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Imaging the evolution of lithium-solid electrolyte interface using operando scanning electron microscopy.

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The Li-solid electrolyte interface quality is key for solid-state batteries. Operando microscopy reveals Li-Mg alloys form fewer voids than Li, enabling stable cycling at low pressure.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • The solid electrolyte interface (SEI) quality is critical for solid-state lithium metal battery performance, especially under low stack pressure.
  • Understanding SEI dynamics during cell operation is limited by a lack of operando characterization techniques.

Purpose of the Study:

  • To investigate the evolution of the lithium-electrolyte interface with high spatial resolution using operando techniques.
  • To compare the interfacial behavior of lithium metal anodes and lithium-magnesium alloy anodes during stripping.
  • To elucidate the origins of high overpotential in metal anodes and enable stable battery cycling.

Main Methods:

  • Operando scanning electron microscopy (SEM) under realistic operating conditions.
  • Tracking the stripping process of lithium (Li) and Li-rich Li-Mg alloy anodes.
  • Density functional theory (DFT) calculations.
  • Analysis of pressure-dependent voltage profiles during Li and Li-Mg stripping.

Main Results:

  • Operando SEM revealed void coalescence and interface delamination in Li anodes, contrasted with void splitting and partial recovery in Li-Mg anodes.
  • DFT calculations indicated stronger Mg-S interaction in Li-Mg anodes reduces voids by attracting Mg and repelling Li-vacancies.
  • Loss of interfacial contact due to void formation, not Mg accumulation, was identified as the primary cause of high overpotential.

Conclusions:

  • Improved interfacial contact, facilitated by Li-Mg alloy anodes, enables stable cycling of all-solid-state lithium full cells at low stack pressure (1 MPa) and moderate rates (2 mA cm⁻²).
  • Real-time visualization of Li-electrolyte interface dynamics offers crucial insights for designing advanced solid-state battery interfaces.