Halide segregation to boost all-solid-state lithium-chalcogen batteries

• 成果类型: Article
• 署名作者: Lee, Jieun; Zhou, Shiyuan; Ferrari, Victoria C.; Zhao, Chen; Sun, Angela; Nicholas, Sarah; Liu, Yuzi; Sun, Chengjun; Wierzbicki, Dominik; Parkinson, Dilworth Y.; Bai, Jianming; Xu, Wenqian; Du, Yonghua; Amine, Khalil; Xu, Gui-Liang
• 署名单位: United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Brookhaven National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Argonne National Laboratory; United States Department of Energy (DOE); Lawrence Berkeley National Laboratory; University of Chicago; Korea Institute of Science & Technology (KIST)
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11136
• DOI: 10.1126/science.adt1882
• 发表日期: 2025-05-15
• 页码: 724-729
• 关键词: sulfur battery; electrolyte; mechanism; redox

摘要

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.