Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution  

作　　者：Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang 

机构地区：[1]Key Laboratory of Green Chemical Engineering Process of Ministry of Education,Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education,Hubei Key Laboratory of Novel Reactor and Green Chemical Technology,School of Chemical Engineering&Pharmacy,Wuhan Institute of Technology,Wuhan 430205,Hubei,China [2]Key Laboratory of Pesticide&Chemical Biology of Ministry of Education,Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education,College of Chemistry,Central China Normal University,Wuhan 430079,Hubei,China [3]College of Materials Science and Engineering,Fuzhou University,Fuzhou 350108,Fujian,China

出　　处：《Journal of Energy Chemistry》2025年第1期226-233,共8页能源化学(英文版)

基　　金：National Natural Science Foundation of China(22478310,U21A20286 and 22206054)。

摘　　要：Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction(OER).Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process.However,most of them undergo incomplete reconstruction with limited thickness of reconstruction layer,leading to low component utilization and arduous exploration of real catalytic mechanism.Herein,we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER.The hollow phytic acid(PA)cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability,in favor of the fast and complete reconstruction.A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co(Fe)(OH)xand subsequent potential-driven oxidation to Co(Fe)OOH.The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm^(-2)and a long-term stability.The experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity.The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关 键 词：Complete reconstruction Co-based complex PRECATALYSTS Oxygen evolution reaction 

分 类 号：TQ116.2[化学工程—无机化工] O643.36[理学—物理化学]