Engineering Papers⌕ Search
Home/Archive/DOE OSTI

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)
View original source ↗Read source document ↗Export metadata ↓

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.

Explore related subjects

36 MATERIALS SCIENCE

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

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

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related reports

DOE OSTI2026

Cyclic moisture reactivation of calcium sorbents for long duration thermochemical energy storage

The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

36 MATERIALS SCIENCE↗