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DOE OSTI · 2571072

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

Lee, Jieun [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000342274125)·Zhou, Shiyuan [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000292702573)·Ferrari, Victoria C. [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000258328901)·Zhao, Chen [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000315377671)·Sun, Angela [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0009000678621191)·Nicholas, Sarah [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000156392873)·Liu, Yuzi [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000287331683)·Sun, Chengjun [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000191588337)·Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405)·Parkinson, Dilworth Y. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000218170716)·Bai, Jianming [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000205752987)·Xu, Wenqian [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000248156253)·Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X)·Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000192063719)·Xu, Gui-Liang [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:000000019969883X)
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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. Here, 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.

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36 MATERIALS SCIENCE

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Lee, Jieun [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000342274125), Zhou, Shiyuan [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000292702573), Ferrari, Victoria C. [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000258328901), Zhao, Chen [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000315377671), Sun, Angela [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0009000678621191), Nicholas, Sarah [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000156392873), Liu, Yuzi [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000287331683), Sun, Chengjun [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000191588337), Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405), Parkinson, Dilworth Y. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000218170716), Bai, Jianming [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000205752987), Xu, Wenqian [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000248156253), Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X), Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:0000000192063719), Xu, Gui-Liang [Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)] (ORCID:000000019969883X). 2025-05-15. Halide segregation to boost all-solid-state lithium-chalcogen batteries. https://doi.org/10.1126/science.adt1882

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