High-Density W Single Atoms in Two-Dimensional Spinel Oxide Break the Structural Integrity for Enhanced Oxygen Evolution Catalysis
The performance of oxygen evolution reaction (OER) catalysts heavily depends on intrinsically active and robust sites as well as high active site number, which poses challenges in catalyst design concerning composition and structure. This study presents a general oxygen-vacancy anchoring strategy for preparing oxide-based 4d/5d transition metal single-atom 2D materials as efficient and robust OER catalysts. In a typical synthesis, Keggin-structure polyoxometalate [PW<sub>12</sub>O<sub>40</sub>]<sup>3-</sup> clusters decompose into tetrahedral WO<sub>4</sub><sup>2-</sup> anions, which in situ adhere to the newly nucleated metal (Co, Fe, Ni) hydroxide (M(OH)<sub><i>x</i></sub>) due to the latter's abundant oxygen vacancies, ensuring a uniform distribution of W single atoms. The anchoring of W stabilizes the ultrathin structure, resulting in the annealed W-Co<sub>3</sub>O<sub>4</sub> exhibiting a specific surface area 5-7 times greater than that of pure Co<sub>3</sub>O<sub>4</sub>, even though W has three times the atomic weight of Co. Moreover, the strengthened adsorption of OH induced by W breaks the surface structural integrity of Co<sub>3</sub>O<sub>4</sub> to form a highly active oxyhydroxide, while the increased distortion in Co-O octahedrons further enhances the intrinsic activity. As a result, the catalyst shows a low η<sub>10</sub> of 261 mV in alkaline media, 84 mV lower than that of pure Co<sub>3</sub>O<sub>4</sub>, and an excellent stability of over 290 h. This places it among the best OER catalysts, particularly in comparison to low-activity Ni or -unstable NiFe alternatives.
Authors
- Jun Fan (ORCID: https://orcid.org/0000-0001-8227-9671)
- Yunpu Qin
- Wanjun Qin
- Juping Tu
- Heng Liu (ORCID: https://orcid.org/0000-0002-7272-3908)
- Baorui Jia (ORCID: https://orcid.org/0000-0002-1846-6971)
- Mingli Qin (ORCID: https://orcid.org/0000-0002-4001-6539)
- Yongzhi Zhao (ORCID: https://orcid.org/0000-0002-2509-8089)
- Xuanhui Qu (ORCID: https://orcid.org/0000-0002-2943-3008)
- Luan Liu
- Haoyang Wu (ORCID: https://orcid.org/0000-0002-7372-0872)
- Haoyin Zhong (ORCID: https://orcid.org/0000-0002-3838-6872)
- Sijia Liu (ORCID: https://orcid.org/0000-0002-4050-3548)
- Hao Li (ORCID: https://orcid.org/0000-0002-7577-1366)
- Di Zhang (ORCID: https://orcid.org/0000-0001-6347-9344)
- Yuhang Wang (ORCID: https://orcid.org/0009-0003-8376-0055)
- Yadong Liu (ORCID: https://orcid.org/0000-0001-5373-476X)
- Jianfang Liu (ORCID: https://orcid.org/0000-0002-7239-8797)
- Deyin Zhang (ORCID: https://orcid.org/0000-0001-9842-5047)
- Yong Wang
Institutions
- National University of Singapore (SG)
- City University of Hong Kong (HK)
- Tohoku University (JP)
- Peking University (CN)
- Advanced Institute of Materials Science (JP)
- Guangdong Shunde Innovative Design Institute (CN)
- Advanced Materials and Technologies (Slovenia) (SI)
- Beijing Advanced Sciences and Innovation Center (CN)
- Institute for Materials Research, Tohoku University
- Liaoning Academy of Materials
- University of Science and Technology Beijing (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-08-20
- DOI
- https://doi.org/10.1021/jacs.5c12122
- Citations
- 10
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 3.63
Funders
- Hirose Foundation
- National Natural Science Foundation of China
- China Scholarship Council
- University of Tokyo
- Japan Society for the Promotion of Science
- National Key Research and Development Program of China
- Fundamental Research Funds for the Central Universities
- Institute for Materials Research, Tohoku University
- Basic and Applied Basic Research Foundation of Guangdong Province