期刊
NANO LETTERS
卷 21, 期 19, 页码 8166-8174出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c02623
关键词
Perovskite/spinet catalysts; electronic structure; heterogeneous interfaces; cation deficiencies; d-band center
类别
资金
- Natural Science Foundation of Gansu Province, China [20JR5RA303, 20JR10RA648]
- Fudan University [JIH2203010, IDH2203008/003]
- Education Department of Gansu Province, China [2021CXZX-016]
In this study, a double-cation gradient etching technique was introduced to manipulate the electronic structure of perovskite LaCoO3, resulting in the reconstruction of the surface and the realization of V-LCO/Co3O4. The directional reconstruction of surface electronic structure enhanced the electrocatalytic activity of V-LCO/Co3O4 for the oxygen evolution reaction by adjusting the d-band center to a moderate position with perfect adsorption strength for oxo groups.
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 x 10(21) cm(-3)) compared with LCO (6.03 x 10(19) cm(-3)). Density functional theory (DFT) calculation unveils that the directional reconstruction of surfaceelectronic-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.
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