Scientists Decipher the Atomic-Scale Failure Mechanisms of Layered Oxide Cathodes in All-Solid-State Batteries

 
The ever-increasing demand for safety has thrust all-solid-state batteries (ASSBs) into the forefront of next-generation energy storage technologies. However, the atomic-scale mechanisms underlying the failure of layered cathodes in ASSBs, as opposed to their counterparts in liquid electrolyte-based lithium-ion batteries (LIBs), have remained elusive. A research team led by Prof. WANG Chunyang from Institute of Metal Research, Chinese Academy of Sciences (IMR, CAS) and Prof. Huolin Xin from UC Irvine deciphered the atomic origins dictating the chemomechanical degradation of layered oxide cathode materials in ASSBs, by leveraging an artificial intelligence-aided super-resolution transmission electron microscopy (AI-TEM) technique. This work was published in the Journal of the American Chemical Society.

The research discovered that the coupling of surface frustration and interlayer-shear-induced phase transformation exacerbates the chemomechanical breakdown of layered cathodes. Surface frustration, a phenomenon previously unobserved in liquid electrolyte-based LIBs, emerges through electrochemical processes involving surface nanocrystallization coupled with rock salt transformation. Simultaneously, delithiation-induced interlayer shear leads to the formation of chunky O1 phases and intricate interfaces/transition motifs, distinct from scenarios observed in liquid electrolyte-based LIBs. This work provides an unprecedented atomic-scale understanding of the degradation mechanisms of layered oxides in ASSBs and underscores the pivotal role of advanced electron microscopy techniques in addressing core scientific issues in the energy field.


Conceptual Diagram of Resolving Atomic-Scale Failure Mechanisms of Layered Cathodes in ASSBs Using AI-TEM Technique (Image by IMR)

Schematic Overview of the Degradation Mechanisms of Layered Oxide Cathodes in ASSBs (Image by IMR)

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