Halide segregation to boost all-solid-state lithium-chalcogen batteries
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.
Authors
- Shiyuan Zhou (ORCID: https://orcid.org/0000-0002-9270-2573)
- Gui‐Liang Xu (ORCID: https://orcid.org/0000-0001-9969-883X)
- Jianming Bai (ORCID: https://orcid.org/0000-0002-0575-2987)
- Dilworth Y. Parkinson (ORCID: https://orcid.org/0000-0002-1817-0716)
- Dominik Wierzbicki (ORCID: https://orcid.org/0000-0003-0558-7405)
- Khalil Amine (ORCID: https://orcid.org/0000-0001-9206-3719)
- Victoria Castagna Ferrari (ORCID: https://orcid.org/0000-0002-5832-8901)
- Sarah Nicholas (ORCID: https://orcid.org/0000-0001-5639-2873)
- Yuzi Liu (ORCID: https://orcid.org/0000-0002-8733-1683)
- Wenqian Xu (ORCID: https://orcid.org/0000-0002-4815-6253)
- Yonghua Du (ORCID: https://orcid.org/0000-0003-2655-045X)
- Jieun Lee (ORCID: https://orcid.org/0000-0003-4227-4125)
- Chen Zhao (ORCID: https://orcid.org/0000-0003-1537-7671)
- Cheng‐Jun Sun (ORCID: https://orcid.org/0000-0001-9158-8337)
- Angela Sun (ORCID: https://orcid.org/0009-0006-7862-1191)
Institutions
- Argonne National Laboratory (US)
- Lawrence Berkeley National Laboratory (US)
- Brookhaven National Laboratory (US)
- University of Chicago (US)
Publication Details
- Journal
- Science
- Published
- 2025-05-15
- DOI
- https://doi.org/10.1126/science.adt1882
- Citations
- 23
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 16.80