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Related Experiment Video

Updated: May 23, 2025

Characterization of Electrode Materials for Lithium Ion and Sodium Ion Batteries Using Synchrotron Radiation Techniques

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Published on: November 11, 2013

Deciphering Interfacial Stability of Sulfide and Halide-Based Electrolytes via Operando X-ray Photoelectron

Zhicong Liu^1,2, Jianming Tao^1,2, Han Jiang¹

¹College of Physics and Energy, Fujian Normal University, Fuzhou 350117, China.

|March 10, 2025

Summary

Composite solid electrolytes in all-solid-state Li-ion batteries (ASSLBs) face interface challenges. Li₆PS₅Cl and Li₃InCl₆ composites fail due to Li⁺ migration inhibition, unlike stable Li_1.75ZrO_0.5Cl_4.75 composites.

Keywords:

Halide electrolytes Interface stability Solid-state batteries Sulfide electrolytes

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Area of Science:

Materials Science
Electrochemistry
Battery Technology

Background:

All-solid-state Li-ion batteries (ASSLBs) utilize composite solid electrolytes to enhance cathode-anode compatibility.
Interface stability and ion transport mechanisms in mixed solid electrolyte systems remain poorly understood, hindering ASSLB development.

Purpose of the Study:

To investigate the interfacial behavior and ion transport mechanisms in composite solid electrolytes comprising Li₆PS₅Cl (LPSC), Li₃InCl₆ (LIC), and Li_1.75ZrO_0.5Cl_4.75 (LZOC).
To elucidate the role of electrolyte compatibility in the failure pathways of ASSLBs.

Main Methods:

Electrochemical analysis was employed to assess battery performance.
Operando X-ray photoelectron spectroscopy (XPS) was utilized to study interfacial reactions in situ.

Main Results:

The LPSC-LIC interface exhibits an electrostatic potential difference that impedes Li⁺ migration, leading to LIC decomposition and battery failure.
The LZOC-LCO interface forms a stable, oxygen-rich interphase, promoting Li⁺ diffusion and preventing severe degradation.
The LCO-LZOC composite cathode demonstrates superior electrochemical performance compared to the LCO-LIC composite.

Conclusions:

Electrolyte compatibility is critical for ASSLB performance and longevity.
Understanding interfacial reactions and ion diffusion in sulfide-halide electrolytes is key to designing stable and efficient ASSLBs.
LZOC-based composite electrolytes offer a promising alternative for stable ASSLB interfaces.