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Fluorine-Rich Oxyfluoride Spinel-like Li1.25Ni0.625Mn1.125O3F Utilizing Redox-Active Ni and Mn for High Capacity and Improved Cyclability AITranslate

Hong Cai; Ruiyong Chen; Mounib Bahri; Cara J. Hawkins; Manel Sonni; Luke M. Daniels; Jungwoo Lim; Jae A. Evans; Marco Zanella; Leanne A. H. Jones; Troy D. Manning; Tim D. Veal; Laurence J. Hardwick; Matthew S. Dyer; Nigel D. Browning; John B. Claridge; Matthew J. Rosseinsky
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Abstract AITranslate

Extending the accessible capacity and cyclability is of central interest for cathode materials for Li-ion batteries. Here, we report the successful synthesis of a new spinel-like Li1.25Ni0.625Mn1.125O3F (Fd3m) oxyfluoride with significant cation disorder characterized by combined refinement of X-ray and neutron diffraction data. Li1.25Ni0.625Mn1.125O3F utilizes redox reactions of both Ni and Mn, accessing capacities of 225 (i.e., 1.46 Li+ capacity) and 285 mAh g–1 (i.e., 1.85 Li+ capacity) at 25 and 40 °C, respectively, through intercalation of additional Li+ into the lattice. Moreover, compared to lithium transition metal disordered rocksalt or spinel-like oxyfluorides previously reported, Li1.25Ni0.625Mn1.125O3F shows significantly improved cycling stability. Ex situ compositional, structural, and spectroscopic analyses of samples at different states of charge/discharge confirm a single-phase intercalation reaction and high structural integrity over cycling.

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DOI：https://doi.org/10.1021/acsmaterialslett.2c00973

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Citation Information:

Extending the accessible capacity and cyclability is of central interest for cathode materials for Li-ion batteries. Here, we report the successful synthesis of a new spinel-like Li1.25Ni0.625Mn1.125O3F (Fd3m) oxyfluoride with significant cation disorder characterized by combined refinement of X-ray and neutron diffraction data. Li1.25Ni0.625Mn1.125O3F utilizes redox reactions of both Ni and Mn, accessing capacities of 225 (i.e., 1.46 Li+ capacity) and 285 mAh g–1 (i.e., 1.85 Li+ capacity) at 25 and 40 °C, respectively, through intercalation of additional Li+ into the lattice. Moreover, compared to lithium transition metal disordered rocksalt or spinel-like oxyfluorides previously reported, Li1.25Ni0.625Mn1.125O3F shows significantly improved cycling stability. Ex situ compositional, structural, and spectroscopic analyses of samples at different states of charge/discharge confirm a single-phase intercalation reaction and high structural integrity over cycling.

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GB/T 7714-2015 [1] Hong Cai, Ruiyong Chen, Mounib Bahri, et al. ACS Materials Letters, 2023(5). DOI:10.1021/acsmaterialslett.2c00973.
MLA [1] Hong Cai, et al., ACS Materials Letters, no. 5, 2023, https://doi.org/10.1021/acsmaterialslett.2c00973.
APA [1] Hong Cai, Ruiyong Chen, Mounib Bahri, Cara J. Hawkins, Manel Sonni, Luke M. Daniels, Jungwoo Lim, Jae A. Evans, Marco Zanella, Leanne A. H. Jones, Troy D. Manning, Tim D. Veal, Laurence J. Hardwick, Matthew S. Dyer, Nigel D. Browning, John B. Claridge, & Matthew J. Rosseinsky. (2023). ACS Materials Letters(5). https://doi.org/10.1021/acsmaterialslett.2c00973
IEEE [1] Hong Cai, Ruiyong Chen, Mounib Bahri, Cara J. Hawkins, Manel Sonni, Luke M. Daniels, Jungwoo Lim, Jae A. Evans, Marco Zanella, Leanne A. H. Jones, Troy D. Manning, Tim D. Veal, Laurence J. Hardwick, Matthew S. Dyer, Nigel D. Browning, John B. Claridge, and Matthew J. Rosseinsky, ACS Materials Letters, no. 5, 2023, doi: 10.1021/acsmaterialslett.2c00973.