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Article Dependency of the Charge–Discharge Rate on Lithium Reaction Distributions for a Commercial Lithium Coin Cell Visualized by Compton Scattering Imaging Kosuke Suzuki 1,* , Ryo Kanai 1, Naruki Tsuji 2, Hisao Yamashige 3, Yuki Orikasa 4, Yoshiharu Uchimoto 5, Yoshiharu Sakurai 2 and Hiroshi Sakurai 1 1 2 3 4 5 uchimoto.yoshiharu.2n@kyoto-u.ac.jp Graduate School of Science and Technology, Gunma University, Kiryu, Gunma 376-8515, Japan; t161d023@gunma-u.ac.jp (R.K.); sakuraih@gunma-u.ac.jp (H.S.) Japan Synchrotron Radiation Research Institute (JASRI), SPring-8, Sayo, Hyogo 679-5198, Japan; ntsuji@spring8.or.jp (N.T.); sakurai@spring8.or.jp (Y.S.) Material Platform Engineering Division, Toyota Motor Corporation, Toyota, Aichi 471-8572, Japan; hisao_yamashige@mail.toyota.co.jp Department of Applied Chemistry, Ritsumeikan University, Kusatsu, Shiga 525-8577, Japan; orikasa@fc.ritsumei.ac.jp Graduate School of Human and Environmental Studies, Kyoto University, Sakyo, Kyoto 606-8501, Japan; * Correspondence: kosuzuki@gunma-u.ac.jp; Tel.: +81-277-30-1714 Received: 23 August 2018; Accepted: 13 September 2018; Published: 19 September 2018 Abstract: In this study, lithium reaction distributions, dependent on the charge–discharge rate, were non-destructively visualized for a commercial lithium-ion battery, using the Compton scattering imaging technique. By comparing lithium reaction distributions obtained at two different charge–discharge speeds, residual lithium ions were detected at the center of the negative electrode in a fully discharged state, at a relatively high-speed discharge rate. Moreover, we confirmed that inhomogeneous reactions were facilitated at a relatively high-speed charge–discharge rate, in both the negative and positive electrodes. A feature of our technique is that it can be applied to commercially used lithium-ion batteries, because it uses high-energy X-rays with high penetration power. Our technique thus opens a novel analyzing pathway for developing advanced batteries. Keywords: lithium reaction distribution; in-operando measurement; Compton scattering imaging 1. Introduction Although lithium-ion rechargeable batteries are already widely used in our daily life, demand for them is rapidly increasing, since the development of electric vehicles is attracting much attention all over the world. To further expand the use of electric vehicles, batteries require not only high capacities, but also high safety and long lifetimes. Moreover, people expect fast-charging batteries at a similar refueling speed as in the gasoline car. However, in a previous neutron diffraction study, it was reported that inhomogeneous reactions occur in the graphite-negative electrode at a high-speed charge–discharge rate [1]. These inhomogeneous reactions are related to the degradation of the battery performance; furthermore, they carry some great risks. Therefore, it is important to monitor lithium reactions directly in the batteries under in situ or in operando conditions. Although the neutron diffraction technique is a powerful tool for in operando measurement, it reveals the reaction mechanism through the change of the lattice parameter in the electrode materials. Condens. Matter 2018, 3, 27; doi:10.3390/condmat3030027 www.mdpi.com/journal/condensedmatterPDF Image | Dependency of the Charge–Discharge Rate on Lithium Reaction Distributions
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