Reaction Mechanism of Li2MnO3 Electrodes in an All-Solid-State Thin-Film Battery Analyzed by Operando Hard X-ray Photoelectron Spectroscopy
- Kazuhiro HikimaKazuhiro HikimaDepartment of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, JapanDepartment of Electrical and Electronic Information Engineering, Toyohashi University of Technology, 1-1 Hibarigaoka, Tempaku, Toyohashi, Aichi 441-8580, JapanMore by Kazuhiro Hikima
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- Keisuke ShimizuKeisuke ShimizuResearch Center for All-Solid-State Battery, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, JapanMore by Keisuke Shimizu
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- Hisao KiuchiHisao KiuchiOffice of Society-Academia Collaboration for Innovation, Kyoto University, Kyoto 611-0011, JapanMore by Hisao Kiuchi
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- Yoyo HinumaYoyo HinumaResearch Center for All-Solid-State Battery, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, JapanResearch Institute of Electrochemical Energy, Department of Energy and Environment, National Institute of Advanced Industrial Science and Technology (AIST), 1-8-31, Midorigaoka, Ikeda, Osaka 563-8577, JapanMore by Yoyo Hinuma
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- Kota SuzukiKota SuzukiDepartment of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, JapanResearch Center for All-Solid-State Battery, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, JapanMore by Kota Suzuki
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- Masaaki HirayamaMasaaki HirayamaDepartment of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, JapanResearch Center for All-Solid-State Battery, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, JapanMore by Masaaki Hirayama
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- Eiichiro MatsubaraEiichiro MatsubaraDepartment of Materials Science and Engineering, Kyoto University, Kyoto 606-8501, JapanMore by Eiichiro Matsubara
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- Ryoji Kanno*Ryoji Kanno*(R.K.) Phone: +81-459245401. Fax: +81-459245403. Email: [email protected]Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, JapanResearch Center for All-Solid-State Battery, Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, JapanMore by Ryoji Kanno
Abstract
Li2MnO3 is a promising cathode candidate for Li-ion batteries because of its high discharge capacity; however, its reaction mechanism during cycling has not been sufficiently explicated. Observations of Mn and O binding energy shifts in operando hard X-ray photoelectron spectroscopy measurements enabled us to determine the charge-compensation mechanism of Li2MnO3. The O 1s peak splits at an early stage during the first charge, and the concentration of lower-valence O changes reversibly with cycling, indicating the formation of a low-valence O species that intrinsically participates in the redox reaction. The O 1s peak-splitting behavior, which indicates the number of valences of O in Li2MnO3, is supported by the computational results for an O3 to O1 structural transition. This is in agreement with the results of our previous study, wherein we confirmed this O3 to O1 transition based on in situ surface X-ray diffraction analysis, X-ray photoelectron spectroscopy, and first-principles formation energy calculations.
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