Unravelling the Chemistry and Microstructure Evolutionof a Cathodic Interface in Sulfide-Based All-Solid-State Li-Ion Batteries

Abstract

All-solid-state lithium-ion batteries (SSLIBs) are promising candidates to meet the requirement of electric vehicles due to the intrinsic safety characteristics and high theoretical energy density. A stable cathodic interface is critical for maximizing the performance of SSLIBs. In this study, operando X-ray absorption near-edge spectroscopy (XANES) combined with transmission electron microscopy (TEM) and electron energy loss spectroscopy (EELS) is employed to investigate the interfacial behavior between the Ni-rich layered cathodes and sulfide solid-state electrolyte. The study demonstrates a metastable intermediate state of sulfide electrolyte at high voltage and parasitic reactions with cathodes during the charge/discharge process, which leads to the surface structural reconstruction of Ni-rich cathodes. Constructing a uniform interlayer by atomic layer deposition (ALD) is also employed in this study to further investigate the cathodic interface stability. These results provide new insight into the cat...