Mitigation of Rapid Capacity Decay in Silicon- LiNi0.6Mn0.2Co0.2O2 Full Batteries

Wei Zhang, Seoung-Bum Son, Harvey Guthrey, Chumei Ban

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8 Scopus Citations


Silicon (Si)-based materials have been considered as the most promising anode materials for high-energy-density lithium-ion batteries because of their higher storage capacity and similar operating voltage, as compared to the commercial graphite (Gr) anode. But the use of Si anodes including silicon-graphite (Si-Gr) blended anodes often leads to rapid capacity decay in Si-Gr/LiNixMnyCozO2 (x+y+z=1) full cells, which has been attributed to surface instability of the Si component. In addition to stabilizing the surface, this work investigates the potential of the Si-Gr blended anodes in a full-cell configuration and its impact on the capacity contribution from active components. Using dQ/dV plots of the full cells, a powerful but simple-to-implement differential potential approach is developed to decouple the capacity contribution and degradation from the graphite and silicon components. Data collected from three-electrode cells confirm the results from the differential potential approach, which suggests a voltage slippage to a higher voltage at the blended anode side. The voltage slippage causes a reduced utilization of the Gr component and exacerbates side reactions between the Si-Gr anode and carbonate electrolytes. Furthermore, based on these failure mechanisms, we adopted a mitigation strategy to tune the open circuit voltage of the prelithiated anode while stabilizing the surface. As a result, the full cells with the modified Si-Gr anodes (mass loading, 2.5 mAh/cm2) offer a highly reversible full-cell energy density of 390 Wh/kg (based on the mass of both anode and cathode materials in a full cell) with a cycling CE of 99.9% over 200 cycles.

Original languageAmerican English
Pages (from-to)111-121
Number of pages11
JournalEnergy Storage Materials
StatePublished - 2022

Bibliographical note

Publisher Copyright:
© 2022

NREL Publication Number

  • NREL/JA-5K00-82480


  • Energy storage
  • Lithium-ion batteries
  • Molecular layer deposition
  • Pre-lithiation
  • Silicon anodes
  • Surface modification


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