Li\(_{5}\)FeO\(_{4}\) as a cathode prelithiation additive: Doping engineering and first-principles research

Zixiang LI; Zile ZOU; Jialan LI; Chennan MA; Jiarun LI; Xiaoyu LIU; Jin  YI; Jianhui LI

doi:10.55713/jmmm.v36i3.2819

Authors

Zixiang LI School of Materials and New Energy, South China Normal University, Shanwei Guangdong, 516600, China
Zile ZOU School of Materials and New Energy, South China Normal University, Shanwei Guangdong, 516600, China
Jialan LI School of Materials and New Energy, South China Normal University, Shanwei Guangdong, 516600, China
Chennan MA School of Materials and New Energy, South China Normal University, Shanwei Guangdong, 516600, China
Jiarun LI School of Materials and New Energy, South China Normal University, Shanwei Guangdong, 516600, China
Xiaoyu LIU Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444,China
Jin YI Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444,China
Jianhui LI School of Materials and New Energy, South China Normal University, Shanwei Guangdong, 516600, China

DOI:

https://doi.org/10.55713/jmmm.v36i3.2819

Keywords:

Lithium ion batteries, Prelithiation, Li5FeO4, Doping, First principles

Abstract

During the initial charge-discharge cycle, irreversible loss of active lithium (~ 5% to 15%) severely affects the battery energy density and shortens cycle life of lithium‑ion batteries (LIBs). Prelithiation strategy has gradually become an effective approach to compensate for the irreversible loss of active lithium. Lithium ferrate (Li₅FeO₄, LFO) is considered to be a promising cathode prelithiation additive due to its high theoretical capacity (867 mAh·g^‒1), suitable delithiation potential (3.5 V to 4.1 V), and competitive raw material. However, the application of LFO is limited by the its properties including poor air stability, low electronic conductivity, and incomplete delithiation. Currently, great efforts are made to address the above limitations through surface coating and bulk doping. This review summarizes the recent advances in Fe‑site and non‑Fe‑site doping, highlighting the effects of dopants on modulating the crystal structure, Li⁺ diffusion kinetics, and electrochemical properties of LFO. The studies of first‑principles on doped LFO, including formation energies, density of states, and migration barriers together with the value of theoretical tools when assessing doping performance are presented. In the end, the remaining challenges and future development directions for LFO doping design are put forward, offering perspectives for advancing prelithiation strategy in high‑energy‑density LIBs.

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