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

引用本文: 许文涛, 莫栩妍, 周洋, 翁祖贤, 莫坤玲, 吴炎桦, 蒋欣霖, 李丹, 蓝汤淇, 文欢, 郑伏琴, 樊友军, 陈卫. 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[J]. 物理化学学报, 2024, 40(8): 230800. doi: 10.3866/PKU.WHXB202308003 shu

Citation: 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. Bimetal Leaching Induced Reconstruction of Water Oxidation Electrocatalyst for Enhanced Activity and Stability[J]. Acta Physico-Chimica Sinica, 2024, 40(8): 230800. doi: 10.3866/PKU.WHXB202308003 shu

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.
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

通讯作者: 郑伏琴, fqzheng@mailbox.gxnu.edu.cn; 樊友军, youjunfan@mailbox.gxnu.edu.cn; 陈卫, weichen@gxnu.edu.cn

基金项目:
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

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:

English

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

Wentao Xu ^1, ,
Xuyan Mo ^1, ,
Yang Zhou ^1, ,
Zuxian Weng ^1, ,
Kunling Mo ^1, ,
Yanhua Wu ^1, ,
Xinlin Jiang ^1, ,
Dan Li ^1, ,
Tangqi Lan ^1, ,
Huan Wen ^2, ,
Fuqin Zheng ^{1,
,} ,
Youjun Fan ^{1,
,} ,
Wei Chen ^{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

Corresponding author: Email: fqzheng@mailbox.gxnu.edu.cn (F.Z.); Email: youjunfan@mailbox.gxnu.edu.cn (Y.F.); Email: weichen@gxnu.edu.cn (W.C.)

Received Date: 01 August 2023
Accepted Date: 22 September 2023
Revised Date: 22 September 2023
Available Online: 15 August 2024
Fund Project:
the Natural Science Foundation of Guangxi, China

the Natural Science Foundation of Guangxi, China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the Guangxi Technology Base and Talent Subject, China

the Guangxi Normal University Research Grant, China

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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1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: 郑伏琴, fqzheng@mailbox.gxnu.edu.cn; 樊友军, youjunfan@mailbox.gxnu.edu.cn; 陈卫, weichen@gxnu.edu.cn

English

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

Corresponding author: Email: fqzheng@mailbox.gxnu.edu.cn (F.Z.); Email: youjunfan@mailbox.gxnu.edu.cn (Y.F.); Email: weichen@gxnu.edu.cn (W.C.)

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

通讯作者: 郑伏琴, fqzheng@mailbox.gxnu.edu.cn; 樊友军, youjunfan@mailbox.gxnu.edu.cn; 陈卫, weichen@gxnu.edu.cn

English

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

Corresponding author: Email: fqzheng@mailbox.gxnu.edu.cn (F.Z.); Email: youjunfan@mailbox.gxnu.edu.cn (Y.F.); Email: weichen@gxnu.edu.cn (W.C.)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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