Abstract
Co- and Ni-free disordered rocksalt cathodes utilize oxygen redox to increase the energy density of lithium-ion batteries, but it is challenging to achieve good cycle life at high voltages >4.5 V (versus Li/Li+). Here we report a family of Li-excess Mn-rich cathodes that integrates rocksalt- and polyanion-type structures. Following design rules for cation filling and ordering, we demonstrate the bulk incorporation of polyanion groups into the rocksalt lattice. This integration bridges the two primary families of lithium-ion battery cathodes—layered/spinel and phosphate oxides—dramatically enhancing the cycling stability of disordered rocksalt cathodes with 4.8 V upper cut-off voltage. The cathode exhibits high gravimetric energy densities above 1,100 Wh kg−1 and >70% retention over 100 cycles. This study opens up a broad compositional space for developing battery cathodes using earth-abundant elements such as Mn and Fe.
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The authors declare that all data supporting the findings of this study are available within the Article and its Supplementary Information files. Source data are provided with this paper.
Change history
31 October 2025
A Correction to this paper has been published: https://doi.org/10.1038/s41560-025-01923-5
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Acknowledgements
We acknowledge funding by Honda Research Institute USA, Inc. This research used resources of 7-BM of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. The authors acknowledge support by the Molecular Foundry at Lawrence Berkeley National Laboratory (LBNL), which is supported by the US Department of Energy under contract no. DE-AC02-05-CH11231. This research used resources of the Advanced Photon Source (11-BM and 11-ID-B), a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. This research used resources of the 17B and 16U1 beamlines of Shanghai Synchrotron Radiation Facility. Y.Y., Y.S. and Y. Han thank the support from the Institutes of Energy and the Environment (IEE) Seed Grant Program at The Pennsylvania State University.
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Y. Huang, Y.D. and J. Li. conceived the project. Y. Huang synthesized the materials and conducted XRD, SEM, ICP-OES and XRF measurements. Y. Huang, M.Y., S.L., E.Y.Z., Y.L. and H.J. contributed to electrochemical testing. Y.Y., Y.S., Y. Han, J.C., C.O., C.S. and A.P. contributed to sample preparations, data collection and data processing for HAADF-STEM and EELS. T.L. contributed to high-resolution XRD and PDF measurements. W.H.K., H.C. and W.Y. contributed to neutron powder diffraction measurements. Y.P. and M.L. contributed to DEMS measurements. B.W. contributed to TEM imaging, SAED and STEM–EDS. B.W., Z.C., Y.Z. and H.J. contributed to Raman measurements. Z.C. and J.X contributed to ICP-MS measurements. L.M., X.X. and L.G. contributed to XANES measurements. W.L., R.M. and C.Y. contributed to XRD Rietveld refinement. Y. Huang and Y.D. analysed the data. Y. Huang, Y.D. and J. Li. wrote the paper. All authors discussed and contributed to the writing.
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Y. Huang, Y.D. and J. Li report a US non-provisional patent application filed by the Massachusetts Institute of Technology, patent application no. 18/790,946. The patent is related to the compositions and synthesis method reported in this Article. The other authors declare no competing interests.
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Huang, Y., Dong, Y., Yang, Y. et al. Integrated rocksalt–polyanion cathodes with excess lithium and stabilized cycling. Nat Energy 9, 1497–1505 (2024). https://doi.org/10.1038/s41560-024-01615-6
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DOI: https://doi.org/10.1038/s41560-024-01615-6
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