4.6 Article

Investigating phase transformation in the Li1.2Co0.1Mn0.55Ni0.15O2 lithium-ion battery cathode during high-voltage hold (4.5 V) via magnetic, X-ray diffraction and electron microscopy studies

期刊

JOURNAL OF MATERIALS CHEMISTRY A
卷 1, 期 20, 页码 6249-6261

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/c3ta10304h

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  1. U.S. Department of Energy (DOE) [DE-AC05-00OR22725]
  2. Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office's Applied Battery Research Program
  3. DOE, Basic Energy Sciences, Materials Sciences and Engineering Division
  4. ORNL's ShaRE User Facility
  5. Scientific User Facilities Division, Office of Basic Energy Sciences, DOE
  6. DOE Vehicle Technologies Office (VTO)

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This study is the first that provides evidence of phase transformation in a Li-rich Li1.2Co0.1Mn0.55Ni0.15O2 cathode material for lithium-ion batteries (LIBs) during constant voltage charging. Diffraction and magnetic measurement techniques were successfully implemented to investigate the structural transformation in this cathode material during holding a half-cell at 4.5 V in a charged state. The results from X-ray diffraction showed a decrease in c-lattice parameters during high-voltage hold. Magnetic data revealed an increase in average effective magnetic moments of transition metal (TM) ions at constant voltage corresponding to a change in electronic states of TM ions. Analysis showed the reduction of Ni4+ to Ni2+, which was attributed to charge compensation due to oxygen loss. The appearance of the strong {1010} forbidden reflection in the single-crystal selected area electron diffraction (SAED) data was attributed to migration of transition metal ions to the octahedral vacancy sites in the lithium layer during high-voltage hold, which was in agreement with the magnetization results. After prolonged hold at 4.5 V, high-resolution transmission electron microscopy (TEM) images along with SAED results showed the presence of spinel phases in the particles, indicating a layered to spinel like phase transformation at constant voltage in agreement with the magnetic data. The results obtained from these magnetic and diffraction studies furnish the fundamental understanding of the structural transformation pathways in Li-rich cathodes at constant voltage and will be instrumental for modifying the parent structure to achieve greater stability.

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