Tailoring Local Superstructure Units to Mitigate Voltage Decay in Na‐Ion Batteries

H Haojie Dong X Xu Zhu (Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering) S Si‐Fan Chen (Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China) H Haoliang Liu C Chao Li S Shao‐Wen Xu (Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China) G Guang‐Xu Wei (Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China) Y Yuanguang Xia (Institute of High Energy Physics, Chinese Academy of Sciences) Y Yongwei Tang (Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering) Y Yi‐Hu Feng (Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China) M Mengting Liu (Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering) K Kai Chen B Bing Xiao (Department of Orthopaedics) Y Yonghong Cheng P Peng‐Fei Wang (Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P.R. China)

Abstract

ABSTRACT The practical application of high‐energy‐density P2‐type cathodes is hindered by severe voltage decay upon high‐potential cycling. This voltage decay primarily originates from irreversible interlayer cation migration and detrimental structural degradation, which can be notably suppressed by regulating the arrangement of superstructure units. Herein, we incorporate LiTiMn 5 superstructure units in P2‐Na 0.7 K 0.04 Li 0.1 Ni 0.22 Mn 0.6 Ti 0.08 O 2 (NaKLNMT) to construct the long‐range in‐plane ordered arrangement within transition metal slabs, creating a stable oxygen coordination environment and high energy barriers along the migration path. Furthermore, the circumscribed P‐type to O‐type stacking evolution and restricted Li/TM migration restrain the formation of vacancy clusters, prohibiting consequential overoxidation of lattice oxygen and inhomogeneous lattice strain accumulation under high‐voltage. Therefore, the target NaKLNMT compound exhibits a negligible voltage decay of 0.15 mV/cycle and 96.3% capacity retention over 100 cycles at 1 C. Our findings demonstrate that regulating cation migration through local superstructure control helps steer strategies to address the issues of voltage decay in sodium‐layered oxide cathodes.

Article Details

Volume / Issue Vol. 1, Issue 1
Published June 22, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (15)

H

Haojie Dong

X

Xu Zhu

Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering

S

Si‐Fan Chen

Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China

H

Haoliang Liu

C

Chao Li

S

Shao‐Wen Xu

Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China

G

Guang‐Xu Wei

Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China

Y

Yuanguang Xia

Institute of High Energy Physics, Chinese Academy of Sciences

Y

Yongwei Tang

Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering

Y

Yi‐Hu Feng

Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China

M

Mengting Liu

Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering

K

Kai Chen

B

Bing Xiao

Department of Orthopaedics

Y

Yonghong Cheng

P

Peng‐Fei Wang

Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi P.R. China