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Quantitative Lithiation Depth Profiling in Silicon Containing Anodes Investigated by Ion Beam Analysis

Authors: Sören Möller; Hyunsang Joo; Marcin Rasinski; Markus Mann; Egbert Figgemeier; Martin Finsterbusch;

Quantitative Lithiation Depth Profiling in Silicon Containing Anodes Investigated by Ion Beam Analysis

Abstract

The localisation and quantitative analysis of lithium (Li) in battery materials, components, and full cells are scientifically highly relevant, yet challenging tasks. The methodical developments of MeV ion beam analysis (IBA) presented here open up new possibilities for simultaneous elemental quantification and localisation of light and heavy elements in Li and other batteries. It describes the technical prerequisites and limitations of using IBA to analyse and solve current challenges with the example of Li-ion and solid-state battery-related research and development. Here, nuclear reaction analysis and Rutherford backscattering spectrometry can provide spatial resolutions down to 70 nm and 1% accuracy. To demonstrate the new insights to be gained by IBA, SiOx-containing graphite anodes are lithiated to six states-of-charge (SoC) between 0–50%. The quantitative Li depth profiling of the anodes shows a linear increase of the Li concentration with SoC and a match of injected and detected Li-ions. This unambiguously proofs the electrochemical activity of Si. Already at 50% SoC, we derive C/Li = 5.4 (< LiC6) when neglecting Si, proving a relevant uptake of Li by the 8 atom % Si (C/Si ≈ 9) in the anode with Li/Si ≤ 1.8 in this case. Extrapolations to full lithiation show a maximum of Li/Si = 1.04 ± 0.05. The analysis reveals all element concentrations are constant over the anode thickness of 44 µm, except for a ~6-µm-thick separator-side surface layer. Here, the Li and Si concentrations are a factor 1.23 higher compared to the bulk for all SoC, indicating preferential Li binding to SiOx. These insights are so far not accessible with conventional analysis methods and are a first important step towards in-depth knowledge of quantitative Li distributions on the component level and a further application of IBA in the battery community.

Country
Germany
Keywords

TK1001-1841, electrochemical stability, garnet solid-state electrolyte, all-solid-state batteries; garnet solid-state electrolyte; lithium-ion transport; electrochemical stability; ion-beam analysis; depth-resolved analysis, all-solid-state batteries, 530, TP250-261, depth-resolved analysis, Production of electric energy or power. Powerplants. Central stations, Industrial electrochemistry, lithium-ion transport, ion-beam analysis, info:eu-repo/classification/ddc/530

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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
3
Average
Average
Average
Green
gold
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Energy Research