4.8 Article

Temperature-Driven Chemical Segregation in Co-Free Li-Rich-Layered Oxides and Its Influence on Electrochemical Performance

期刊

CHEMISTRY OF MATERIALS
卷 34, 期 8, 页码 3637-3647

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c04150

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资金

  1. Generalitat de Catalunya [2017 SGR 327, 2017 SGR 1246]
  2. Spanish MINECO [ENE2017-85087-C3, PID2020116093RB-C43/AEI]
  3. CERCA Programme/Generalitat de Catalunya
  4. HORIZON 2020-supported EU project COBRA [H2020-EU.3.4.-875568]

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Co-free Li-rich layered oxides with a segregated structure show high electrochemical stability and good rate capability, making them promising positive electrode materials for lithium-ion batteries. The study provides new insights into the development and commercialization of cobalt-free positive electrode materials for LIBs.
Co-free Li-rich layered oxides are gaining interest as feasible positiveelectrode materials in lithium-ion batteries (LIBs) in terms of energy density, costreduction, and alleviating safety concerns. Unfortunately, their commercialization ishindered by severe structural degradation that occurs during electrochemical operation.The study at hand demonstrates advanced structural engineering of a Li-rich Co-freeoxide with composition Li1.1Ni0.35Mn0.55O2by spray pyrolysis and subsequentcalcination of an aqueous precursor, creating a segregated structure of two distinctlayered phases with space groupsR3??m(rhombohedral) andC2/m(monoclinic). Thisparticular structure was investigated with powder neutron diffraction, high-resolutionanalytical transmission electron microscopy imaging, and electron energy loss spectroscopic characterization. This complex structurecontributes to the high electrochemical stability and good rate capability observed for this compound (160 mAh/g at C/3 and 100mAh/g at 1C).These results provide new insights into the feasibility of developing and commercializing cobalt-free positiveelectrode materials for LIBs

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