Interfacial engineering is an effective strategy for the design of active oxygen evolution electrode. Yet the intrinsic mechanism of heterogeneous interfaces remains largely unclear for the lack of direct evidence of real active phases. Herein, operando ultraviolet-visible (UV–vis) and Raman spectroscopies were used to probe the surface reconstruction behaviors of FeOOH@NiFe layered double hydroxides (LDH) hybrid catalysts, which revealed that FeOOH@NiFe LDH was converted into highly active FeOOH@ β-Ni(Fe)OOH phases during the OER process. The FeOOH-NiFe LDH interface can promote interfacial charge transfer, delay the Ni oxidation and induce the NiFe LDH phases to highly reactive β-Ni(Fe)OOH. The FeOOH@ β-Ni(Fe)OOH exhibited excellent OER performance (252 mV at 100 mA cm⁻²) and a 1.6 times increase (at overpotential of 300 mV) in turnover frequency (TOF) with respect to the active phase γ-Ni(Fe)OOH of NiFe LDH. This work clarifies that ration interface engineering can regulate the generation of highly active phases in the OER process.

界面工程是设计活性析氧电极的有效策略。然而，由于缺乏真实活性相的直接证据，异质界面的内在机制在很大程度上仍不清楚。在此，使用紫外-可见（UV-vis）和拉曼光谱对FeOOH@NiFe层状双氢氧化物（LDH）杂化催化剂的表面重建行为进行了研究，结果表明FeOOH@NiFe LDH转化为高活性FeOOH@β -OER 过程中的 Ni(Fe)OOH 相。FeOOH-NiFe LDH界面可以促进界面电荷转移，延缓Ni氧化并将NiFe LDH相诱导为高活性的β-Ni(Fe)OOH。FeOOH@β-Ni(Fe)OOH 表现出优异的 OER 性能（252 mV at 100 mA cm ^-2) 并且相对于 NiFe LDH 的活性相 γ-Ni(Fe)OOH，转换频率 (TOF) 增加了 1.6 倍（在 300 mV 的过电势下）。这项工作阐明了日粮界面工程可以调节 OER 过程中高活性相的产生。