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Integrated rocksalt–polyanion cathodes with excess lithium and stabilized cycling

Journal Article · · Nature Energy
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  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Tsinghua Univ., Beijing (China); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Pennsylvania State Univ., University Park, PA (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Gachon University, Seongnam (Korea, Republic of)
  6. McGill Univ., Montreal, QC (Canada)
  7. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
  8. Huazhong Univ. of Science and Technology, Wuhan (China)
  9. Fudan Univ., Shanghai (China)
  10. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  11. Spallation Neutron Source Science Center, Dongguan (China); Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics (IHEP)
  12. Chinese Academy of Sciences (CAS), Shanghai (China)
  13. Chung Yuan Christian University, Taoyuan City (Taiwan)
  14. National Central Univ., Taoyuan (Taiwan)
+ Show Author Affiliations
Co- and Ni-free disordered rocksalt cathodes utilize oxygen redox to increase the energy density of lithium-ion batteries, but it is challenging to achieve good cycle life at high voltages >4.5 V (versus Li/Li+). Here, in this study, we report a family of Li-excess Mn-rich cathodes that integrates rocksalt- and polyanion-type structures. Following design rules for cation filling and ordering, we demonstrate the bulk incorporation of polyanion groups into the rocksalt lattice. This integration bridges the two primary families of lithium-ion battery cathodes—layered/spinel and phosphate oxides—dramatically enhancing the cycling stability of disordered rocksalt cathodes with 4.8 V upper cut-off voltage. The cathode exhibits high gravimetric energy densities above 1,100 Wh kg-1 and >70% retention over 100 cycles. This study opens up a broad compositional space for developing battery cathodes using earth-abundant elements such as Mn and Fe.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; SC0012704
OSTI ID:
2440607
Alternate ID(s):
OSTI ID: 2473051
Report Number(s):
BNL--226070-2024-JAAM
Journal Information:
Nature Energy, Journal Name: Nature Energy Vol. 9; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE