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Uniform pore structure enables negligible degradation in undoped and uncoated Ni-rich cathodes

Nature Energy (2026)Cite this article

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Abstract

Ni-rich layered oxide cathodes for lithium-ion batteries exhibit chemomechanical failures, with the consensus attributing this to high-voltage phase transitions. Existing mitigation strategies rely on compositional modifications (for example, doping), nanostructuring (for example, coatings and primary-particle engineering) and microstructure modifications, but these approaches increase synthesis complexity. Here, we demonstrate a simple synthesis strategy that enables exceptionally stable Ni-rich cathodes without doping, coating or concentration gradients. We show that chemomechanical failure is closely linked to microstructural non-uniformity (specifically, nanoscale pores), stemming from limited contact between solid-state reactants during calcination. By increasing the LiOH melting rate, we enhance liquid–solid interfacial contact between precursors, resulting in uniformly evolved microstructures. This uniformity leads to excellent cycle life by dissipating strain energy and mitigating chemomechanical failure even in the presence of high-voltage phase transition. Our findings challenge the prevailing belief that suppressing this phase transition and hierarchal material design are necessary for stable Ni-rich cathodes.

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Fig. 1: Synthesis pathway of Ni-rich layered oxides.
Fig. 2: Liquid-mediated reaction via increased heating rate.
Fig. 3: Increasing heating rate increases the fraction of molten LiOH during synthesis.
Fig. 4: Heating rate homogenizes microstructure.
Fig. 5: Mitigating chemomechanical degradation through homogeneous microstructure.

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Data availability

All data are available in the main text or the Supplementary Information. Additional data in this paper are available via Dryad at https://doi.org/10.5061/dryad.mpg4f4rf3 (ref. 47).

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Acknowledgements

The battery aspect of this work was supported by the Assistant Secretary for Critical Minerals & Energy Innovation, Transportation Technologies Office, Battery Materials Research Program, US Department of Energy (DOE). The synthesis aspect of this work was supported by BASF Corporation through the California Research Alliance. X-ray imaging work was supported by the US Air Force Office Multidisciplinary University Research Initiative (MURI) programme under grant no. FA9550-23-1-0281. TGA-MS work was supported by the Regional Innovation System & Education (RISE) programme funded by the Ministry of Education (MOE) and the Jeollanamdo, Republic of Korea (grant no. 2025-RISE-14-003).

This research used resources of the National Synchrotron Light Source II, which is a DOE Office of Science User Facility under contract no. DE-SC0012704. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. This research also used resources of the Pohang Light Source II at the Pohang Accelerator Laboratory, Republic of Korea. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under grant no. ECCS-2026822. We thank P. Wallace for assistance with the Helios Hydra PFIB-SEM and S. Yoo for assistance with TXM/XNI image processing.

Author information

Author notes

  1. These authors contributed equally: Donggun Eum, Hari Ramachandran, Tianxiao Sun.

Authors and Affiliations

  1. Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA

    Donggun Eum, Hari Ramachandran, Zhelong Jiang, Nicolas B. Liang, Joon-Hyung Lee & William C. Chueh

  2. SLAC-Stanford Battery Research Center, Applied Energy Division, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Donggun Eum, Zhelong Jiang, Emma P. K. L. Choy, Yan-Kai Tzeng & William C. Chueh

  3. Walker Department of Mechanical Engineering, The University of Texas Austin, Austin, TX, USA

    Tianxiao Sun & Yijin Liu

  4. Department of Mechanical Engineering, Stanford University, Stanford, CA, USA

    Samuel S. Lee

  5. Department of Materials Science and Engineering, Korea University, Seoul, Republic of Korea

    Hyeokjun Park

  6. Department of Energy Science and Engineering, Sunchon National University, Suncheon, Republic of Korea

    Keeyoung Jung

  7. Institute for Battery Research (IBR), Sunchon National University, Suncheon, Republic of Korea

    Keeyoung Jung

  8. Department of Chemical and Biomolecular Engineering, University of California Berkeley, Berkeley, CA, USA

    Jaeheon Lee & Bryan D. McCloskey

  9. Pohang Accelerator Laboratory, Pohang University of Science and Technology, Pohang, Republic of Korea

    Sugeun Jo

  10. Department of Chemistry, Stanford University, Stanford, CA, USA

    Emma P. K. L. Choy

  11. Department of Advanced Materials Science and Engineering, Kyungpook National University, Daegu, Republic of Korea

    Joon-Hyung Lee

  12. Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    William C. Chueh

  13. Department of Energy Science and Engineering, Stanford University, Stanford, CA, USA

    William C. Chueh

Authors
  1. Donggun Eum
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  2. Hari Ramachandran
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Contributions

D.E. and H.R. conceived the original idea, and D.E., H.R., T.S., Y.L. and W.C.C. designed the research. D.E. performed electrochemical tests and characterizations, such as OM, TXM, XNI and XRD. H.R. synthesized the materials and collected SEM, XANES and XRD data. T.S. analysed and processed the datasets of OM, TXM and XNI. S.S.L. conducted PFIM-SEM and interpreted the mechanical properties of the materials. Z.J. and Y.-K.T. contributed to XRD and OM experiments, respectively. H.P. provided constructive advice for experimental design. J.L. and B.D.M. conducted DEMS experiments. K.J. and S.J. carried out TGA-MS analysis and PXM measurements, respectively. E.P.K.L.C performed EIS measurements and fitting. N.B.L. and J.-H.L. offered valuable feedback throughout the project. D.E., H.R., T.S., Y.L. and W.C.C. wrote the manuscript, and D.E., Y.L. and W.C.C. supervised all aspects of the research.

Corresponding authors

Correspondence to Donggun Eum, Yijin Liu or William C. Chueh.

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Nature Energy thanks Lianzhou Wang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Reaction heterogeneity across multiple particles at 440 °.

a,b, PXM images showing spatial distribution of the Ni white-line energy across multiple particles quenched at 440 °C under heating rates of (a) 2 °C/min and (b) 10 °C/min.

Extended Data Fig. 2 Reaction heterogeneity across multiple particles at 560 °C.

a,b, Additional PXM images, taken from areas complementary to those in Fig. 4c and d, showing spatial distribution of the Ni white-line energy across multiple particles quenched at 560 °C under heating rates of (a) 2 °C/min and (b) 10 °C/min.

Extended Data Fig. 3 Primary-particle morphology and size comparison in the pristine state.

a,b, Cross-sectional SEM images of the (a) 2 and (b) 10 °C/min electrodes in the pristine state, each shown as a pair of original and watershed-segmented images. c,d, Histograms of equivalent primary-particle sizes for the (c) 2 and (d) 10 °C/min samples, with mean particle sizes indicated.

Extended Data Fig. 4 Microstructural degradation across multiple particles after 100 cycles.

a,b, Cross-sectional SEM images of the (a) 2 and (b) 10 °C/min electrodes after 100 cycles. Scale bar, 10 µm.

Supplementary information

Supplementary Information (download PDF )

Supplementary Notes 1–5, Figs. 1–28, Tables 1 and 2 and References.

Supplementary Video 1 (download MP4 )

2 °C per min.

Supplementary Video 2 (download MP4 )

10 °C per min.

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Eum, D., Ramachandran, H., Sun, T. et al. Uniform pore structure enables negligible degradation in undoped and uncoated Ni-rich cathodes. Nat Energy (2026). https://doi.org/10.1038/s41560-026-01988-w

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