Negative Enthalpy Doping Stabilizes P2‐Type Oxides Cathode for High‐Performance Sodium‐Ion Batteries

Y Yongcong Huang (Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China) S Shuai Gu (College of Chemistry and Chemical Engineering, Hunan Key Laboratory of Micro & Nano Materials Interface Science) X Xin Xu Z Zibing An X Xiaodong Han Y Yulin Cao (Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China) D Dongsheng He F Fangchang Zhang (Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China) H Hao Guo Y Yan Liu X Xingqun Liao (Shenzhen Highpower Technology Co., Ltd. Shenzhen Guangdong 518111 P. R. China) G Guiyu Liu (Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen Guangdong 518055 P. R. China) P Peiwen Liu (Shanghai Key Laboratory of Chemical Biology, School of Pharmacy) F Feng Wu (Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering) Y Yingzhi Li Z Zhenyu Wang (Institute of Environmental Processes and Pollution Control, School of Environment and Ecology) Z Zhiqiang Wang C Chao Ding Y Yanfang Wang (State Key Laboratory of Advanced Drug Delivery and Release Systems, College of Pharmaceutical Sciences) J Jingjing Chen (School of Pharmaceutical Science and Technology, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences) M Mingyang Yang (Key Laboratory of Thermo-Fluid Science and Engineering, Ministry of Education, School of Energy and Power Engineering, Xi’an Jiaotong University) F Feng Jiang (State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China) Y Yonghong Deng Z Zhenghe Xu (Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen China) Z Zhouguang Lu (Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Department of Materials Science and Engineering)

Abstract

Abstract P2‐type Na 0.67 Ni 0.33 Mn 0.67 O 2 (NNMO) as cathode material for sodium‐ion batteries (SIBs) largely suffers from continuous accumulation of local stress caused by destructive structural evolution and irreversible oxygen loss upon cycling, leading to rapid capacity degradation. Herein, a strategy of negative enthalpy doping (NED), wherein transition metal (TM) sites are substituted with 0.01 mol each Sn, Sb, Cu, Ti, Mg, and Zn to increase the stability of the TM layers, is proposed. The robust structure of NED‐NNMO significantly suppresses the P2 to O2 phase transition and improves the Na + kinetics upon long‐term cycling. Consequently, the NED‐NNMO exhibits much smoothened voltage platforms and improved oxygen redox reversibility, thus considerably extended lifetime as compared with the pristine NNMO sample. The NED‐NNMO delivers a high capacity of 138.9 mAh g −1 with an operation voltage of 3.51 V under 0.1 C and prominent capacity retention of 94.6% after 100 cycles under 1 C, and 90.0% over 3000 cycles under ultra‐high rate of 30 C, which is among the best over previous reports. Moreover, an ampere‐hour scale pouch cell based on the NED‐NNMO demonstrates an energy density of 139 Wh kg −1 . This work sheds light on a route of negative enthalpy doping to design high‐performance sodium‐ion batteries.

Article Details

Volume / Issue Vol. 37, Issue 17
Published April 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (25)

Y

Yongcong Huang

Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China

S

Shuai Gu

College of Chemistry and Chemical Engineering, Hunan Key Laboratory of Micro & Nano Materials Interface Science

X

Xin Xu

Z

Zibing An

X

Xiaodong Han

Y

Yulin Cao

Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China

D

Dongsheng He

F

Fangchang Zhang

Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China

H

Hao Guo

Y

Yan Liu

X

Xingqun Liao

Shenzhen Highpower Technology Co., Ltd. Shenzhen Guangdong 518111 P. R. China

G

Guiyu Liu

Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen Guangdong 518055 P. R. China

P

Peiwen Liu

Shanghai Key Laboratory of Chemical Biology, School of Pharmacy

F

Feng Wu

Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering

Y

Yingzhi Li

Z

Zhenyu Wang

Institute of Environmental Processes and Pollution Control, School of Environment and Ecology

Z

Zhiqiang Wang

C

Chao Ding

Y

Yanfang Wang

State Key Laboratory of Advanced Drug Delivery and Release Systems, College of Pharmaceutical Sciences

J

Jingjing Chen

School of Pharmaceutical Science and Technology, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences

M

Mingyang Yang

Key Laboratory of Thermo-Fluid Science and Engineering, Ministry of Education, School of Energy and Power Engineering, Xi’an Jiaotong University

F

Feng Jiang

State Key Laboratory of Integrated Optoelectronics, JLU Region, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China

Y

Yonghong Deng

Z

Zhenghe Xu

Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen China

Z

Zhouguang Lu

Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Department of Materials Science and Engineering