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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Understanding all-solid-state batteries (ASSBs) requires multi-length scale analysis.
  • Microstructural evolution, including pore formation and contact loss, challenges ASSB studies.
  • Chemical degradation at interfaces significantly impacts ASSB performance.

Purpose of the Study:

  • To investigate the impact of chemical degradation on reaction behavior and microstructural evolution in Ni-rich cathode particles within sulfide-based ASSBs.
  • To evaluate the role of lithium difluorophosphate (LiDFP) in suppressing chemical degradation.

Main Methods:

  • Utilized a model system with LiNi0.6Co0.2Mn0.2O2 cathodes, Li-In alloy anodes, and a non-decomposable coating layer.
  • Employed LiDFP to suppress interfacial chemical degradation.
  • Analyzed reaction uniformity, mechanical degradation, pore formation, and tortuosity.

Main Results:

  • Suppressing chemical degradation with LiDFP enhanced particle reaction uniformity and homogenized mechanical degradation, but increased pore formation and tortuosity.
  • Uncontrolled chemical degradation led to significant reaction heterogeneity and non-uniform mechanical degradation with fewer pores and lower tortuosity.
  • Coating layers are crucial for maintaining cathode surface contact and promoting lithium conduction.

Conclusions:

  • Chemical degradation critically influences reaction and mechanical degradation heterogeneity in ASSBs.
  • LiDFP effectively suppresses chemical degradation, impacting microstructural evolution.
  • Findings emphasize the importance of interfacial engineering and protective coatings for ASSB performance.