailbox.gxnu.edu.cn (Youjun Fan)weichen@gxnu.edu.cn (Wei Chen)
  • Supported by:
    the Natural Science Foundation of Guangxi, China(2019GXNSFGA245003); the Natural Science Foundation of Guangxi, China(2021GXNSFBA220058); the National Natural Science Foundation of China(22002026); the National Natural Science Foundation of China(22272036); the Guangxi Technology Base and Talent Subject, China(GUIKE AD23026272); the Guangxi Normal University Research Grant, China(2022TD)

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摘要：

析氧反应(OER)催化剂在催化反应过程中不可避免地会发生表面重构，这一过程使得设计、构筑高性能和高稳定性的OER电催化剂充满挑战。在此，我们采用双金属浸出诱导表面重构的策略，构建了高活性和高稳定性的水氧化电催化剂。在该策略中，通过水热、离子交换和后续的退火工艺处理，将由α-CoMoO4、K2Co2(MoO4)3、Co3O4和CoFe2O4四种氧化物晶相组成的材料阵列转换为OER预催化剂。原位电化学拉曼光谱和非原位X射线衍射(XRD)分析表明，其中的不稳定成分K2Co2(MoO4)3的快速溶解引发了Mo和K的适度浸出，从而在低电压下加速表面富集的α-Co(OH)2向CoOOH活性相的转化。此外，CoFe2O4相耦合重构产生新相CoO与无定形层CoOOH，从而形成CoFe2O4@CoO@CoOOH紧密的多相结构，起到“纳米栅栏”的作用，可有效防止催化剂的过度重构，从而赋予重构后的催化剂优异的催化活性和稳定性。本工作为设计高电流密度下具有优异活性和稳定性的OER催化剂提供了新的思路。

关键词: 析氧反应, 表面重构, 离子浸出, 水分解, 电催化, 催化剂

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.

Key words: Oxygen evolution reaction, Surface reconstruction, Ion leaching, Water splitting, Electrocatalysis, Catalyst