TY - JOUR AU - Liang, Yuxin AU - Zheng, Tianle AU - Sun, Kun AU - Xu, Zhuijun AU - Guan, Tianfu AU - Apfelbeck, Fabian A. C. AU - Ding, Pan AU - Sharp, Ian D. AU - Cheng, Yajun AU - Schwartzkopf, Matthias AU - Roth, Stephan V. AU - Müller-Buschbaum, Peter TI - 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 JO - ACS applied materials & interfaces VL - 16 IS - 26 SN - 1944-8244 CY - Washington, DC PB - Soc. M1 - PUBDB-2025-00231 SP - 33307-33315 PY - 2024 AB - 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 LB - PUB:(DE-HGF)16 C6 - pmid:38913824 UR - <Go to ISI:>//WOS:001253335500001 DO - DOI:10.1021/acsami.4c01661 UR - https://bib-pubdb1.desy.de/record/622179 ER -