Abstract
All-solid-state batteries using sulfur-based positive electrodes (cathodes) offer a cost-effective route to achieve high specific energy. However, low active material utilization and cycle life hinder performance. Here, we demonstrate a positive electrode design that employs sulfide solid-state electrolytes, where a high energy synthesis approach forms a metastable and ionically conductive interphase on the active material surface. This interphase facilitates high active material utilization and contributes capacity with cycling. We also show that tailoring active material particle sizes to the micron-scale improves rate performance and cycling stability. Structural analysis reveals that the substantial volume change of sulfur-based positive electrodes during operation can partially offset that of the negative electrodes, thereby mitigating internal mechanical stress. The combined design principles enable sulfur areal capacities up to 11 mAh cm-2 while maintaining stable cycling at 25 °C. We further demonstrate several specific-energy-focused cell architectures, particularly a Li2S anode-free pouch cell that operates under “low stack pressure” of 10 MPa. This work outlines practical design strategies for constructing high-specific-energy all-solid-state batteries for a broad range of emerging applications.
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Acknowledgements
This work was supported by the LG Energy Solution – U.C. San Diego Frontier Research Laboratory (FRL) Program (A.C., S.-Y.H., C.H., H.Y., M.V., C.L., D.L., M.-S.S., J.J., J.B.L., and Y.S.M.). A.C. acknowledges the National Science Foundation for having supported their Ph.D. research through the NSF Graduate Research Fellowship Program. The authors (A.C., B.S., and P.R.) would like to acknowledge the UCSD Crystallography Facility. This work was also performed in part at the San Diego Nanotechnology Infrastructure (SDNI) of UCSD, a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (Grant ECCS−1542148, A.C., S.-Y.H., S.B., D.C., G.D., and M.V.), along with the use of facilities and instrumentation supported by NSF through the UC San Diego Materials Research Science and Engineering Center (UCSD MRSEC) (Grant DMR-201192). The authors (A.C., C.H., Y.S.M.) would like to acknowledge Prof. Bing Joe Hwang and Ms. Chia-Yu Chang for their help on XAS measurements at the Taiwan Light Source (TLS) beamline 16A1 of the National Synchrotron Radiation Research Center (NSRRC) in Hsinchu, Taiwan. The authors (A.C. and Y.S.M.) thank Dr. Jinkwan Jung for his assistance in sample preparation and cell fabrication.
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A.C. and Y.S.M. conceived the ideas for the study. A.C., J.B.L., and X.W. designed the experiments. B.S. and P.R. collected XRD measurements. S.B. contributed cryo-TEM characterization and investigation. C.H. performed XAS and analysis. A.C., M.V., and D.C. performed SEM-FIB. M.C. performed the electrode modeling and FEM simulations. C.L. and D.L. fabricated and evaluated the pouch cells. J.A.S.O., G.D., S.-Y.H., H.Y., M.V., J.J., M.-S.S., J.B.L., and Y.S.M. participated in the scientific discussion and data analysis. A.C. wrote the manuscript. Y.S.M. supervised the project. All authors discussed the results and commented on the manuscript.
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Y.S.M., A.C., J.B.L., and M.-S.S. declare that two patents were filed for this work through UC San Diego’s Office of Innovation and Commercialization and LG Energy Solution, Ltd. The remaining authors declare no competing interests.
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Cronk, A., Wang, X., Oh, J.A.S. et al. A highly utilized and practical lithium-sulfur positive electrode enabled in all-solid-state batteries. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69750-0
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DOI: https://doi.org/10.1038/s41467-026-69750-0
