Journal Article

FZJ-2022-00266

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Absolute Local Quantification of Li as Function of State-of-Charge in All-Solid-State Li Batteries via 2D MeV Ion-Beam Analysis

Möller, S. (Corresponding author)FZJ* ; Satoh, T. ; Ishii, Y. ; Teßmer, B. ; Guerdelli, R. ; Kamiya, T. ; Fujita, K. ; Suzuki, K. ; Kato, Y. ; Wiemhöfer, H.-D.FZJ* ; Mima, K. ; Finsterbusch, M. (Corresponding author)FZJ*

2021
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Please use a persistent id in citations: http://hdl.handle.net/2128/29985  doi:10.3390/batteries7020041

Abstract: 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.

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Contributing Institute(s):

1. Werkstoffsynthese und Herstellungsverfahren (IEK-1)
2. Helmholtz-Institut Münster Ionenleiter für Energiespeicher (IEK-12)

Research Program(s):

1. 1222 - Components and Cells (POF4-122) (POF4-122)
2. InDiCate - In-situ Analyse der Li-Verteilung in Kathoden (03XP0124A) (03XP0124A)
3. FestBatt-Oxide - Materialplattform 'Oxide' im Rahmen des Kompetenzclusters für Festkörperbatterien (13XP0173A) (13XP0173A)
4. InCa - Interfaces von Mischkathoden in Festkörperbatterien - Fortschrittliche Charakterisierung und Optimierung, Teilvorhaben: Fortschrittliche Ionenstrahlanalytik an Festkörperzellen (13XP0228D) (13XP0228D)

Appears in the scientific report 2021

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