Amorphous iron fluorosulfate as a high-capacity cathode utilizing combined intercalation and conversion reactions with unexpectedly high reversibility

Jaehoon Heo, Sung-Kyun Jung, Insang Hwang, Sung-Pyo Cho, Donggun Eum, Hyeokjun Park, Jun-Hyuk Song, Seungju Yu, Kyungbae Oh, Giyun Kwon, Taehyun Hwang, Kun-Hee Ko and Kisuk Kang ()
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Jaehoon Heo: Seoul National University
Sung-Kyun Jung: Ulsan National Institute of Science and Technology (UNIST)
Insang Hwang: Seoul National University
Sung-Pyo Cho: Seoul National University
Donggun Eum: Seoul National University
Hyeokjun Park: Seoul National University
Jun-Hyuk Song: Seoul National University
Seungju Yu: Seoul National University
Kyungbae Oh: Seoul National University
Giyun Kwon: Seoul National University
Taehyun Hwang: Seoul National University
Kun-Hee Ko: Seoul National University
Kisuk Kang: Seoul National University

Nature Energy, 2023, vol. 8, issue 1, 30-39

Abstract: Abstract To achieve the desirable dual characteristics of high-capacity performance and low-cost production for the batteries of tomorrow, leveraging of multi-redox reactions of Earth-abundant transition metals in electrodes is fundamentally important. Here we identify an amorphous iron fluorosulfate electrode, a-LiFeSO4F, that can exploit both the intercalation and conversion reactions with a stable reversibility. The a-LiFeSO4F electrode delivers a capacity of 360 mAh g−1 with ~98.6% capacity retention after 200 cycles even at an elevated temperature (60 °C). In contrast to the conventional intercalation/conversion-type electrodes, the reversible cycle stability is attributed to the inherent amorphous structure of a-LiFeSO4F, whose structural integrity is not severely disturbed even after the conversion reaction, allowing its continuation as an intercalation host. We believe that this cycle stability of the intercalation/conversion reaction can be generally extended to various amorphous intercalation materials, offering new insights into the design of high-capacity electrodes through the exploitation of multi-mechanistic lithiation processes.

Date: 2023
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DOI: 10.1038/s41560-022-01148-w

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