Reconstructing the surface-electronic-structure of catalysts for efficient electrocatalytic activity is crucial but still under intense exploration. Herein, we introduce a double-cation gradient etching technique to manipulate the electronic structure of perovskite LaCoO. With the gradient dissolution of cations, the surface was reconstructed, and the perovskite/spinel heterostructure V-LCO/CoO (V-LCO refers to LaCoO with La and Co vacancies) can be realized. Its surface-electronic-structure is effectively regulated due to the heterogeneous interface effect and abundant vacancies, resulting in a significantly enhanced activity for oxygen evolution reaction (OER). The V-LCO/CoO exhibits low electrochemical activation energy and 2 orders of magnitude higher carrier concentrations (1.36 × 10 cm) compared with LCO (6.03 × 10 cm). Density functional theory (DFT) calculation unveils that the directional reconstruction of surface-electronic-structure enables the -band center of V-LCO/CoO to a moderate position, endowing perfect adsorption strength for oxo groups and thus promoting the electrocatalytic activity.
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