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Reaction Mechanism of FePS3 Electrodes in All-Solid-State Lithium Secondary Batteries Using Sulfide-Based Solid Electrolytes

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Title: Reaction Mechanism of FePS3 Electrodes in All-Solid-State Lithium Secondary Batteries Using Sulfide-Based Solid Electrolytes
Authors: Fujii, Yuta Browse this author
Miura, Akira Browse this author →KAKEN DB
Rosero-Navarro, Nataly Carolina Browse this author
Mizuguchi, Yoshikazu Browse this author
Moriyoshi, Chikako Browse this author
Kuroiwa, Yoshihiro Browse this author
Higuchi, Mikio Browse this author →KAKEN DB
Tadanaga, Kiyoharu Browse this author →KAKEN DB
Keywords: All-solid-state battery
Li ion
Issue Date: 15-Sep-2018
Publisher: The Electrochemical Society (ECS)
Journal Title: Journal of The Electrochemical Society
Volume: 165
Issue: 13
Start Page: A2948
End Page: A2954
Publisher DOI: 10.1149/2.0191813jes
Abstract: In this study, we investigated the reaction mechanism of the FePS3 electrode in all-solid-state lithium secondary batteries that utilized sulfide-based solid electrolytes by X-ray diffraction patterns, X-ray absorption spectra, Raman spectra, and density-functional theory (DFT) calculations. In discharge-charge measurements, the reversible discharge-charge reaction (FePS3 + xLi+ + xe− ⇄ LixFePS3, 0 ⩽ x ⩽ 1.5) was confirmed. With this reaction, Li+-inserted FePS3 with low crystallinity was formed with the reduction of iron during the discharge cycle, and crystalline FePS3 appeared along with the oxidation of iron during the charge cycle. Raman spectra showed that P2S64− units were not destroyed during this discharge-charge cycle. In the second cycle, the discharge voltage of the batteries that used FePS3 increased relative to that at the first cycle. The reversible change in chemical states of iron and sulfur was confirmed by X-ray absorption. The first-principle calculation explained the experimental results of the change of crystalline phase and the increase in the discharge voltage. Further, the calculation results indicated that not only iron but also sulfur was oxidized and reduced from the first charge cycle onwards.
Rights: © The Electrochemical Society, Inc. 2018. All rights reserved. Except as provided under U.S. copyright law, this work may not be reproduced, resold, distributed, or modified without the express permission of The Electrochemical Society (ECS). The archival version of this work was published in J. Electrochem. Soc. 2018 volume 165, issue 13, A2948-A2954.
Type: article (author version)
Appears in Collections:工学院・工学研究院 (Graduate School of Engineering / Faculty of Engineering) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 三浦 章

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