Visualization of the Interfacial Decomposition of Composite Cathodes in Argyrodite-Based All-Solid-State Batteries Using Time-of-Flight Secondary-Ion Mass Spectrometry

作者：Felix Walther, Raimund Koerver, Till Fuchs, Saneyuki Ohno, Joachim Sann, Marcus Rohnke, Wolfgang G. Zeier, Jürgen Janek · 发表于：Chemistry of Materials · 年份：2019 · DOI：10.1021/acs.chemmater.9b00770 · 被引用次数：428 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Advanced Battery Technologies Research

All-solid-state lithium-ion batteries (ASSBs) are expected to represent a future alternative compared to conventional lithium-ion batteries with liquid electrolytes (LIBs). The excellent performance of today’s LIBs relies to a large extent on the development of liquid electrolytes that form stable, or at least slowly degrading, interfaces (interphases) with both anodes and cathodes. This has not yet been achieved in ASSBs, and degradation of anode and cathode interfaces of solid electrolytes (SE) is one of the key issues to be solved. Unlike investigations of liquid/solid interfaces, the degradation of interfaces between the solid electrodes and the SE is challenging since (i) solid/solid interfaces are less easily accessed analytically, (ii) interface compounds may contribute only in very low concentrations to spectroscopic or spectrometric data, and (iii) a high spatial resolution is required to determine the local component distribution. Typically, solid/solid interface investigations are primarily based on electrochemical experiments, diffraction studies, electron microscopy, or on theoretical calculations to obtain sufficient information. Interestingly, the prospects of recent advanced analytical tools such as time-of-flight secondary-ion mass spectrometry (ToF-SIMS) are not fully exploited yet; therefore, we demonstrate in this paper that ToF-SIMS can provide valuable insights into the interphase composition and microstructure of ASSBs. For this purpose, we combine loca...