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Surface-Electronic-Structure Reconstruction of Perovskite via Double-Cation Gradient Etching for Superior Water
Jingyan Zhang1, Junfu Li1, Chenglin Zhong2,3
1Key Laboratory for Magnetism and Magnetic Materials of MOE, Key Laboratory of Special Function Materials and Structure Design of MOE, Lanzhou University, Lanzhou 730000, China.
Abstract:
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 LaCoO3. With the gradient dissolution of cations, the surface was reconstructed, and the perovskite/spinel heterostructure V-LCO/Co3O4 (V-LCO refers to LaCoO3 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/Co3O4 exhibits low electrochemical activation energy and 2 orders of magnitude higher carrier concentrations (1.36 × 1021 cm-3) compared with LCO (6.03 × 1019 cm-3). Density functional theory (DFT) calculation unveils that the directional reconstruction of surface-electronic-structure enables the d-band center of V-LCO/Co3O4 to a moderate position, endowing perfect adsorption strength for oxo groups and thus promoting the electrocatalytic activity.
