D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries

Yin Zhou, Kun Yin, Yingying Huang, Jiapei Li, Anquan Zhu, Dewu Lin, Guoqiang Gan, Jianfang Zhang, Kai Liu, Tian Zhang, Kunlun Liu, Chuhao Luan, Huawei Yang, Hou Chen, Shaojun Guo (), Wenjun Zhang () and Guo Hong ()
Additional contact information
Yin Zhou: 83 Tat Chee Avenue
Kun Yin: Ludong University
Yingying Huang: 83 Tat Chee Avenue
Jiapei Li: 83 Tat Chee Avenue
Anquan Zhu: 83 Tat Chee Avenue
Dewu Lin: 83 Tat Chee Avenue
Guoqiang Gan: 83 Tat Chee Avenue
Jianfang Zhang: 83 Tat Chee Avenue
Kai Liu: 83 Tat Chee Avenue
Tian Zhang: 83 Tat Chee Avenue
Kunlun Liu: 83 Tat Chee Avenue
Chuhao Luan: 83 Tat Chee Avenue
Huawei Yang: Ludong University
Hou Chen: Ludong University
Shaojun Guo: Peking University
Wenjun Zhang: 83 Tat Chee Avenue
Guo Hong: 83 Tat Chee Avenue

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Charge overpotential for oxygen evolution reaction is a crucial parameter for the energy conversion efficiency of lithium-oxygen (Li-O2) batteries. So far, the realization of low charge overpotential via catalyst design is a grand challenge in this field, which usually exceeds 0.25 V. Herein, we report an orbital reconstruction strategy to significantly decrease the charge overpotential to the low 0.11 V by employing PdCo nanosheet catalyst under a low-loading mass (0.3 mg/cm2) and capacity (0.3 mAh/cm2). Experimental and theoretical calculations demonstrate that the precise d-d orbital coupling (dxz-dxz, dyz-dyz and dz2-dz2) between the low-electronegativity Co and Pd leads to the reconstruction of Pd 4 d orbitals in PdCo nanosheets, thereby resulting in a downward shift of all the three active Pd 4 d orbitals (dz2, dxz and dyz) relative to that of Pd nanosheets. Furthermore, the highest energy level of the Pd 4dz2 orbital in PdCo is lower than the lowest energy levels of the Pd 4dxz and 4dyz orbitals in pure Pd, significantly decreasing the charge activation energy and achieving a highest energy conversion efficiency of 91%. This finding provides the orbital-level tuning into rational design of highly efficient electrocatalysts for Li-O2 batteries.

Date: 2025
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DOI: 10.1038/s41467-025-58640-6

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