journal article·2024-07-03Open access

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

Yuxin Liang, Tianle Zheng, Kun Sun, Zhuijun Xu, Tianfu Guan, Fabian A.C. Apfelbeck, Pan Ding, Ian D. Sharp, Yajun Cheng, Matthias Schwartzkopf, Stephan V. Roth, Peter Müller-Buschbaum

ACS Applied Materials & Interfaces· Volume 16· Issue 26

Abstract

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.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced Battery Technologies Research

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Affiliations

TUM School of Natural Sciences, Department of Physics, Chair for Functional Materials, James-Franck-Str. 1, Garching 85748, Germany

Walter Schottky Institute and Physics Department, Technical University of Munich, Am Coulombwall 4, Garching 85748, Germany

Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences, 1219 Zhongguan West Rd, Ningbo, Zhejiang Province 315201, P. R. China

Deutsches Elektronen-Synchrotron DESY, Photon Science, Notkestr. 85, Hamburg 22607, Germany

Department of Fibre and Polymer Technology, KTH Royal Institute of Technology, Teknikringen 56-58, Stockholm SE-100 44, Sweden

Funding

Deutsche Forschungsgemeinschaft · Center for NanoScience, Ludwig-Maximilians-Universit?t M?nchen · Bayerisches Staatsministerium f?r Bildung und Kultus, Wissenschaft und Kunst · China Scholarship Council · National Natural Science Foundation of China · International Research Training Group 2022 Alberta/Technical University of Munich International Graduate School for Environmentally Responsible Functional Hybrid Materials · Center for NanoScience

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