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Dissecting the Solid Polymer Electrolyte-Electrode Interface in the Vicinity of Electrochemical Stability Limits.

Christofer Sångeland1, Guiomar Hernández1, Daniel Brandell1

  • 1Department of Chemistry─Ångström Laboratory, Uppsala University, Box 538, SE-751 21 Uppsala, Sweden.

ACS Applied Materials & Interfaces
|June 16, 2022
PubMed
Summary

Understanding solid polymer electrolyte-electrode interfaces is key for solid-state lithium-ion batteries. This study reveals how interfacial layers form and impact performance, using combined electrochemical and spectroscopic methods.

Keywords:
X-ray photoelectron spectroscopycathode electrolyte interphaseelectrochemical impedance spectroscopyelectrochemical stability windowlithium-ion batteriessolid electrolyte interphasesolid polymer electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Solid-state lithium-ion batteries require understanding solid polymer electrolyte-electrode interfaces.
  • Probing buried solid-solid interfaces is challenging for surface-sensitive techniques.

Purpose of the Study:

  • Evaluate the electrochemical stability window of poly(ε-caprolactone):lithium bis(trifluoromethanesulfonyl)imide (PCL:LiTFSI).
  • Investigate interfacial layer formation and its impact on cell performance.
  • Combine electrochemistry and spectroscopy for accurate interface analysis.

Main Methods:

  • Staircase voltammetry to determine electrochemical stability window.
  • Postmortem spectroscopic analysis (e.g., photoelectron spectroscopy) to identify interfacial species.
  • Electrochemical impedance spectroscopy to estimate resistance and thickness of interphase layers.

Main Results:

  • The electrochemical stability window for PCL:LiTFSI was determined to be 1.5 to 4 V vs Li+/Li.
  • Decomposition outside the stability window resulted in carbonaceous, lithium oxide, and salt-derived species.
  • Highly resistive interphase layers formed, hindering solid polymer electrolyte (SPE) system performance.

Conclusions:

  • Combined electrochemical and spectroscopic methods are crucial for accurately assessing performance at electrochemical stability limits.
  • Interfacial layer formation significantly impacts solid-state battery performance.
  • Understanding these interfaces is vital for developing practical solid-state lithium-ion batteries.