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Updated: Jun 15, 2025

Applying Dynamic Strain on Thin Oxide Films Immobilized on a Pseudoelastic Nickel-Titanium Alloy
Published on: July 28, 2020
Unleashing Electrocatalytic Oxygen Evolution Activity: Engineering Spin States in Strained Correlated Oxides for
Shanquan Chen1, Feng-Hui Gong2, Xiaowen Li3
1State Key Laboratory of Precision Welding and Joining of Materials and Structures, School of Materials Science and Engineering, Harbin Institute of Technology, Shenzhen 518055, China.
None:
Perovskite oxides have emerged as compelling contenders for catalyzing the oxygen evolution reaction (OER) due to their low cost, high efficiency, and structural flexibility. Nevertheless, unraveling the intricate structure-activity relationships within correlated oxides remains challenging, impeding the rational design of efficient catalysts. Here, using LaCoO3 epitaxial thin films as a model system, we illustrate a direct correlation between the spin state and OER activity. Through comprehensive investigations via X-ray absorption spectroscopy, scanning transmission electron microscopy, and first-principles calculations, we pinpoint that the enhanced OER activity observed in the tensile-strained films originates from lattice oxygen oxidation triggered by strain-engineered high-spin Co3+. Particularly, the high-spin sites correlated oxygen vacancies during OER lead the reaction into a new pathway, facilitating both the deprotonation of OH* at the metal site and the formation of O-O bonds at the oxygen redox center. Our findings reveal the intricate interplay among strain, spin-state transition, and the transformation of OER mechanism, providing valuable insights for correlated oxide electrocatalysts.
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