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Eutectic salt-assisted planetary centrifugal deagglomeration for single-crystalline cathode synthesis

Nature Energy volume 8, pages 482–491 (2023)Cite this article

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Abstract

Single-crystalline layered cathodes are often desirable for advanced lithium-ion batteries. However, constrained by the accessible temperature range to prevent lithium evaporation, lattice defects and particle agglomerations, the production of single-crystalline cathodes with high phase purity, good electrochemical performance and scalability remains challenging. Here we invent a new mechanochemical activation process that offers a general solution to the conundrum of synthesizing coarse single-crystal cathodes with Li-/Mn-rich or Ni-rich chemistry, which differs from the equipment- and energy-intense and long-duration mechanochemical routes that are difficult to scale up. Our approach is based on interfacial reactive wetting, mediated by transient eutectic salts in situ melted by moderate mechanical agitations, to form a colloidal suspension of nanosized oxides dispersed in liquified lithium salts. It efficiently deagglomerates the polycrystalline precursors, repacks the crystals and homogenizes the lithium-salt distribution, thus enabling facile particle coarsening later into the single-crystalline morphology with improved electrochemical performance.

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Fig. 1: Planetary centrifugal deagglomeration for single-crystalline cathode synthesis.
Fig. 2: Secondary-particle deagglomeration by molten lithium salts during planetary centrifugal mixing.
Fig. 3: Mechanochemical reactive wetting at nanoscale.
Fig. 4: Structural characterizations of micro-sized single-crystalline LMR.
Fig. 5: Superior electrochemical performance of SC-LMR over PC-LMR.
Fig. 6: Demonstration of single-crystalline Ni-rich layered cathodes.

Data availability

Data generated and analysed in the present work are available in the paper and Supplementary Information. Source data are provided with this paper.

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Acknowledgements

M.Y. acknowledges support by the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2022R1A6A3A03069190). J.L. acknowledges support by Defense Advanced Research Projects Agency (DARPA) MINT programme under contract number HR001122C0097.

Author information

Author notes

  1. These authors contributed equally: Moonsu Yoon, Yanhao Dong.

Authors and Affiliations

  1. Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Moonsu Yoon, Yanhao Dong, Baoming Wang, Jin-Sung Park & Ju Li

  2. Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, Republic of Korea

    Moonsu Yoon, Jaeseong Hwang, Jaehyun Park, Seok Ju Kang & Jaephil Cho

  3. State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, China

    Yanhao Dong

  4. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Yimeng Huang, Junghwa Kim & Ju Li

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  1. Moonsu Yoon
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Contributions

M.Y., Y.D., J.C. and J.L. conceived the project. M.Y. and Y.D. designed the experiments and analysed the data. M.Y. synthesized the materials and conducted electrochemical testing. Y.H. and J.-S.P. conducted SEM and ex situ XRD measurements. B.W., J.K. and J.H. conducted focused ion beam and TEM measurements. J.P. and S.J.K. conducted in situ DEMS analysis. M.Y., Y.D., J.C. and J.L. wrote the paper. All authors discussed and contributed to the writing.

Corresponding authors

Correspondence to Jaephil Cho or Ju Li.

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Competing interests

M.Y., Y.D., J.C. and J.L declare that this work has been filed as US Provisional Patent Application (US 63/484,989). The other authors declare no competing interests.

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Nature Energy thanks Ke Du, Raffael Ruess and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Figs. 1–26, Tables 1–9, Note 1 and References.

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Source data for Fig. 5.

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Yoon, M., Dong, Y., Huang, Y. et al. Eutectic salt-assisted planetary centrifugal deagglomeration for single-crystalline cathode synthesis. Nat Energy 8, 482–491 (2023). https://doi.org/10.1038/s41560-023-01233-8

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