Operando Identification of the Dynamic Behavior of Oxygen Vacancy-Rich Co 3 O 4 for Oxygen Evolution Reaction
Abstract
The exact role of a defect structure on transition metal compounds for electrocatalytic oxygen evolution reaction (OER), which is a very dynamic process, remains unclear. Studying the structure-activity relationship of defective electrocatalysts under operando conditions is crucial for understanding their intrinsic reaction mechanism and dynamic behavior of defect sites. Co 3 O 4 with rich oxygen vacancy (V O ) has been reported to efficiently catalyze OER. Herein, we constructed pure spinel Co 3 O 4 and V O -rich Co 3 O 4 as catalyst models to study the defect mechanism and investigate the dynamic behavior of defect sites during the electrocatalytic OER process by various operando characterizations. Operando electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) implied that the V O could facilitate the pre-oxidation of the low-valence Co (Co 2+ , part of which was induced by the V O to balance the charge) at a relatively lower applied potential. This observation confirmed that the V O could initialize the surface reconstruction of V O -Co 3 O 4 prior to the occurrence of the OER process. The quasi-operando X-ray photoelectron spectroscopy (XPS) and operando X-ray absorption fine structure (XAFS) results further demonstrated the oxygen vacancies were filled with OH • first for V O -Co 3 O 4 and facilitated pre-oxidation of low-valence Co and promoted reconstruction/deprotonation of intermediate Co-OOH • . This work provides insight into the defect mechanism…
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Oxygen vacancies can boost the pre-oxidation of Co2+ at lower potentials, thereby generating more Co-OOH species that are beneficial for the OER catalytic process.
“the oxygen vacancies can boost the pre-oxidation of Co2+ at lower potentials hence generating more Co-OOH species, which are beneficial for the OER catalytic process”
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- Authors
- Xiao, Z., Huang, Y.-C., Dong, C.-L., Xie, C., Liu, Z., Du, S., Chen, W., Yan, D., Tao, L., Shu, Z., Zhang, G., Duan, H., Wang, Y., Zou, Y., Chen, R., & Wang, S.
- Affiliations
- Hunan University (CN)
- Department of Physics, Tamkang University, New Taipei City 25137, Taiwan
- Tamkang University (TW)
- State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan 410082, P. R. China
- Corresponding author
- Wang, Shuangyin
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-06-14
- Volume
- 142
- Issue
- 28
- Pages
- 12087-12095
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3035082486
- Cited by
- 1,445
- References
- 1
- Citations by year
- 2026: 207 · 2025: 263 · 2024: 297 · 2023: 251 · 2022: 237 · 2021: 157 · 2020: 33
- FWCI
- 33.49
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- Tamkang University Institutional Repository (TKUIR) (submittedVersion)
- Funders
- Academia Sinica (AS-iMATE-109-22)
- Ministry of Science and Technology, Taiwan (MoST 108-2218-E-032-003-MY3, MoST107-2112-M-032-004-MY3)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Keywords
- oxygen evolution reaction, Co3O4, oxygen vacancies, operando characterization, surface reconstruction, hydroxyl radicals, active site, spinel cobalt oxide
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