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Site-Selective Modification of Lanthanum Oxychloride to Modulate Halide-Ion Conduction
Jingxiang Cheng1,2, Victor Alexander Gomez3,4, Alice R Giem1,2
1Department of Chemistry, Texas A&M University, College Station, Texas 77843-3012, United States.
ACS Applied Energy Materials
|May 1, 2026
Summary
This study enhances chloride-ion conductivity in LaOCl solid electrolytes by introducing aliovalent cations like Ca2+, creating vacancies and softening the lattice. This offers a new strategy for designing efficient solid-state halide-ion conductors for energy storage.
Area of Science:
- Solid-state chemistry and materials science
- Energy storage materials
- Electrochemical technologies
Background:
- Design principles for solid-state halide-ion conduction are poorly understood.
- Halide ions are crucial charge carriers in energy storage and electrochemical computing.
- LaOCl is a promising material for halide-ion conduction.
Purpose of the Study:
- To establish design principles for solid-state halide-ion conduction.
- To enhance chloride-ion conductivity in LaOCl via site-selective aliovalent alloying.
- To investigate the effects of aliovalent substitution on lattice dynamics and conductivity.
Main Methods:
- Site-selective aliovalent substitution of La3+ with Mg2+, Ca2+, and Sr2+ in LaOCl.
- X-ray excited optical luminescence measurements using Dy3+ as a reporter.
- Temperature-dependent Raman spectroscopy and powder X-ray diffraction with Rietveld refinement.
Main Results:
- Aliovalent substitution generates charge-compensating chloride vacancies, preserving the matlockite structure.
- Ca alloying (8-10 at.%) increases chloride-ion conductivity by 3-4 orders of magnitude.
- Ca and Sr alloying soften the La-Cl sublattice, creating a more compliant lattice for ion migration.
- Local distortions and modified lattice dynamics enhance chloride-ion mobility.
Conclusions:
- Site-selective aliovalent alloying of LaOCl is an effective strategy for developing halide-ion solid electrolytes.
- Vacancy formation and lattice softening are key design principles for facile anion transport.
- This approach provides generalizable principles for designing advanced solid electrolytes.
