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PreprintCC BYChemRxiv

Atomistic Origin of Transition-Metal Dissolution in Ni-Rich Cathodes: The Role of Oxygen Loss

  • Michael Woodcox1,2
  • Nickil A. Shah3
  • Eleni Fiamegkou3,4
  • Pardeep K. Thakur5,6
  • Tien-Lin Lee5,6
  • Galo Paez Fajardo3,4
  • Louis F. J. Piper3,4
6 affiliations
  1. 1Material Measurement Laboratory
  2. 2National Institute of Standards and Technology
  3. 3University of Warwick
  4. 4Faraday Institution
  5. 5Harwell Science and Innovation Campus
  6. 6Diamond Light Source Ltd.,
Open at sourceDOICite

Abstract

High-voltage operation of Ni-rich cathodes accelerates degradation through surface reconstruction and transition-metal dissolution. Although these processes occur concurrently, their mechanistic relationship remains unresolved. Here, we identify oxygen loss as the unifying mechanism coupling cathode surface reconstruction and transition-metal release in LiNi0.8Mn0.1Co0.1O2||graphite cells, consistent with the increased Ni deposition observed at the graphite anode. Surface-sensitive Ni L-edge X-ray absorption spectroscopy reveals that crossing the oxygen-loss threshold not only induces cathode surface reconstruction, but also progressively thins the reconstructed surface layer, evidenced by the evolution of signal attenuation. Ab initio molecular dynamics simulations corroborate this interpretation by showing that reconstructed-layer thinning originates from energetically favorable surface-layer detachment following oxygen-loss-driven destabilization of the near-surface lattice. Together, these findings establish oxygen loss as the mechanistic origin of coupled cathode degradation and transition-metal deposition, and identify stabilization of lattice oxygen as a key materials-engineering strategy to mitigate degradation and extend the cycling performance of next-generation Ni-rich Li-based energy storage devices.

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Cite

BibTeXRIS
BibTeX
@misc{woodcox2026atomistic,
  title = {{Atomistic Origin of Transition-Metal Dissolution in Ni-Rich Cathodes: The Role of Oxygen Loss}},
  author = {Michael Woodcox and Nickil A. Shah and Eleni Fiamegkou and Pardeep K. Thakur and Tien-Lin Lee and Galo Paez Fajardo and Louis F. J. Piper},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15010806/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010806/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Atomistic Origin of Transition-Metal Dissolution in Ni-Rich Cathodes: The Role of Oxygen Loss
AU  - Michael Woodcox
AU  - Nickil A. Shah
AU  - Eleni Fiamegkou
AU  - Pardeep K. Thakur
AU  - Tien-Lin Lee
AU  - Galo Paez Fajardo
AU  - Louis F. J. Piper
PY  - 2026
DA  - 2026/10/21
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15010806/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010806/v1
AB  - High-voltage operation of Ni-rich cathodes accelerates degradation through surface reconstruction and transition-metal dissolution. Although these processes occur concurrently, their mechanistic relationship remains unresolved. Here, we identify oxygen loss as the unifying mechanism coupling cathode surface reconstruction and transition-metal release in LiNi0.8Mn0.1Co0.1O2||graphite cells, consistent with the increased Ni deposition observed at the graphite anode. Surface-sensitive Ni L-edge X-ray absorption spectroscopy reveals that crossing the oxygen-loss threshold not only induces cathode surface reconstruction, but also progressively thins the reconstructed surface layer, evidenced by the evolution of signal attenuation. Ab initio molecular dynamics simulations corroborate this interpretation by showing that reconstructed-layer thinning originates from energetically favorable surface-layer detachment following oxygen-loss-driven destabilization of the near-surface lattice. Together, these findings establish oxygen loss as the mechanistic origin of coupled cathode degradation and transition-metal deposition, and identify stabilization of lattice oxygen as a key materials-engineering strategy to mitigate degradation and extend the cycling performance of next-generation Ni-rich Li-based energy storage devices.
ER  -