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Title: Exploring Lithium-Cobalt-Nickel Oxide Spinel Electrodes for ≥3.5 V Li-Ion Cells

Some recent reports have indicated that a manganese oxide spinel component, when embedded in a relatively small concentration in layered xLi 2MnO 3center dot(1-x)LiMO 2 (M = Ni, Mn, or Co) electrode systems, can act as a stabilizer that increases their capacity, rate capability, cycle life, and first-cycle efficiency. Our findings prompted us to explore the possibility of exploiting lithiated cobalt oxide spinel stabilizers by taking advantage of (1) the low mobility of cobalt ions relative to that of manganese and nickel ions in close-packed oxides and (2) their higher potential (similar to 3.6 V vs Li0) relative to manganese oxide spinels (similar to 2.9 V vs Li0) for the spinel-to-lithiated spinel electrochemical reaction. In particular, we revisited the structural and electrochemical properties of lithiated spinels in the LiCo 1-xNi xO 2 (0 <= x <= 0.2) system, first reported almost 25 years ago, by means of high-resolution (synchrotron) X-ray diffraction, transmission electron microscopy, nuclear magnetic resonance spectroscopy, electrochemical cell tests, and theoretical calculations. These results provide a deeper understanding of the complexity of intergrown layered/lithiated spinel LiCo 1-xNi xO 2 structures when prepared in air between 400 and 800 degrees C and the impact of structural variations on theirmore » electrochemical behavior. These structures, when used in low concentrations, offer the possibility of improving the cycling stability, energy, and power of high energy (>= 3.5 V) lithium-ion cells.« less
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  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering, NUANCE Center
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
AC02-06CH11357; AC02-05CH11231
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 8; Journal Issue: 41; Journal ID: ISSN 1944-8244
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; lithium-cobalt-nickel oxide; lithium-ion battery; spinel; stabilizer; structure
OSTI Identifier: