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Welding surface epitaxial layer enables high-loading sulfide all-solid-state batteries.

Zhuomin Qiang1, Yanbin Ning1, Wei Zhao1

  • 1State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China.

Science Bulletin
|November 6, 2025
PubMed
Summary
This summary is machine-generated.

We stabilized high-nickel cathodes in sulfide all-solid-state batteries using an in situ indium oxide coating. This surface engineering approach prevents side reactions and structural damage, enhancing battery performance and longevity.

Keywords:
Chemo-mechanical failureSolid-state batteriesSulfide electrolyteUltrahigh-Ni layered oxides

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Ultrahigh-nickel layered oxide cathodes (e.g., LiNi0.9Co0.05Mn0.05O2 or NCM90) exhibit high energy density but suffer from surface reactivity and strain issues in sulfide all-solid-state batteries (ASSLBs).
  • These challenges lead to interfacial instability and structural degradation, limiting the practical application of high-energy density cathodes in ASSLBs.

Purpose of the Study:

  • To develop an effective surface modification strategy for ultrahigh-nickel layered oxide cathodes to improve their stability and electrochemical performance in sulfide ASSLBs.
  • To investigate the mechanism by which the proposed surface treatment mitigates interfacial side reactions and structural fatigue.

Main Methods:

  • An in situ transformation strategy using indium oxide (In₂O₃) was employed to treat the NCM90 cathode surface.
  • The treated cathode was characterized using advanced techniques including synchrotron X-ray tomography (micro-/nano-CT) and X-ray absorption near-edge structure (XANES).
  • Electrochemical performance was evaluated in sulfide ASSLBs with high cathode loading (9 mg cm⁻²).

Main Results:

  • The in situ indium oxide treatment successfully captured residual lithium impurities and reconstructed the near-surface structure, forming a conformal epitaxial layer.
  • This reconstructed layer effectively suppressed spontaneous side reactions at the cathode-electrolyte interface and prevented bulk structural fatigue.
  • The modified NCM90 cathodes in ASSLBs achieved a high reversible capacity of ~2 mAh cm⁻² (>190 mAh g⁻¹ at 0.069 mA cm⁻²), excellent cycling stability, and good rate capability.
  • Multi-scale observations confirmed significantly alleviated interfacial instability and chemo-mechanical disintegration.

Conclusions:

  • Surface engineering via in situ indium oxide transformation is a crucial strategy for stabilizing ultrahigh-nickel layered cathodes.
  • This approach enhances the electrochemical performance and cycling stability of ASSLBs, paving the way for high-energy density applications.
  • The findings underscore the importance of addressing interfacial phenomena for the advancement of next-generation solid-state batteries.