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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Commercialization of all-solid-state lithium-ion batteries (ASSLIBs) is hindered by the challenge of preparing effective low-temperature solid electrolytes.
  • Existing solid electrolytes often struggle to maintain high ionic conductivity and stability at sub-ambient temperatures.

Purpose of the Study:

  • To develop a novel starch-based solid electrolyte with superior electrochemical properties for low-temperature operation.
  • To demonstrate the potential of this electrolyte in enhancing the performance and applicability of ASSLIBs.

Main Methods:

  • Synthesis of a starch-based solid electrolyte using two cross-linking reactions to create ordered lithium salt binding sites.
  • Electrochemical characterization including ionic conductivity (σ), lithium-ion transfer number (t+), and decomposition potential (dP) measurements at various temperatures.
  • Assembly and testing of ASSLIBs using LiFePO4 and LiNi0.8Co0.1Mn0.1O2 cathodes with the developed electrolyte.

Main Results:

  • The starch-based solid electrolyte achieved high ionic conductivity (3.10 × 10⁻⁴ S cm⁻¹ at 25 °C, 3.10 × 10⁻⁵ S cm⁻¹ at -20 °C).
  • Exceptional electrochemical stability was observed with a lithium-ion transfer number of 0.82 at 25 °C and 0.72 at -20 °C, and decomposition potentials of 4.91 V and 5.50 V, respectively.
  • ASSLIBs utilizing this electrolyte demonstrated good specific capacity, long cycle life below room temperature, and operational capability at 0 °C with a 4.3 V cathode.

Conclusions:

  • The developed starch-based solid electrolyte offers a viable solution for low-temperature operation of ASSLIBs.
  • This material significantly improves the electrochemical performance and widens the application scope of ASSLIBs in cold environments.
  • The synthesis strategy provides an effective method for creating ordered binding sites, crucial for high-performance solid electrolytes.