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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

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

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【作者】 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

【Author】 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;School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University;Guangxi Key Laboratory of Electrochemical Energy Materials, School of Chemistry and Chemical Engineering, Guangxi University;

【通讯作者】 郑伏琴;樊友军;陈卫;

【机构】 广西师范大学化学与药学院广西大学化学化工学院,广西电化学能源材料重点实验室

【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(MoO43、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(MoO43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了表面富集的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,从而形成了CoFe2O4@CoO@CoOOH紧密的多相结构,起到了“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。

【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(MoO43, 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(Mo O4)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.

【基金】 广西自然科学基金(2019GXNSFGA245003,2021GXNSFBA220058);国家自然科学基金(22002026,22272036);广西科技基地与人才课题(桂科AD23026272);广西师范大学科研基金(2022TD)资助项目~~
  • 【文献出处】 物理化学学报 ,Acta Physico-Chimica Sinica , 编辑部邮箱 ,2024年08期
  • 【分类号】O643.36
  • 【下载频次】6
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