Interfacial electronic structure regulation has been shown to be beneficial for a variety of electrocatalytic reactions. However, integrating foreign species into anion vacancy defect electrocatalysts, and investigating their interfacial electron structure and synergistic catalytic effect are still somewhat controversial. Herein, Fe₂O₃/NiSe₂ and Fe₂O₃/Ni₃S₂ heterostructures catalysts with abundant anion defects (Se, S) were constructed through an efficient spatial combination of primary hydroxide nanosheets. The Fe₂O₃/NiSe₂ and Fe₂O₃/Ni₃S₂ catalysts exhibited outstanding electrocatalytic activities, as shown by the overpotentials of 200 mV at 100 mA cm⁻² for OER, and 60 mV at 10 mA cm⁻² for HER, respectively. The Fe₂O₃/NiSe₂ (anode)‖Fe₂O₃/Ni₃S₂ (cathode) device accelerated water splitting at 1.54 V with 10 mA cm⁻², surpassing the integrated couple of Pt and Ir-based oxide (1.57 V). The chemical valence state, combined with DFT calculations, revealed that interface engineering and anion defects could modulate the electronic structures of the Fe₂O₃ modified NiSe₂ and Ni₃S₂ catalysts, reduce the energy barrier of intermediate, and therefore dramatically improve their catalytic performances. This work not only presents a universal strategy for the construction of active and durable electrocatalyst with abundant anion defects, but also provides a new way for the rational design of novel nanostructure for electrocatalytic applications.

已经表明界面电子结构调节对于多种电催化反应是有益的。然而，将异种掺入阴离子空位缺陷电催化剂中，并研究它们的界面电子结构和协同催化作用仍存在一定争议。在此，通过伯羟基氢氧化物纳米片的有效空间组合，构造了具有丰富的阴离子缺陷（Se，S）的Fe ₂ O ₃ / NiSe ₂和Fe ₂ O ₃ / Ni ₃ S ₂异质结构催化剂。Fe ₂ O ₃ / NiSe ₂和Fe ₂ O ₃/ Ni ₃ S ₂催化剂表现出优异的电催化活性，如分别由OER在100 mA cm ^-2处200 mV和HER在10 mA cm ^-2处60 mV的过电势所示。中的Fe ₂ ö ₃ / NISE ₂（阳极）‖Fe ₂ ö ₃ /镍₃小号₂（阴极）装置加速水在1.54 V分裂与10毫安厘米^-2，超越了集成夫妇Pt和Ir基丙烷（ 1.57 V）。化学价态结合DFT计算表明，界面工程和阴离子缺陷可以调节Fe ₂的电子结构O ₃改性的NiSe ₂和Ni ₃ S ₂催化剂降低了中间体的能垒，因此大大提高了它们的催化性能。这项工作不仅为构建具有丰富阴离子缺陷的活性持久电催化剂提供了一种通用策略，而且为合理设计用于电催化应用的新型纳米结构提供了一种新途径。