Unleashing Electrocatalytic Oxygen Evolution Activity: Engineering Spin States in Strained Correlated Oxides for Enhanced Performance
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 LaCoO<sub>3</sub> 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 Co<sup>3+</sup>. 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.
Authors
- Cheng‐Yan Xu (ORCID: https://orcid.org/0000-0002-7835-6635)
- Zhiwei Hu (ORCID: https://orcid.org/0000-0003-0324-2227)
- Kelvin H. L. Zhang (ORCID: https://orcid.org/0000-0001-9352-6236)
- Chang‐Yang Kuo (ORCID: https://orcid.org/0000-0003-1968-8020)
- C. F. Chang (ORCID: https://orcid.org/0000-0003-1803-2468)
- Yun‐Long Tang (ORCID: https://orcid.org/0000-0001-6555-3296)
- S. Chen
- Sujit Das (ORCID: https://orcid.org/0000-0001-9823-0207)
- Yan Huang (ORCID: https://orcid.org/0000-0003-4841-7262)
- Cheng-En Liu
- Yangyang Si (ORCID: https://orcid.org/0009-0009-7770-4210)
- Feng‐Hui Gong (ORCID: https://orcid.org/0000-0002-0853-0992)
- Kaikai Li (ORCID: https://orcid.org/0000-0003-4237-8696)
- Zuhuang Chen (ORCID: https://orcid.org/0000-0003-1912-6490)
- Hua‐Jun Qiu (ORCID: https://orcid.org/0000-0003-0396-1942)
- Jingyu Lu (ORCID: https://orcid.org/0000-0001-9777-9388)
- Kailong Hu (ORCID: https://orcid.org/0000-0003-0489-5836)
- Shuai Yuan (ORCID: https://orcid.org/0000-0003-2180-3956)
- Yuefeng Nie (ORCID: https://orcid.org/0000-0002-3449-5393)
- Lang Chen (ORCID: https://orcid.org/0000-0003-2460-8232)
- Xiaowen Li
- Xiu Liang (ORCID: https://orcid.org/0000-0002-6591-5178)
- Yu‐Chieh Ku
Institutions
- National Yang Ming Chiao Tung University (TW)
- Xiamen University (CN)
- Chinese Academy of Sciences (CN)
- Harbin Institute of Technology (CN)
- Southern University of Science and Technology (CN)
- National Synchrotron Radiation Research Center (TW)
- Max Planck Institute for Chemical Physics of Solids (DE)
- Division of Materials Science and Engineering (AU)
- Welding Science (Brazil) (BR)
- Printed Electronics (United Kingdom) (GB)
- Indian Institute of Science Bangalore (IN)
Publication Details
- Journal
- ACS Nano
- Published
- 2025-06-13
- DOI
- https://doi.org/10.1021/acsnano.5c02188
- Citations
- 5
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 1.82
Funders
- Science and Technology Foundation of Shenzhen City
- National Natural Science Foundation of China
- National Science and Technology Council
- Fundamental Research Funds for the Central Universities