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Electrochemical degradation of solid electrolytes is a major roadblock in thedevelopment of solid-state batteries, and the formed solid-solid interphase(SSI) plays a key role in the performance of solid-state batteries. In thisstudy, by combining experimental X-ray absorption spectroscopy (XAS)measurements, first-principles simulations, and unsupervised machine learning,we have unraveled the atomic-scale oxidative degradation mechanisms of sulfideelectrolytes at the interface using the baseline Li3PS4 (LPS) electrolyte as amodel system. The degradation begins with a decrease of Li neighbor affinity toS atoms upon initial delithiation, followed by the formation of S-S bonds asthe PS4 tetrahedron deforms. After the first delithiation cycle, the PS4 motifsbecome strongly distorted and PS3 motifs start to form. Spectral fingerprintsof the local structural evolution are identified, which correspond to the mainpeak broadening and the peak shifting to a higher energy by about 2.5 eV in PK-edge XAS and a new peak emerging at 2473 eV in S K-edge XAS duringdelithiation. The spectral fingerprints serve as a proxy for theelectrochemical stability of phosphorus sulfide solid electrolytes beyond LPS,as demonstrated in argyrodite Li6PS5Cl. We observed that the strong distortionand destruction of PS4 tetrahedra and the formation of S-S bonds are correlatedwith an increased interfacial impedance. To the best of our knowledge, thisstudy showcases the first atomic-scale insights into the oxidative degradationmechanism of the LPS electrolyte, which can provide guidance for controllingmacroscopic reactions through microstructural engineering and, more generally,can advance the rational design of sulfide electrolytes.

Atomic Insights into the Oxidative Degradation Mechanisms of Sulfide Solid Electrolytes