Fluorinated Rocksalt Cathode with Ultra-high Active Li Content for Lithium-ion Batteries
- Univ. of Waterloo, ON (Canada)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Chinese Academy of Sciences (CAS), Beijing (China)
- Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Univ. of Toronto, ON (Canada)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- McMaster Univ., Hamilton, ON (Canada)
- Nanjing Univ. (China)
AbstractThe key to increasing the energy density of lithium‐ion batteries is to incorporate high contents of extractable Li into the cathode. Unfortunately, this triggers formidable challenges including structural instability and irreversible chemistry under operation. Here, we report a new kind of ultra‐high Li compound: Li4+xMoO5Fx (1≤x≤3) for cathode with an unprecedented level of electrochemically active Li (>3 Li+ per formula), delivering a reversible capacity up to 438 mAh g−1. Unlike other reported Li‐rich cathodes, Li4+xMoO5Fx presents distinguished structure stability to immunize against irreversible behaviors. Through spectroscopic and electrochemical techniques, we find an anionic redox‐dominated charge compensation with negligible oxygen release and voltage decay. Our theoretical analysis reveals a “reductive effect” of high‐level fluorination stabilizes the anionic redox by reducing the oxygen ions in pure‐Li conditions, enabling a facile, reversible, and high Li‐portion cycling.
- Research Organization:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science and Engineering Research Council of Canada (NSERC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
- Grant/Contract Number:
- SC0012704; AC02-06CH11357; AC02-05CH11231; DEAC02-05CH11231
- OSTI ID:
- 1973512
- Alternate ID(s):
- OSTI ID: 1898160; OSTI ID: 2280945
- Report Number(s):
- BNL-224386-2023-JAAM
- Journal Information:
- Angewandte Chemie (International Edition), Vol. 61, Issue 47; ISSN 1433-7851
- Publisher:
- WileyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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