Abstract
Solid-state batteries are attractive energy storage systems as a result of their inherent safety, but their development hinges on advanced solid-state electrolytes (SSEs). Most SSEs remain largely confined to single-anion systems (e.g., sulfides, oxides, halides, and polymers). Through mixed-anion design strategy, we develop crystalline Li3Ta3O4Cl10 (LTOC) and its derivatives with excellent ionic conductivities (up to 13.7 millisiemens per centimeter at 25°C) and electrochemical stability. The LTOC structure features mixed-anion spiral chains, consisting of corner-shared oxygen and terminal chlorine atoms, which induces continuous “tetrahedron-tetrahedron” Li-ion migration pathways with low energy barriers. Additionally, LTOC demonstrates holistic cathode compatibility, enabling solid-state batteries operation at 4.9 volts versus Li/Li+ and low temperature, down to −50°C. These findings describe a promising class of superionic conductors for high-performance solid-state batteries.
| Original language | English |
|---|---|
| Pages (from-to) | 199-204 |
| Number of pages | 6 |
| Journal | Science |
| Volume | 390 |
| Issue number | 6769 |
| DOIs | |
| State | Published - Oct 9 2025 |
Funding
The authors thank L.-Y. Chang for collecting the XAS data of Ta L-edge at Taiwan Photon Source and M. Shakouri for collecting XAS data of Cl K-edge at the Canadian Light Source (CLS). Authors acknowledge support from Western University. The synchrotron PXRD was completed at the CLS, which is supported by the Canada Foundation for Innovation, the National Research Council, the Canadian Institutes of Health Research, the Government of Saskatchewan, and the University of Saskatchewan. X.S. acknowledges support from the Natural Sciences and Engineering Research Council of Canada, the Canada Research Chair Program, the Canada Foundation for Innovation, and funding support from the National Natural Science Foundation of China (grant W2441017). Y.M. acknowledges funding support from National Science Foundation under awards 1940166 and 2118838, the computational facilities from the University of Maryland supercomputing resources, and the Maryland Advanced Research Computing Center. This research was conducted at the NOMAD beamlines (Spallation Neutron Source of Oak Ridge National Laboratory) and was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, US Department of Energy (DOE). J.L. was partially supported by ORNL-LDRD 10761. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract DE-AC02-05CH11231. The authors thank L.-Y. Chang for collecting the XAS data of Ta L-edge at Taiwan Photon Source and M. Shakouri for collecting XAS data of Cl K-edge at the Canadian Light Source (CLS).Authors acknowledge support from Western University.The synchrotron PXRD was completed at the CLS, which is supported by the Canada Foundation for Innovation, the National Research Council, the Canadian Institutes of Health Research, the Government of Saskatchewan, and the University of Saskatchewan. Funding: X.S. acknowledges support from the Natural Sciences and Engineering Research Council of Canada, the Canada Research Chair Program, the Canada Foundation for Innovation, and funding support from the National Natural Science Foundation of China (grant W2441017).Y.M. acknowledges funding support from National Science Foundation under awards 1940166 and 2118838, the computational facilities from the University of Maryland supercomputing resources, and the Maryland Advanced Research Computing Center.This research was conducted at the NOMAD beamlines (Spallation Neutron Source of Oak Ridge National Laboratory) and was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, US Department of Energy (DOE).J.L. was partially supported by ORNL-LDRD 10761.This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract DE-AC02-05CH11231. Author contributions: X.S. and F.Z. conceived the project. F.Z. and S.Z. performed the electrolyte synthesis and electrochemical performance characterizations. S.W. performed computational simulations (under the supervision of Y.M.) J.R. performed the synchrotron PXRD data collection and structural analysis. Jue L. performed neutron data collection and analysis.W.X., G.K., and J.K. helped to solve the crystal structure.Jianwen L., Jing L.,Y.G.,Y.Z., S.A., and Y.H. helped with physical characterizations and analyses. S.Z., F.Y.,W.L.,J.G., and T.S. helped with the synchrotron XAS data analysis. F.Z. and S.Z. interpreted the data and wrote the manuscript.X.S. supervised the project.All the authors commented on the final manuscript. Competing interests: The authors declare that they have no competing interests. Data and materials availability: All data are available in the manuscript or the supplementary materials. License information: Copyright © 2025 the authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original US government works. https://www.science.org/content/page/science-licenses-journal-article-reuse
Fingerprint
Dive into the research topics of 'Anion sublattice design enables superionic conductivity in crystalline oxyhalides'. Together they form a unique fingerprint.Cite this
- APA
- Author
- BIBTEX
- Harvard
- Standard
- RIS
- Vancouver