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Local crystallization inside the polymer electrolyte for lithium metal batteries observed by operando nanofocus WAXS
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Local crystallization inside the polymer electrolyte for lithium metal batteries observed by operando nanofocus WAXS
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Journal Article
Local crystallization inside the polymer electrolyte for lithium metal batteries observed by operando nanofocus WAXS
2025
Overview
The development of next-generation lithium-based batteries is accompanied by the intention to suppress the formation of dendritic lithium on the electrode, and is dominated by the picture that dendrites start to grow at the electrodes. Shifting from liquid to solid-state electrolytes, a high transference number is a quantity that promises the restraint of such parasitic side reactions. In this study, nanofocus X-ray wide-angle scattering is used to detect possible lithium-based crystallites in the polymer-based electrolyte. We perform
operando
scanning nanofocus wide-angle X-ray scattering on a composite gel-type polymer consisting of poly(vinylidene fluoride-co-hexafluoropropylene) and the single-ion conducting polymer poly((trifluoromethane) sulfonimide lithium styrene) in a lithium symmetric cell. We observe the occurrence and kinetics of lithium carbonate crystallites inside the electrolyte over a depth of 16 µm during three half-cycles. Furthermore, we prove the existence of lithium hydroxide crystallites near the lithium electrode and their absence in the bulk. Importantly, we identify the growth of pure metallic lithium inside the electrolyte as a sign of lithium dendrite growth happening inside the polymer-based electrolyte and not at the electrodes. Thus, nanofocus wide-angle X-ray scattering visualizes local structure changes such as dendrite formation inside the polymer-based electrolyte despite an unchanged electrochemical performance.
Polymer electrolytes are promising candidates as separators in lithium metal batteries. Here, authors reveal the existence of local lithium-based crystallites inside the polymer electrolyte in a lithium symmetric cell. A combination of unique operando wide-angle X-ray scattering with a nano-sized beam and complementary spectroscopic techniques identifies these crystallites as lithium carbonate, lithium hydroxide, and even metallic lithium. It is shown that these crystallites lower the ionic conductivity and the transference number.
