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Fe-based polyanion materials such as LiFePO4 or LiFeBO3 are safe and can achieve high energy density, so they have been considered as cathode materials for large-scale lithium ion batteries. Among these compounds, LiFeSO4F achieves the highest voltage (3.9 V) among Fe2+/Fe3+ redox couples and therefore can have higher energy density than LiFePO4. However, full utilization of 3.9 V LiFeSO4F is severely limited by its non-scalable synthesis process and poor electrochemical activity. Here, we report a method to synthesize 3.9 V LiFeSO4F by a scalable solid-state reaction within 1 h by understanding the thermodynamic stability of 3.9 V LiFeSO4F. The resulting material shows the best electrochemical performance reported to date. The process yields nanosized particles that achieve almost full capacity, 140 mA h g−1, which is 93% of the theoretical capacity and that retain excellent capacity, ∼75 mA h g−1 at 1 C for 150 cycles and high rate capability even at 10 C (6 min). This scalable solid-state reaction for 3.9 V LiFeSO4F makes it a plausible replacement for LiFePO4 in the next generation of lithium ion batteries.

High electrochemical performance of 3.9 V LiFeSO4F directly synthesized by a scalable solid- state reaction within 1 h

High electrochemical performance of 3.9 V LiFeSO₄F directly synthesized by a scalable solid- state reaction within 1 h