Abstract
All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability1,2,3. Integrated all-in-one cathodes, which eliminate inactive conductive additives and heterogeneous interfaces, hold promise for substantial energy and stability gains but are hindered by materials lacking sufficient Li+/e− conductivity, mechanical robustness and structural stability4,5,6,7,8,9,10,11,12,13,14. Here we present Li1.3Fe1.2Cl4, a cost-effective halide material that overcomes these challenges. Leveraging reversible Fe2+/Fe3+ redox and rapid Li+/e− transport within its framework, Li1.3Fe1.2Cl4 achieves an electrode energy density of 529.3 Wh kg−1 versus Li+/Li. Critically, Li1.3Fe1.2Cl4 shows unique dynamic properties during cycling, including reversible local Fe migration and a brittle-to-ductile transition that confers self-healing behaviour. This enables exceptional cycling stability, maintaining 90% capacity retention for 3,000 cycles at a rate of 5 C. Integration of Li1.3Fe1.2Cl4 with a nickel-rich layered oxide further increases the energy density to 725.6 Wh kg−1. By harnessing the advantageous dynamic mechanical and diffusion properties of all-in-one halides, this work establishes all-in-one halides as an avenue for energy-dense, durable cathodes in next-generation all-solid-state batteries.
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Acknowledgements
We thank the support from the Natural Sciences and Engineering Research Council of Canada (NSERC), the Canada Research Chair Program (CRC), the Canada Foundation for Innovation (CFI), and Western University. The synchrotron-related characterizations were completed at the HXMA, SXRMB, BXDS and SGM beamline at the Canadian Light Source (CLS), which is supported by the Canadian Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan, as well as the BL02B02 (31124.02.SSRF.BL02B02) beamline of the Shanghai Synchrotron Radiation Facility (SSRF), which is supported by the ME2 project under contract from National Natural Science Foundation of China (11227902). We thank S. Xia and the In-Situ Center for Physical Sciences of Shanghai Jiao Tong University for the assistance with the SEM measurements. J.F. acknowledges the support from the programme of the China Scholarships Council. C.W. acknowledges the Banting Postdoctoral Fellowship (BPF-180162). X.S. and C.W. appreciate the funding support from the National Natural Science Foundation of China (grant nos. W2441017, 22409103), the “Innovation Yongjiang 2035” Key R&D Program (grant nos. 2024Z040, 2025Z063). Part of this work was conducted at the NOMAD beamlines at ORNL’s Spallation Neutron Source, which was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, US Department of Energy. Y.M. acknowledges the support from the National Science Foundation Award 2004837 and the computational facilities from the University of Maryland supercomputing resources.
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J.F. designed the experiments and carried out the sample synthesis and most of the characterizations. S.W. performed the computational simulations (under the supervision of Y.M.). C.W. guided the writing of the paper, the fabrication of pouch cells and the design of schematic figures. J.W.R. helped with all structural analyses of diffraction experiments. Y.Z. and X.L. helped with electron microscope-related experiments. W.L., J.T.K., Y.H., X.H. and Y.G. carried out the synchrotron-related measurements. J. Liu performed neutron data collection and analyses. B.F. and H.A. helped with nanoindentation tests. H.S., J. Liang, X.Y. and F.Z. helped with interpreting and organizing the data. Z.W. and S.Z. helped with the battery and DMA testing. J.F. and J. Luo discussed and wrote the paper. T.-K.S., Y.M. and X.S. supervised the project. All the authors helped to revise the final paper.
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Fu, J., Wang, C., Wang, S. et al. A cost-effective all-in-one halide material for all-solid-state batteries. Nature 643, 111–118 (2025). https://doi.org/10.1038/s41586-025-09153-1
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DOI: https://doi.org/10.1038/s41586-025-09153-1
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