High-Voltage Deprotonation of Layered-Type Materials as a Newly Identified Cause of Electrode Degradation

Junghoon Yang, Sungwon Park, Sungsik Lee, Jungpil Kim, Di Huang, Jihyeon Gim, Eungje Lee, Gilseob Kim, Kyusung Park, Yong-Mook Kang, Eunsu Paek, Sang-Don Han

Research output: Contribution to journalArticlepeer-review

4 Scopus Citations


Further development of electrochemical devices and electric vehicles requires advanced secondary batteries with higher energy density, longer lifetime and enhanced thermal safety. Increasing the cell operating voltage is one of the realistic strategies to extend the energy density, but it is inevitably accompanied by irreversible structural changes and mechanical failure of the electrode materials and continuous parasitic reactions within the electrode-electrolyte interface resulting in capacity fading and subsequent battery failure along with safety issues. Herein, we report deprotonation of layered-type materials at high voltages (>4.5 V vs. Li/Li+) as a newly identified cause of electrode degradation, which has not been addressed previously. Electrochemical analysis and diagnostics combined with advanced characterization studies and computational simulations were employed to understand deprotonation mechanisms and investigate the effect of the deprotonation process on the electrode during high voltage operation. We demonstrated that protons act as charge carriers in lithium (Li)-free materials through the deprotonation process during the initial charging. In addition, this study shows that the deprotonation process is dependent upon transition metals and accordingly deteriorates the electrode by changing its structure and electrochemical properties.
Original languageAmerican English
Pages (from-to)3018-3027
Number of pages10
JournalJournal of Materials Chemistry A
Issue number6
StatePublished - 2023

NREL Publication Number

  • NREL/JA-5900-83071


  • deprotonation
  • electrode degradation
  • high voltage
  • layered hydroxide
  • rechargeable batteries


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