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Tracking dendrites and solid electrolyte interphase formation with dynamic nuclear polarization—NMR spectroscopy

Author

Listed:
  • Ayan Maity

    (Weizmann Institute of Science)

  • Asya Svirinovsky-Arbeli

    (Weizmann Institute of Science)

  • Yehuda Buganim

    (Weizmann Institute of Science)

  • Chen Oppenheim

    (Weizmann Institute of Science)

  • Michal Leskes

    (Weizmann Institute of Science)

Abstract

Polymer-ceramic composite electrolytes enable safe implementation of Li metal batteries with potentially transformative energy density. Nevertheless, the formation of Li-dendrites and its complex interplay with the Li-metal solid electrolyte interphase (SEI) remain a substantial obstacle which is poorly understood. Here we tackle this issue by a combination of solid-state NMR spectroscopy and Overhauser dynamic nuclear polarization (DNP) which boosts NMR interfacial sensitivity through polarization transfer from the metal conduction electrons. We achieve detailed molecular-level insight into dendrites formation and propagation within the composites and determine the composition and properties of their SEI. We find that the dendrite’s quantity and growth path depend on the ceramic content and correlated with battery’s lifetime. We show that the enhancement of Li resonances in the SEI occurs through Li/Li+ charge transfer in Overhauser DNP, allowing us to correlate DNP enhancements and Li transport and directly determine the SEI lithium permeability. These findings have promising implications for SEI design and dendrites management which are essential for the realization of Li metal batteries.

Suggested Citation

  • Ayan Maity & Asya Svirinovsky-Arbeli & Yehuda Buganim & Chen Oppenheim & Michal Leskes, 2024. "Tracking dendrites and solid electrolyte interphase formation with dynamic nuclear polarization—NMR spectroscopy," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54315-w
    DOI: 10.1038/s41467-024-54315-w
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    1. Michael A. Hope & Bernardine L. D. Rinkel & Anna B. Gunnarsdóttir & Katharina Märker & Svetlana Menkin & Subhradip Paul & Ivan V. Sergeyev & Clare P. Grey, 2020. "Selective NMR observation of the SEI–metal interface by dynamic nuclear polarisation from lithium metal," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
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