析氧
离解(化学)
分解水
电解质
催化作用
电化学
化学
分子
化学工程
质子输运
无机化学
电极
物理化学
膜
有机化学
光催化
生物化学
工程类
作者
Liqing Wu,Wenxia Huang,Dongyang Li,Hongnan Jia,Bingbing Zhao,Juan Zhu,Haiqing Zhou,Wei Luo
标识
DOI:10.1002/anie.202413334
摘要
Understanding the structure and dynamic process of interfacial water molecules at the catalyst‐electrolyte interface on acidic oxygen evolution reaction (OER) kinetics is highly desirable for the development of proton exchange membrane water electrolyzers. Herein, we construct a series of p‐block metallic elements (Ga, In, Sn) doped RuO2 catalysts with manipulated electronic structure and Ru‐O covalency to investigate the effect of electrochemical interfacial engineering on the improvement of acidic OER activity. Associated with operando attenuated total reflectance surface‐enhanced infrared absorption spectroscopy measurements and theoretical analysis, we uncover the free‐H2O enriched local environment and dynamic evolution from 4‐coordinated hydrogen‐bonded water and 2‐coordinated hydrogen‐bonded water to free‐H2O on the surface of Ga‐RuO2, are responsible for the optimized connectivity of hydrogen bonding network in the electrical double layer by promoting solvent reorganization. In addition, the structurally ordered interfacial water molecules facilitate high‐efficiency proton‐coupled electron transfer across the interface, leading to reduced energy barrier of the follow‐up dissociation process and enhanced acidic OER performance. This work highlights the key role of structure and dynamic process of interfacial water for acidic OER, and demonstrates the electrochemical interfacial engineering as an efficient strategy to design high‐performance electrocatalysts.
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