2026-04-16 アルゴンヌ国立研究所（ANL）
A solid-state electrolyte sample before (top row) and after (bottom row) high-speed mixing. The electrolyte materials remain intact after mixing (first column). High-speed mixing causes halide segregation, illustrated in the second column by the migration of chlorine (blue) to the interface of the electrolyte, improving its performance. The distribution of phosphorus (green) and sulfur (yellow) is shown for comparative purposes. All images were taken by a technique called high-angle annular dark-field scanning transmission electron microscopy. (Image by Argonne National Laboratory.)
＜関連情報＞
- https://www.anl.gov/article/argonne-scientists-discover-how-to-boost-solidstate-battery-energy-density-and-longevity
- https://www.science.org/doi/10.1126/science.adt1882
ハロゲン化物分離による全固体リチウムカルコゲン電池の性能向上 Halide segregation to boost all-solid-state lithium-chalcogen batteries
Jieun Lee, Shiyuan Zhou, Victoria C. Ferrari, Chen Zhao, […] , and Gui-Liang Xu
Science Published:15 May 2025
DOI:https://doi.org/10.1126/science.adt1882
Editor’s summary
All-solid-state lithium-sulfur batteries offer significantly increased energy density, safety, and cost-effectiveness compared with existing lithium-ion batteries. However, optimizing the solid-solid interface remains a grand challenge to achieve high sulfur utilization and long cycle life. Lee et al. used ultra-high-speed mixing of a sulfur cathode with a halide-based solid electrolyte to fabricate composite electrodes. This process leads to interfacial segregation and formation of a lithium chloride–rich shell on the surface of the particles. This structure enhances charge transport kinetics, boosts interfacial stability, and mitigates mechanical failure in solid-state batteries. The formation and efficacy of the halide segregation was confirmed using cryogenic transmission electron microscopy and synchrotron x-ray diffraction and spectroscopy techniques. —Marc S. Lavine
Abstract
Mixing electroactive materials, solid-state electrolytes, and conductive carbon to fabricate composite electrodes is the most practiced but least understood process in all-solid-state batteries, which strongly dictates interfacial stability and charge transport. We report on universal halide segregation at interfaces across various halogen-containing solid-state electrolytes and a family of high-energy chalcogen cathodes enabled by mechanochemical reaction during ultrahigh-speed mixing. Bulk and interface characterizations by multimodal synchrotron x-ray probes and cryo–transmission electron microscopy show that the in situ segregated lithium halide interfacial layers substantially boost effective ion transport and suppress the volume change of bulk chalcogen cathodes. Various all-solid-state lithium-chalcogen cells demonstrate utilization close to 100% and extraordinary cycling stability at commercial-level areal capacities.
