journal article·2025-07-08Open access

Unleashing Electrocatalytic Oxygen Evolution Activity: Engineering Spin States in Strained Correlated Oxides for Enhanced Performance

Shanquan Chen, Feng-Hui Gong, Xiaowen Li, Yu-Chieh Ku, Cheng-En Liu, Yiyang Nie, Yangyang Si, Shuai Yuan, Jingyu Lu, Hua-Jun Qiu, Kailong Hu, Kaikai Li, Yan Huang, Cheng-Yan Xu, Kelvin Hongliang Zhang, Yun-Long Tang, Lang Chen, Chun-Fu Chang, Zhiwei Hu, Sujit Das, Xiu Liang Ma, Chang-Yang Kuo, Zuhuang Chen

ACS Nano· Volume 19· Issue 26

Abstract

High Resolution Image Download MS PowerPoint Slide 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 3 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 3+ . 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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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Electronic and Structural Properties of Oxides · Advanced Memory and Neural Computing

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Precision Welding and Joining of Materials and Structures, School of Materials Science and Engineering

Harbin Institute of Technology

Shenyang National Laboratory for Materials Science

Institute of Metal Research, Chinese Academy of Sciences

Department of Physics

Southern University of Science and Technology

Department of Electrophysics

National Yang Ming Chiao Tung University

School of Science

State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering

Xiamen University

Max-Planck Institute for Chemical Physics of Solids

Materials Research Centre, Indian Institute of Science

National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, Hsinchu 30076, Taiwan

Flexible Printed Electronics Technology Center

Funding

Science and Technology Foundation of Shenzhen City · Fundamental Research Funds for the Central Universities · National Natural Science Foundation of China · National Science and Technology Council · Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials · State Key Laboratory of Precision Welding and Joining of Materials and Structures

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