Operando Study Insights into Lithiation/Delithiation Processes in a Poly(ethylene oxide) Electrolyte of All-Solid-State Lithium Batteries by Grazing-Incidence X-ray Scattering

作者：Yuxin Liang, Tianle Zheng, Kun Sun, Zhuijun Xu, Tianfu Guan, Fabian A. C. Apfelbeck, Pan Ding, Ian D. Sharp, Ya‐Jun Cheng, Matthias Schwartzkopf, Stephan V. Roth, Peter Müller‐Buschbaum · 发表于：ACS Applied Materials & Interfaces · 年份：2024 · DOI：10.1021/acsami.4c01661 · 被引用次数：14 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Advanced Battery Technologies Research

High Resolution Image Download MS PowerPoint Slide Poly(ethylene oxide) (PEO)-based composite electrolytes (PCEs) are considered as promising candidates for next-generation lithium-metal batteries (LMBs) due to their high safety, easy fabrication, and good electrochemical stability. Here, we utilize operando grazing-incidence small-angle and wide-angle X-ray scattering to probe the correlation of electrochemically induced changes and the buried morphology and crystalline structure of the PCE. Results show that the two irreversible reactions, PEO-Li + reduction and TFSI – decomposition, cause changes in the crystalline structure, array orientation, and morphology of the PCE. In addition, the reversible Li plating/stripping process alters the inner morphology, especially the PEO-LiTFSI domain radius and distance between PEO-LiTFSI domains, rather than causing crystalline structure and orientation changes. This work provides a new path to monitor a working battery in real time and to a detailed understanding of the Li + diffusion mechanism, which is essential for developing highly transferable and interface-stable PCE-based LMBs.