4.6 Article

Ultrahigh power and energy density in partially ordered lithium-ion cathode materials

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NATURE ENERGY
卷 5, 期 3, 页码 213-221

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NATURE PUBLISHING GROUP
DOI: 10.1038/s41560-020-0573-1

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资金

  1. Umicore Specialty Oxides and Chemicals
  2. Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the US Department of Energy (DOE) under the Advanced Battery Materials Research (BMR) Program [DE-AC02-05CH11231]
  3. Vehicle Technologies Office, under the Applied Battery Materials Program, of the US DOE [DE-AC02-05CH11231]
  4. Office of Science, Office of Basic Energy Sciences, of the US DOE [DE-AC02-05CH11231]
  5. Scientific User Facilities Division, Office of Basic Sciences of the US DOE
  6. Office of Science, Office of Basic Energy Sciences of the US DOE [DE-AC02-05CH11231]
  7. US DOE [DE-AC02-06CH11357]
  8. Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the US DOE [DE-AC02-05CH11231]
  9. NSF Graduate Research Fellowship [DGE-1106400]
  10. UCSB MRSEC [NSF DMR 1720256]

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There is an intensive search for high-performance cathode materials for rechargeable batteries. Here the authors report that oxyfluorides with partial spinel-like cation order, made from earth-abundant elements, display both exceptionally high energy and power. The rapid market growth of rechargeable batteries requires electrode materials that combine high power and energy and are made from earth-abundant elements. Here we show that combining a partial spinel-like cation order and substantial lithium excess enables both dense and fast energy storage. Cation overstoichiometry and the resulting partial order is used to eliminate the phase transitions typical of ordered spinels and enable a larger practical capacity, while lithium excess is synergistically used with fluorine substitution to create a high lithium mobility. With this strategy, we achieved specific energies greater than 1,100 Wh kg(-1) and discharge rates up to 20 A g(-1). Remarkably, the cathode materials thus obtained from inexpensive manganese present a rare case wherein an excellent rate capability coexists with a reversible oxygen redox activity. Our work shows the potential for designing cathode materials in the vast space between fully ordered and disordered compounds.

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