High-Voltage-Driven Surface Structuring and Electrochemical Stabilization of Ni-Rich Layered Cathode Materials for Li Rechargeable Batteries

Seok Hyun Song, Moses Cho, Inchul Park, Jong Gyu Yoo, Kyung Tae Ko, Jihyun Hong, Jongsoon Kim, Sung Kyun Jung, Maxim Avdeev, Sungdae Ji, Seongsu Lee, Joona Bang, Hyungsub Kim

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2 Citations (Scopus)

Abstract

Layered lithium–nickel–cobalt–manganese oxide (NCM) materials have emerged as promising alternative cathode materials owing to their high energy density and electrochemical stability. Although high reversible capacity has been achieved for Ni-rich NCM materials when charged beyond 4.2 V versus Li+/Li, full lithium utilization is hindered by the pronounced structural degradation and electrolyte decomposition. Herein, the unexpected realization of sustained working voltage as well as improved electrochemical performance upon electrochemical cycling at a high operating voltage of 4.9 V in the Ni-rich NCM LiNi0.895Co0.085Mn0.02O2 is presented. The improved electrochemical performance at a high working voltage at 4.9 V is attributed to the removal of the resistive Ni2+O rock-salt surface layer, which stabilizes the voltage profile and improves retention of the energy density during electrochemical cycling. The manifestation of the layered Ni2+O rock-salt phase along with the structural evolution related to the metal dissolution are probed using in situ X-ray diffraction, neutron diffraction, transmission electron microscopy, and X-ray absorption spectroscopy. The findings help unravel the structural complexities associated with high working voltages and offer insight for the design of advanced battery materials, enabling the realization of fully reversible lithium extraction in Ni-rich NCM materials.

Original languageEnglish
Article number2000521
JournalAdvanced Energy Materials
Volume10
Issue number23
DOIs
Publication statusPublished - 2020 Jun 1

Keywords

  • Li-ion batteries
  • Ni-rich NCM
  • cathodes
  • high voltages
  • surface stabilization

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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    Song, S. H., Cho, M., Park, I., Yoo, J. G., Ko, K. T., Hong, J., Kim, J., Jung, S. K., Avdeev, M., Ji, S., Lee, S., Bang, J., & Kim, H. (2020). High-Voltage-Driven Surface Structuring and Electrochemical Stabilization of Ni-Rich Layered Cathode Materials for Li Rechargeable Batteries. Advanced Energy Materials, 10(23), [2000521]. https://doi.org/10.1002/aenm.202000521