Local electronic regulation of Na5V12O32 cathode suppressing structural distortion toward enhanced sodium storage

Xuexia Song, Jingjing Wang, Wenbin Li (), Wei Xiao, Gaini Zhang, Shuling Liu, Yunkai Xu, Jun Lu () and Xifei Li ()
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Xuexia Song: Xi’an University of Technology, Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering
Jingjing Wang: Xi’an University of Technology, Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering
Wenbin Li: Xi’an University of Technology, Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering
Wei Xiao: Xi’an University of Technology, Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering
Gaini Zhang: Xi’an University of Technology, Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering
Shuling Liu: Shaanxi University of Science and Technology, Department of Chemistry and Chemical Engineering, Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry & Technology, Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry, Ministry of Education
Yunkai Xu: Zhejiang University, College of Chemical and Biological Engineering
Jun Lu: Zhejiang University, College of Chemical and Biological Engineering
Xifei Li: Xi’an University of Technology, Institute of Advanced Electrochemical Energy & School of Materials Science and Engineering

Nature Communications, 2025, vol. 16, issue 1, 1-15

Abstract: Abstract High-voltage layered oxide cathodes have received extensive attention for sodium-ion batteries owing to their potential high energy and power densities, but their stabilization remains a universal challenge. Herein, a stable high-voltage KxNa5-xV12O32 cathode is designed by synergistically tuning the irreversible phase and oxygen vacancies through the substitution of Na with K. The functional mechanism regulating the electronic structure of KxNa5-xV12O32 is elucidated: K substitution strengthens V 3d–O 2p hybridization and V 3d–orbital electron delocalization in the K0.147Na4.853V12O32 structure, enriching charge distribution and reinforcing the V3O8 structure. This promots electron transfer kinetics, suppresses irreversible phase transition, and lowers the Na+ diffusion energy barrier. Moreover, the reversible redox reaction of V5+/V4+ is significantly enhanced, delivering 250.1 mA h g−1 (1.5–4.3 V vs. Na/Na+), which increases the average operating voltage from 4.0 to 4.3 V and boosts the overall energy density. Consequently, the K0.147Na4.853V12O32 electrode significantly enhances cycling performance, retaining 98.2% of the capacity after 1000 cycles at 1300 mA g−1 and enabling stable cycling with 98.7% retention after 300 cycles in a hard carbon | | K0.147Na4.853V12O32 pouch cell. This strategy of electronic structure modulation offers avenues for developing high energy density stable vanadium-based cathode materials for sodium-ion batteries.

Date: 2025
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DOI: 10.1038/s41467-025-63879-0

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