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Effect of current density on the solid electrolyte interphase formation at the lithium∣Li6PS5Cl interface.

Sudarshan Narayanan1,2, Ulderico Ulissi3, Joshua S Gibson1,2

  • 1Department of Materials, University of Oxford, Oxford, OX1 3PH, UK.

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Lithium plating current density influences the solid electrolyte interphase (SEI) formation on solid-state electrolytes. A uniform, Li3P-rich SEI, achieved via optimized plating, reduces interfacial resistance for better all-solid-state lithium batteries.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Developing reliable all-solid-state lithium batteries requires understanding the solid electrolyte interphase (SEI) at the lithium metal electrode interface.
  • The chemical composition and morphology of the SEI significantly impact battery performance and longevity.

Purpose of the Study:

  • To investigate the influence of lithium plating current density on SEI formation.
  • To elucidate the chemical and morphological evolution of the SEI on Li6PS5Cl solid-state electrolytes.
  • To correlate SEI properties with interfacial resistance.

Main Methods:

  • X-ray photoemission spectroscopy (XPS) was used to analyze SEI composition during in-situ lithium plating.
  • Electron beam was utilized for lithium plating on Li6PS5Cl pellets.
  • Electrochemical impedance spectroscopy (EIS) validated XPS findings in full cells.

Main Results:

  • XPS analysis revealed that lithium plating current density dictates SEI evolution.
  • Optimized current density promotes a uniform and Li3P-rich SEI.
  • The Li3P-rich SEI effectively decreases the electrode-solid electrolyte interfacial resistance.

Conclusions:

  • Lithium plating current density is a critical parameter for controlling SEI properties.
  • A uniform, ionically conductive SEI is achievable, leading to reduced interfacial resistance.
  • These findings are vital for advancing the performance of solid-state lithium batteries.