Abstract
Single crystallization remains a debated strategy for advancing Ni-rich cathode materials. While it mitigates particle cracking and improves tap density by eliminating particle boundaries, extended diffusion pathways introduce volumetric and lattice distortions, compromising electrochemical and structural stability. These challenges hinder the commercialization of high-Ni single-crystal cathodes, calling for a reassessment of their viability. Here we report a structural design: intralattice-bonded phase single-crystal LiNi0.92Co0.03Mn0.05O2 (IBP-SC92). This architecture maintains structural integrity while shortening diffusion pathways, resulting in almost zero electrochemical degradation during cycling. The robust structure and fast ion transport mitigate lattice strain, as confirmed by multiscale high-resolution diffraction and imaging techniques, preventing intragranular cracks and irreversible phase transitions. As a result, IBP-SC92 shows outstanding cycling stability, with nearly 100% capacity retention after 100 cycles in half cells and 94.5% retention after 1,000 cycles in full cells. This redefined single-crystal cathode represents a significant step towards the industrial adoption of high-energy-density materials.
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Acknowledgements
This work was supported by the Major Research plan of the National Natural Science Foundation of China (grant no. 92372207) and the National Key R&D Program of China (grant nos. 2022YFB4000120 and 2023YFB2405800). This work was also supported by Leading Innovative and Entrepreneurial Projects in Zhejiang Province (grant no. 2023R01007). We thank Z. Xia and Y. Wang from the State Key Laboratory of Luminescent Materials and Devices, School of Physics and Optoelectronics at South China University of Technology for their support in providing advanced temperature detection techniques. We thank L. Zeng and Q. Zhang from Southern University of Science and Technology for their assistance in acquiring atomic-resolution STEM data. We acknowledge support from the US Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. Argonne National Laboratory is operated for DOE Office of Science by UChicago Argonne, LLC, under contract number DE-AC02-06CH11357. Use of the National Synchrotron Light Source II (beamline 3-ID, 7-BM and 18-ID) is supported by the US DOE, an Office of Science user Facility operated by Brookhaven National Laboratory under contract number DE-SC0012704.
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C.Y., Q.Z., T.L., J.W. and J.L. conceived the idea and developed the theory. Q.Z. synthesized the materials and carried out electrochemical testing as well as in situ XRD, XAS and DEMS measurements. W.H., X.H., X.X., T.L., K.A. and L.M. conducted synchrotron XRD, XAS, X-ray scanning nanodiffraction and TXM measurements. Q.Z., J.W. and Y.C. analysed the data. Q.Z., C.Y., J.W. and T.L. wrote the paper. All authors discussed and contributed to the writing.
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Nature Energy thanks Jungjin Park and the other, anonymous, reviewers for their contribution to the peer review of this work.
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Supplementary Figs. 1–41, Discussion and Tables 1–5.
Supplementary Video 1
The rocking curves of SC92 at the (003) diffraction peak positions.
Supplementary Video 2
The rocking curves of IBP-SC92 at the (003) diffraction peak positions.
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Zhang, Q., Wang, J., Chu, Y. et al. Intralattice-bonded phase-engineered ultrahigh-Ni single-crystalline cathodes suppress strain evolution. Nat Energy 10, 1001–1012 (2025). https://doi.org/10.1038/s41560-025-01827-4
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DOI: https://doi.org/10.1038/s41560-025-01827-4
