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Strain-retardant coherent perovskite phase stabilized Ni-rich cathode

Nature volume 611, pages 61–67 (2022)Cite this article

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Abstract

The use of state-of-the-art Ni-rich layered oxides (LiNixCoyMn1−x−yO2, x > 0.5) as the cathode material for lithium-ion batteries can push the energy and power density to a higher level than is currently available1,2. However, volume variation associated with anisotropic lattice strain and stress that is being developed during lithium (de)intercalation induces severe structural instability and electrochemical decay of the cathode materials, which is amplified further when the battery is operating at a high voltage (above 4.5 V), which is essential for unlocking its high energy3,4,5,6. Even after much effort by the research community, an intrinsic strain-retardant method for directly alleviating the continuous accumulation of lattice strain remains elusive. Here, by introducing a coherent perovskite phase into the layered structure functioning as a ‘rivet’, we significantly mitigate the pernicious structural evolutions by a pinning effect. The lattice strain evolution in every single cycle is markedly reduced by nearly 70% when compared with conventional materials, which significantly enhances morphological integrity leading to a notable improvement in battery cyclability. This strain-retardant approach broadens the perspective for lattice engineering to release the strain raised from lithium (de)intercalation and paves the way for the development of high-energy-density cathodes with long durability.

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Fig. 1: Strain-retardant strategy and implementation.
Fig. 2: Strain-retarding behaviour characterized by in-operando synchrotron XRD.
Fig. 3: Electrochemical performance characterized in half cells.
Fig. 4: Chemical phase distribution and 3D morphology changes.

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Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

The work at Argonne National Laboratory was supported by the US Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office. Argonne National Laboratory is operated for the US DOE Office of Science by UChicago Argonne, LLC, under contract no. DE-AC02-06CH11357. This research used the 9-BM, 11-BM, 11-ID-C and 32-ID-C beamlines at APS, a US DOE Office of Science User Facility operated for the US DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. This work was also supported by Clean Vehicles, US–China Clean Energy Research Centre (CERC-CVC2) under US DOE EERE Vehicle Technologies Office. J.L. acknowledges financial support from the start-up research funding of Zhejiang University. We also thank Y. Ren, L. Yin, V. D. Andrade and K. Shelly for their support of the synchrotron-based experiments.

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Author notes

  1. These authors contributed equally: Liguang Wang, Tongchao Liu

Authors and Affiliations

  1. College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, China

    Liguang Wang, Tianpin Wu & Jun Lu

  2. X‐ray Science Division, Argonne National Laboratory, Lemont, IL, USA

    Liguang Wang & Tianpin Wu

  3. Institute of Zhejiang University-Quzhou, Quzhou, China

    Liguang Wang

  4. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA

    Tongchao Liu & Jun Lu

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Contributions

L.W. and J.L. conceived the ideas and designed the experiments. L.W., T.L. and T.W. carried out the synchrotron-based experiments and analysed the data. L.W. and T.L. prepared the materials and conducted the electrochemical measurements. L.W., T.W. and J.L. wrote the manuscript. J.L. supervised the project.

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Correspondence to Tianpin Wu or Jun Lu.

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Wang, L., Liu, T., Wu, T. et al. Strain-retardant coherent perovskite phase stabilized Ni-rich cathode. Nature 611, 61–67 (2022). https://doi.org/10.1038/s41586-022-05238-3

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