Unlocking the Orbital Interaction Mode in Li–O <sub>2</sub> Batteries
Understanding electrocatalyst-intermediate orbital interaction in oxygen evolution reactions (OER) is critical for designing high-performance lithium-oxygen (Li-O<sub>2</sub>) batteries, yet remains a significant challenge. In this study, we employed a CdSe-based catalyst as a model cathode to deeply investigate the catalyst-intermediate interaction and its effect on OER activity. Compared to the 4d orbital electronic states of Cd in CdSe, electron transfer from CdSe to ZnS in the CdSe/ZnS heterojunction results in a downward shift of the Cd 4d suborbital energy levels. The differences in the Cd 4d orbital electronic states between CdSe and CdSe/ZnS cause distinct orbital interaction mode with LiO<sub>2</sub> intermediate, ultimately leading to variations in OER activity. Specifically, compared to the strong Cd 4d<sub>xy</sub>-O 2P<sub>x/y</sub> orbital interaction mode between CdSe and LiO<sub>2</sub>, the weaker Cd 4d<sub>z</sub> <sup>2</sup>-O 2P<sub>y</sub> orbital interaction mode between CdSe/ZnS and LiO<sub>2</sub> significantly reduces the activation energy of the rate-determining step, thereby enhancing OER activity. This finding provides theoretical guidance for the design of OER electrocatalysts in Li-O<sub>2</sub> batteries.
Authors
- Yicheng Zeng
- Yin Zhou (ORCID: https://orcid.org/0000-0001-9609-407X)
- Fangze Liu (ORCID: https://orcid.org/0000-0003-3114-5280)
- Hongbo Li (ORCID: https://orcid.org/0000-0002-3378-0870)
Institutions
- Beijing Institute of Technology (CN)
- City University of Hong Kong (HK)
- Beijing Research Institute of Mechanical and Electrical Technology (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-11-13
- DOI
- https://doi.org/10.1002/anie.202520062
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Natural Science Foundation of China