Absolute Local Quantification of Li as Function of State-of-Charge in All-Solid-State Li Batteries via 2D MeV Ion-Beam Analysis
Sören Möller,
Takahiro Satoh,
Yasuyuki Ishii,
Britta Teßmer,
Rayan Guerdelli,
Tomihiro Kamiya,
Kazuhisa Fujita,
Kota Suzuki,
Yoshiaki Kato,
Hans-Dieter Wiemhöfer,
Kunioki Mima,
Martin Finsterbusch
Affiliations
Sören Möller
Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), Forschungszentrum Jülich GmbH, Wilhelm Johnen Str., 52425 Jülich, Germany
Takahiro Satoh
National Institutes for Quantum and Radiological Science and Technology, 1233 Watanuki-machi, Takasaki 370-1292, Gunma, Japan
Yasuyuki Ishii
National Institutes for Quantum and Radiological Science and Technology, 1233 Watanuki-machi, Takasaki 370-1292, Gunma, Japan
Britta Teßmer
MEET—Münster Electrochemical Energy Technology, Corrensstraße 46, 48149 Münster, Germany
Rayan Guerdelli
Institute of Energy and Climate Research, Helmholtz-Institute Münster (IEK-12), Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
Tomihiro Kamiya
Graduate School of Science and Technology, Gunma University, 1-5-1 Tenjin-cho, Kiryu 376-8515, Gunma, Japan
Kazuhisa Fujita
The Graduate School for the Creation of New Photonics, 1955-1 Kurematsu, Nishiku, Hamamatsu 431-1202, Shizuoka, Japan
Kota Suzuki
Department of Chemical Science and Engineering—School of Materials and Chemical Technology, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, Kanagawa, Japan
Yoshiaki Kato
Institute of Laser Engineering, Osaka University, 2-6 Yamadaoka, Suita 565-0871, Osaka, Japan
Hans-Dieter Wiemhöfer
Institute of Energy and Climate Research, Helmholtz-Institute Münster (IEK-12), Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
Kunioki Mima
Institute of Laser Engineering, Osaka University, 2-6 Yamadaoka, Suita 565-0871, Osaka, Japan
Martin Finsterbusch
Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), Forschungszentrum Jülich GmbH, Wilhelm Johnen Str., 52425 Jülich, Germany
Direct observation of the lithiation and de-lithiation in lithium batteries on the component and microstructural scale is still difficult. This work presents recent advances in MeV ion-beam analysis, enabling quantitative contact-free analysis of the spatially-resolved lithium content and state-of-charge (SoC) in all-solid-state lithium batteries via 3 MeV proton-based characteristic x-ray and gamma-ray emission analysis. The analysis is demonstrated on cross-sections of ceramic and polymer all-solid-state cells with LLZO and MEEP/LIBOB solid electrolytes. Different SoC are measured ex-situ and one polymer-based operando cell is charged at 333 K during analysis. The data unambiguously show the migration of lithium upon charging. Quantitative lithium concentrations are obtained by taking the physical and material aspects of the mixed cathodes into account. This quantitative lithium determination as a function of SoC gives insight into irreversible degradation phenomena of all-solid-state batteries during the first cycles and locations of immobile lithium. The determined SoC matches the electrochemical characterization within uncertainties. The presented analysis method thus opens up a completely new access to the state-of-charge of battery cells not depending on electrochemical measurements. Automated beam scanning and data-analysis algorithms enable a 2D quantitative Li and SoC mapping on the µm-scale, not accessible with other methods.
