@misc{1b95689b-4cb7-4e7d-ae24-f22e1fa0902a,
  abstract     = {{Cathode–solid electrolyte (SE) interfacial stability issues pose a <br>
significant challenge to stable and high-power operations of <br>
all-solid-state batteries, which promise greater energy density, thermal<br>
 stability, and safety than the current liquid electrolyte-based Li-ion <br>
technology. For technologically important Ni-rich NMCs (LiNixMnyCozO2 or<br>
 NMCxyz; x/y/z: Ni/Mn/Co stoichiometry) with sulfide SEs, redox-mediated<br>
 instability of the SE is often blamed for rapid cathode deterioration. <br>
Here, in-depth spectroscopic and electrochemical analyses of Ni-rich <br>
NMCs with a promising sulfide SE reveal rapid interfacial degradations <br>
underpinned by hitherto unknown selective Ni leaching from the NMC <br>
particles, sparking accelerated capacity fading and poor thermal <br>
stability. We demonstrate that introducing a functionalized conductive <br>
carbon in the cathode subdues the oxidative degradation of the sulfide <br>
SE into reactive polysulfides that trigger the NMC degradation. <br>
Consequently, NMC622 and NMC811-based cells display attractive active <br>
material utilization, enhanced stability, and excellent rate capability <br>
and thermal stability – together with a very high average Coulombic <br>
efficiency of 99.8% even for high-temperature cycling, which otherwise <br>
compounds cycling instability. This study unveils a previously <br>
unforeseen interfacial degradation of a technologically critical <br>
cathode-SE combination and presents a scalable approach to its in situ <br>
regulation, enabling remarkable performance improvement.}},
  author       = {{Bhadra, Abhirup and Otabil Bonsu, Jacob and Brunisholz, Maxime and Luo, Tongjun and Thomsen, Lars and Dose, Wesley and Kundu, Dipan}},
  language     = {{eng}},
  month        = {{03}},
  note         = {{Preprint}},
  publisher    = {{ChemRxiv}},
  title        = {{First Observation and Mitigation of Ni-Leaching Mediated Degradation to Enhance Stability of Ni-rich Layered Cathodes in Solid-State Batteries}},
  url          = {{http://dx.doi.org/10.26434/chemrxiv-2025-r1nf2}},
  doi          = {{10.26434/chemrxiv-2025-r1nf2}},
  year         = {{2025}},
}