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Unravelling the convoluted and dynamic interphasial mechanisms on Li metal anodes. | LitMetric

AI Article Synopsis

  • This study reveals that the formation of the solid-electrolyte interphase (SEI) on lithium metal anodes is influenced by a variety of factors, including the electrolyte, cathode, moisture, and native surface species, rather than just the reactions between lithium and the electrolyte.
  • Using advanced techniques like synchrotron-based X-ray diffraction, researchers discovered that lithium hydroxide (LiOH) from the surface of lithium contributes significantly to the creation of lithium hydride (LiH) under different conditions, affecting battery performance.
  • The findings suggest that the typical high-performance SEI associated with concentrated electrolytes can also form in lower concentration settings due to interactions during cycling, which may

Article Abstract

Accurate understanding of the chemistry of solid-electrolyte interphase (SEI) is key to developing new electrolytes for high-energy batteries using lithium metal (Li) anodes. SEI is generally believed to be formed by the reactions between Li and electrolyte. However, our new study shows this is not the whole story. Through synchrotron-based X-ray diffraction and pair distribution function analysis, we reveal a much more convoluted formation mechanism of SEI, which receives considerable contributions from electrolyte, cathode, moisture and native surface species on Li, with highly dynamic nature during cycling. Using isotope labelling, we traced the origin of LiH to electrolyte solvent, moisture and a new source: the native surface species (LiOH) on pristine Li. When lithium accessibility is very limited as in the case of anode-free cells, LiOH develops into plate-shaped large crystals during cycling. Alternatively, when the lithium source is abundant, as in the case of Li||NMC811 cells, LiOH reacts with Li to form LiH and LiO. While the desired anion-derived LiF-rich SEI is typically found in the concentrated electrolytes or their derivatives, we found it can also be formed in low-concentration electrolyte via the crosstalk effect, emphasizing the importance of formation cycle protocol and opening up opportunities for low-cost electrolyte development.

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Source
http://dx.doi.org/10.1038/s41565-022-01273-3DOI Listing

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