Unraveling the Synergistic effects of La and Al co-doping on Ni/Co-free P2-type Na0.67Mn0.67Fe0.33O2 layered oxide cathodes for sodium-ion batteries

Publication Type

Journal Article

Name of Author

• Nkechi Offiakalu, Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, Worcester, USA
• Panya Thanwisai, Department of Physics, Faculty of Science, Khon Kaen University, Khon Kaen, Thailand
• Jaemin Kim, Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, Worcester, MA, USA
• Zifei Meng, Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, Worcester, MA, USA
• Zeyi Yao, Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, Worcester, MA,USA
• Hao Zhou, Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, Worcester, MA, USA
• Hari Adhikari, Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA
• Jianguo Wen, Argonne National Laboratory, Lemont, United States
• Yihao Shen, School of Systems Science and Industrial Engineering, Thomas J. Watson College of Engineering and Applied Science, Binghamton University, Binghamton, NY, USA
• Xiaotu Ma, School of Systems Science and Industrial Engineering, Thomas J. Watson College of Engineering and Applied Science, Binghamton University, Binghamton, NY, USA
• Bello A. Abdulhakeem, African University of Science and Technology, Abuja, Nigeria
• Jianyu Liang, Department of Mechanical and Materials Engineering, Worcester Polytechnic Institute, Worcester, MA, USA
• Yan Wang, School of Engineering, Worcester, United States

Publication Date (Issue Year)

2026

Journal Name

Journal of Energy Storage

Abstract

Recent developments in high-performance cathodes for sodium-ion batteries (SIBs) tend to mitigate use of critical Ni and Co active species to satisfy sustainability. P2-type layered oxide cathodes based on Mn and Fe promise high capacity, sustainability, and low cost on account of the abundance and multiple redox characteristics of Mn and Fe. However, their commercialization is still challenged due to poor cycling stability caused by phase changes emanating from inherent Jahn-Teller distortions. Herein, we propose a novel strategy of trivalent La and Al co-doping to alleviate the drawbacks, innovating a new cathode of Na0.67Mn0.62Al0.05Fe0.31La0.02O2 (AlLa). The co-doped cathode delivers an impressive capacity of 128.7 mAh/g at 1C and 106.5 mAh/g at high rate of 5C with a good capacity retention of 85% after 100 cycles. These are superior to the unmodified material, whose specific capacity was 118.6 mAh/g at 1C and 61.1 mAh/g at 5C with a retention of only 65% after 100 cycles. The synergistic contribution from La and Al associated with their improved oxygen bonding, pillaring, and local electronic structural modification stemming from rigid LaO and AlO bonding resulted in the observed structural and electrochemical improvement. Overall, this research offers novel strategies for designing high-performance cathode materials for sodium-ion batteries.

Keywords

P2-type layered oxides, Mn/Fe-based cathodes, Co-doping, Sodium ion batteries

Rsif Scholar Name

Nkechi Elizabeth Offia-Kalu

Rsif Scholar Nationality

Nigeria

Cohort

Cohort 3

Thematic Area

Minerals, Mining and Materials Engineering

Africa Host University (AHU)

African University of Science and Technology (AUST), Nigeria

Funding Statement

The research was funded by the Regional Scholarship and Innovation Fund (RSIF), a flagship program of the Partnership for Skill in Applied Sciences, Engineering and Technology (PASET), Grant number B850/P10010. The authors thank Prof. Geoffrey Tompsett at the Department of Chemical Engineering, Worcester Polytechnic Institute, for his kind assistance with Raman Spectroscopy. TEM test was performed at the Center for Nanoscale Materials and Advanced Photon Source, both U.S. Department of Energy Office of Science User Facilities, which was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

Recommended Citation

Offiakalu, N., Thanwisai, P., Kim, J., Meng, Z., Yao, Z., Zhou, H., Adhikari, H., Wen, J., Shen, Y., Ma, X., A. Abdulhakeem, B., Liang, J., & Wang, Y. (2026). Unraveling the Synergistic effects of La and Al co-doping on Ni/Co-free P2-type Na0.67Mn0.67Fe0.33O2 layered oxide cathodes for sodium-ion batteries. Journal of Energy Storage https://doi.org/10.1016/j.est.2026.121971