Toward Stable Cycling of a Cost-Effective Cation-Disordered Rocksalt Cathode via Fluorination

Qian, Ji; Ha, Yang; Koirala, Krishna Prasad; Huang, Di; Huang, Zhi; Battaglia, Vincent S.; Wang, Chongmin; Yang, Wanli; Tong, Wei

doi:10.1002/adfm.202205972

Toward Stable Cycling of a Cost-Effective Cation-Disordered Rocksalt Cathode via Fluorination

Journal Article · Wed Mar 08 00:00:00 EST 2023 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202205972· OSTI ID:2325980

Qian, Ji ^[1]; Ha, Yang ^[2]; Koirala, Krishna Prasad ^[3]; Huang, Di ^[1]; Huang, Zhi ^[1]; Battaglia, Vincent S. ^[1]; Wang, Chongmin ^[3]; Yang, Wanli ^[2]; ^[1]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

The recently developed Li-excess cation-disordered rock salts (DRXs) exhibit an excellent chemical diversity for the development of alternative Co/Ni-free high-energy cathodes. Herein, the synthesis of a highly fluorinated DRX cathode, Li_1.2Mn_0.6Ti_0.2O_1.8F_0.2, based on cost-effective and earth-abundant transition metals, via a solid-state reaction, is reported. The fluorinated DRX cathode using ammonium fluoride precursor exhibits more uniform particle size and delivers a specific discharge capacity of 233 mAh g^-1 and specific energy of 754 Wh kg^-1, with 206 mAh g^-1 retained after 200 cycles. Further, the combined synchrotron X-ray absorption spectroscopy and resonant inelastic X-ray scattering spectroscopy analysis reveals that the remarkable cycling performance is attributed to the high fluorination and thus enhanced Mn content, enabling the utilization of more Mn redox than the oxide analog. This study demonstrates a great promise to develop next-generation cost-effective DRX cathodes with enhanced capacity retention for high-energy Li-ion batteries.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515

OSTI ID:: 2325980

Alternate ID(s):: OSTI ID: 1975462

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 22 Vol. 33; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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