Unlocking the Orbital Interaction Mode in Li-O2 Batteries

Yicheng Zeng; Yin Zhou; Fangze Liu; Hongbo Li

doi:10.1002/anie.202520062

Unlocking the Orbital Interaction Mode in Li-O₂Batteries

Yicheng Zeng
, Yin Zhou^*
, Fangze Liu
, Hongbo Li^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

2 Citations (Scopus)

Abstract

Understanding electrocatalyst-intermediate orbital interaction in oxygen evolution reactions (OER) is critical for designing high-performance lithium–oxygen (Li–O2) 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 LiO₂ intermediate, ultimately leading to variations in OER activity. Specifically, compared to the strong Cd 4d_xy–O 2P_x/y orbital interaction mode between CdSe and LiO₂, the weaker Cd 4d_z²–O 2P_y orbital interaction mode between CdSe/ZnS and LiO₂significantly 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–O₂ batteries.
© 2025 Wiley-VCH GmbH

Original language	English
Article number	e20062
Number of pages	8
Journal	Angewandte Chemie International Edition
Volume	65
Issue number	2
Online published	13 Nov 2025
DOIs	https://doi.org/10.1002/anie.202520062
Publication status	Published - 9 Jan 2026

Funding

This work was supported by the National Natural Science Foundation of China (grant no. 22179009, U22A2072, and 52372135) and the China Postdoctoral Science Foundation (grant no. 2025M774199).

Research Keywords

CdSe/ZnS heterojunction
Electrocatalyst-intermediate interaction
Lithium-oxygen batteries
Orbital electronic states
Oxygen evolution reactions

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Cite this

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title = "Unlocking the Orbital Interaction Mode in Li-O2 Batteries",

abstract = "Understanding electrocatalyst-intermediate orbital interaction in oxygen evolution reactions (OER) is critical for designing high-performance lithium–oxygen (Li–O2) 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 LiO2 intermediate, ultimately leading to variations in OER activity. Specifically, compared to the strong Cd 4dxy–O 2Px/y orbital interaction mode between CdSe and LiO2, the weaker Cd 4dz2–O 2Py orbital interaction mode between CdSe/ZnS and LiO2 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–O2 batteries. {\textcopyright} 2025 Wiley-VCH GmbH",

keywords = "CdSe/ZnS heterojunction, Electrocatalyst-intermediate interaction, Lithium-oxygen batteries, Orbital electronic states, Oxygen evolution reactions",

author = "Yicheng Zeng and Yin Zhou and Fangze Liu and Hongbo Li",

year = "2026",

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TY - JOUR

T1 - Unlocking the Orbital Interaction Mode in Li-O2 Batteries

AU - Zeng, Yicheng

AU - Zhou, Yin

AU - Liu, Fangze

AU - Li, Hongbo

PY - 2026/1/9

Y1 - 2026/1/9

N2 - Understanding electrocatalyst-intermediate orbital interaction in oxygen evolution reactions (OER) is critical for designing high-performance lithium–oxygen (Li–O2) 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 LiO2 intermediate, ultimately leading to variations in OER activity. Specifically, compared to the strong Cd 4dxy–O 2Px/y orbital interaction mode between CdSe and LiO2, the weaker Cd 4dz2–O 2Py orbital interaction mode between CdSe/ZnS and LiO2 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–O2 batteries. © 2025 Wiley-VCH GmbH

AB - Understanding electrocatalyst-intermediate orbital interaction in oxygen evolution reactions (OER) is critical for designing high-performance lithium–oxygen (Li–O2) 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 LiO2 intermediate, ultimately leading to variations in OER activity. Specifically, compared to the strong Cd 4dxy–O 2Px/y orbital interaction mode between CdSe and LiO2, the weaker Cd 4dz2–O 2Py orbital interaction mode between CdSe/ZnS and LiO2 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–O2 batteries. © 2025 Wiley-VCH GmbH

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KW - Electrocatalyst-intermediate interaction

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KW - Oxygen evolution reactions

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DO - 10.1002/anie.202520062

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