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Abstract Localized atomistic disorder in halide‐based solid electrolytes (SEs) can be leveraged to boost Li+mobility. In this study, Li+transport in structurally modified Li3HoCl6, via Br−introduction and Li+deficiency, is explored. The optimized Li3‐3yHo1+yCl6‐xBrxachieves an ionic conductivity of 3.8 mS cm−1at 25 °C, the highest reported for holmium halide materials.6,7Li nuclear magnetic resonance and relaxometry investigations unveil enhanced ion dynamics with bromination, attaining a Li+motional rate neighboring 116 MHz. X‐ray diffraction analyses reveal mixed‐anion‐induced phase transitions with disproportionate octahedral expansions and distortions, creating Ho‐free planes with favorable energetics for Li+migration. Bond valence site energy analysis highlights preferred Li+transport pathways, particularly in structural planes devoid of Ho3+blocking effects. Molecular dynamics simulations corroborate enhanced Li+diffusion with Br−introduction into Li3HoCl6. Li‐Ho electrostatic repulsions in the (001) plane presumably drive Li+diffusion into the Ho‐free (002) layer, enabling rapid intraplanar Li+motion and exchange between the 2d and 4h sites. Li3‐3yHo1+yCl6‐xBrxalso demonstrates good battery cycling stability. These findings offer valuable insights into the intricate correlations between structure and ion transport and will help guide the design of high‐performance fast ion conductors for all‐solid‐state batteries.
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This content will become publicly available on April 29, 2026
Enhanced cycling performance of bilayered vanadium oxide cathode in Li-ion batteries via dual metal-ion preintercalation
The simultaneous chemical preintercalation of Li+and Mg2+ions into the interlayer region of bilayered vanadium oxide synergistically enhances its cycling performance in Li-ion cells by improving Li+diffusion and increasing structural stability.
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- Award ID(s):
- 2106445
- PAR ID:
- 10610267
- Publisher / Repository:
- Royal Society of Chemistry
- Date Published:
- Journal Name:
- Journal of Materials Chemistry A
- Volume:
- 13
- Issue:
- 17
- ISSN:
- 2050-7488
- Page Range / eLocation ID:
- 12170 to 12183
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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