Li2O-Based Cathode Additives Enabling Prelithiation of Si Anodes

Yeyoung Ha, Maxwell Schulze, Sarah Frisco, Stephen Trask, Glenn Teeter, Nathan Neale, Gabriel Veith, Christopher Johnson

Research output: Contribution to journalArticlepeer-review

13 Scopus Citations


Low first-cycle Coulombic efficiency is especially poor for silicon (Si)-based anodes due to the high surface area of the Si-active material and extensive electrolyte decomposition during the initial cycles forming the solid electrolyte interphase (SEI). Therefore, developing successful prelithiation methods will greatly benefit the development of lithium-ion batteries (LiBs) utilizing Si anodes. In pursuit of this goal, in this study, lithium oxide (Li2 O) was added to a LiNi0.6 Mn0.2 Co0.2 O2 (NMC622) cathode using a scalable ball-milling approach to compensate for the initial Li loss at the anode. Different milling conditions were tested to evaluate the impact of particle morphology on the additive performance. In addition, Co3 O4, a well-known oxygen evolution reaction catalyst, was introduced to facilitate the activation of Li2 O. The Li2 O + Co3 O4 additives successfully delivered an additional capacity of 1116 mAh/gLi2O when charged up to 4.3 V in half cells and 1035 mAh/gLi2O when charged up to 4.1 V in full cells using Si anodes.

Original languageAmerican English
Article number12027
Number of pages10
JournalApplied Sciences (Switzerland)
Issue number24
StatePublished - 2021

Bibliographical note

Publisher Copyright:
© 2021 by the authors. Licensee MDPI, Basel, Switzerland.

NREL Publication Number

  • NREL/JA-5K00-80607


  • Cathode additives
  • Cobalt oxide
  • Lithium oxide
  • Lithium-ion batteries
  • Prelithiation
  • Silicon anodes


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