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Exploring Tetra-/Penta-/Hexavalent Ion Substitution in Yttrium-Based Halide Solid-State Electrolytes.

Chao Li¹, Zhichao Zeng¹, Wenshuo Zhang¹

¹Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, P.R. China.

|January 22, 2025

Summary

Exploring aliovalent ion doping in halide electrolytes, this study reveals Zr⁴⁺ substitution enhances ionic conductivity by optimizing crystal structure. This leads to improved battery performance, offering a new avenue for solid-state electrolytes.

Keywords:

Aliovalent ion doping All-solid-state lithium batteries Fast ionic conductor Halide solid-state electrolytes Rare earth

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Area of Science:

Materials Science
Solid-State Chemistry
Electrochemistry

Background:

Aliovalent ion substitution is key to improving ionic conductivity in halide electrolytes.
Current research often limits doping ions to tetravalent types, with limited understanding of doping mechanisms.

Purpose of the Study:

Investigate the impact of Zr⁴⁺, Ta⁵⁺, and W⁶⁺ doping on yttrium-based rare-earth halide crystal structure and ionic conductivity.
Elucidate the intrinsic mechanisms behind aliovalent ion doping effects on ion diffusion.

Main Methods:

Synthesis and characterization of yttrium-based rare-earth halides doped with Zr⁴⁺, Ta⁵⁺, and W⁶⁺.
Analysis of crystal structure modifications, including octahedral volume and interstitial space.
Measurement of ionic conductivity and evaluation of electrochemical performance in full batteries.

Main Results:

Zr⁴⁺ doping promotes fast ion diffusion across (001) and (002) planes by altering lattice parameters.
Ta⁵⁺ and W⁶⁺ exhibit anisotropic effects on ion diffusion, enhancing it in one plane while suppressing it in another.
Optimal ionic conductivity of 0.437 mS cm^-1 achieved with Zr⁴⁺ substitution, coupled with excellent battery capacity and cycling stability.

Conclusions:

Zr⁴⁺ is a highly effective dopant for enhancing ionic conductivity in halide electrolytes.
Understanding the anisotropic effects of different aliovalent ions is crucial for designing advanced solid-state electrolytes.
The optimized halide electrolyte demonstrates significant potential for high-performance batteries.