Pseudo-ternary LiBH4-LiCl-P2S5 system as structurally disordered bulk electrolyte for all-solid-state lithium batteries

TL;DR

This study introduces a pseudo-ternary LiBH4-LiCl-P2S5 electrolyte that becomes amorphous upon heating, exhibits high ionic conductivity, and demonstrates promising stability and performance in all-solid-state lithium batteries.

Contribution

It presents a novel amorphous electrolyte with high conductivity and stability, and provides detailed structural and electrochemical characterization for solid-state battery applications.

Findings

Ionic conductivity of 10^-3 S/cm at room temperature after amorphization.

Electrochemical stability up to 5 V vs. Li+/Li.

Achieved 93% capacity retention over 10 cycles in battery tests.

Abstract

The properties of the mixed system LiBH4 LiCl P2S5 are studied with respect to all-solid-state batteries. The studied material undergoes an amorphization upon heating above 601C, accompanied with increased Li+ conductivity beneficial for battery electrolyte applications. The measured ionic conductivity is 10-3 Scm-1 at room temperature with an activation energy of 0.40(2) eV after amorphization. Structural analysis and characterization of the material suggest that BH4 groups and PS4 may belong to the same molecular structure, where Cl ions interplay to accommodate the structural unit. Thanks to its conductivity, ductility and electrochemical stability (up to 5 V, Au vs. Li+/Li), this new electrolyte is successfully tested in battery cells operated with a cathode material (layered TiS2, theo. capacity 239 mAh g-1) and Li anode resulting in 93% capacity retention (10 cycles) and notable cycling stability under the current density 12 mA g-1 (0.05C-rate) at 501C. Further advanced characterisation by means of operando synchrotron X-ray diffraction in transmission mode contributes explicitly to a better understanding of the (de)lithiation processes of solid-state battery electrodes operated at moderate temperatures.