Promoting high-voltage stability through local lattice distortion of halide solid electrolytes.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38368426.
- Also identified by DOI 10.1038/s41467-024-45864-1 and PMC identifier 10874449.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl<sup>-</sup>, which effectively curbs kinetics of their oxidation. The confinement is realized by substituting In with multiple elements in Li<sub>3</sub>InCl<sub>6</sub> to give a high-entropy Li<sub>2.75</sub>Y<sub>0.16</sub>Er<sub>0.16</sub>Yb<sub>0.16</sub>In<sub>0.25</sub>Zr<sub>0.25</sub>Cl<sub>6</sub>. Meanwhile, the lattice distortion promotes longer Li-Cl bonds, facilitating favorable activation of Li<sup>+</sup>. Our results show that this high-entropy halide electrolyte boosts the cycle stability of all-solid-state battery by 250% improvement over 500 cycles. In particular, the cell provides a higher discharge capacity of 185 mAh g<sup>-1</sup> by increasing the charge cut-off voltage to 4.6 V at a small current rate of 0.2 C, which is more challenging to electrolytes|cathode stability. These findings deepen our understanding of high-entropy materials, advancing their use in energy-related applications.