Published February 16, 2023 | Version v1
Journal article Open

Temperature-driven chemical segregation in Co-free Li-rich layered oxides and its influence on electrochemical performance

  • 1. Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, 08930 Barcelona, Spain.
  • 2. Department of Materials and Environmental Chemistry, Stockholm University 106 91 Stockholm, Sweden.
  • 3. Ceramic Powder Technology AS, Kvenildmyra 6, 7093 Tiller, Norway
  • 4. UHasselt, Institute for Materials Research (IMO-Imomec), Imec, division Imomec, and EnergyVille, Agoralaan, Building D, 3590 Diepenbeek, Belgium
  • 5. Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, 08930 Barcelona, Spain

Description

Co-free Li-rich layered oxides are gaining interest as feasible positive electrode materials in lithium-ion batteries (LIBs) in terms of energy density, cost reduction, and alleviating safety concerns. Unfortunately, their commercialization is hindered by the severe structural degradation that occurs during electrochemical operation. The study at hand demonstrates advanced structural engineering of a Li-rich Co-free oxide with composition Li1.1Ni0.35Mn0.55O2 by spray-pyrolysis and subsequent calcination of an aqueous precursor, creating a segregated structure of two distinct layered phases with space groups 𝑅3̅𝑚 (rhombohedral) and 𝐶2/𝑚 (monoclinic) . This particular structure was investigated with powder neutron diffraction, high-resolution analytical transmission electron microscopy imaging, and electron energy loss spectroscopic characterization. This complex structure contributes to the high electrochemical stability and good rate capability observed for this compound (160 mAh/g at C/3 and 100 mAh/g at 1C). These results provide new insights into the feasibility of developing and commercializing of cobalt-free positive electrode materials for LIBs.

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Additional details

Funding

European Commission
COBRA - CObalt-free Batteries for FutuRe Automotive Applications 875568