%0 Journal Article %A Liang, Yuxin %A Zheng, Tianle %A Sun, Kun %A Xu, Zhuijun %A Guan, Tianfu %A Apfelbeck, Fabian A. C. %A Ding, Pan %A Sharp, Ian D. %A Cheng, Yajun %A Schwartzkopf, Matthias %A Roth, Stephan V. %A Müller-Buschbaum, Peter %T 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 %J ACS applied materials & interfaces %V 16 %N 26 %@ 1944-8244 %C Washington, DC %I Soc. %M PUBDB-2025-00231 %P 33307-33315 %D 2024 %X 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<sup>+</sup> 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<sup>+</sup> diffusion mechanism, which is essential for developing highly transferable and interface-stable PCE-based LMBs %F PUB:(DE-HGF)16 %9 Journal Article %$ pmid:38913824 %U <Go to ISI:>//WOS:001253335500001 %R 10.1021/acsami.4c01661 %U https://bib-pubdb1.desy.de/record/622179