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Reactive boride infusion stabilizes Ni-rich cathodes for lithium-ion batteries

Nature Energy volume 6, pages 362–371 (2021)Cite this article

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Abstract

Engineered polycrystalline electrodes are critical to the cycling stability and safety of lithium-ion batteries, yet it is challenging to construct high-quality coatings at both the primary- and secondary-particle levels. Here we present a room-temperature synthesis route to achieve a full surface coverage of secondary particles and facile infusion into grain boundaries, and thus offer a complete ‘coating-plus-infusion’ strategy. Cobalt boride metallic glass was successfully applied to a Ni-rich layered cathode LiNi0.8Co0.1Mn0.1O2. It dramatically improved the rate capability and cycling stability, including under high-discharge-rate and elevated-temperature conditions and in pouch full-cells. The superior performance originates from a simultaneous suppression of the microstructural degradation of the intergranular cracking and of side reactions with the electrolyte. Atomistic simulations identified the critical role of strong selective interfacial bonding, which offers not only a large chemical driving force to ensure uniform reactive wetting and facile infusion, but also lowers the surface/interface oxygen activity, which contributes to the exceptional mechanical and electrochemical stabilities of the infused electrode.

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Fig. 1: ‘Coating-plus-infusion’ microstructure for CoxB-infused NCM.
Fig. 2: Uniform amorphous CoxB infusion at the NCM surface and GBs.
Fig. 3: Superior electrochemical performance of CoxB–NCM over pristine NCM.
Fig. 4: CoxB infusion simultaneously suppresses microstructural degradation and side reactions.
Fig. 5: Morphology and chemical characteristics of cycled LMA.
Fig. 6: Strong interfacial bonding suppresses oxygen activity.

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Data generated and analysed in this study are included in the manuscript and its Supplementary Information.

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Acknowledgements

This work was supported by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) and the Ministry of Trade, Industry & Energy (MOTIE) of the Republic of Korea (no. 20172410100140). 2020 Research Funds (1.200029.1) of the Ulsan National Institute of Science and Technology (UNIST) is also acknowledged. Y.D. and J.L. acknowledge support from the Department of Energy, Basic Energy Sciences, under award no. DE-SC0002633 (Chemomechanics of Far-From-Equilibrium Interfaces).

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

Authors and Affiliations

  1. 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, Jaekyung Sung, Hyungyeon Cha, Kihong Ahn, Seok Ju Kang & Jaephil Cho

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

    Yanhao Dong & Ju Li

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

    Yimeng Huang & Ju Li

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Contributions

M.Y., Y.D., J.L. and J.C. conceived the project. M.Y. synthesized the materials and conducted the electrochemical testing. Y.D. conducted the simulations and theoretical analysis. M.Y. and J.H. conducted ex situ and in situ XRD measurements and analysis. H.C. and J.S. conducted the focused ion beam, TEM, SEM and XPS measurements. S.J.K. provided equipment for the DEMS measurements. M.Y. and K.A. assembled and tested the pouch-type full-cells. M.Y. and Y.D. analysed the data. M.Y., Y.D., J.L. and J.C. wrote the paper. All the authors discussed and contributed to the writing.

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Correspondence to Ju Li or Jaephil Cho.

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Yoon, M., Dong, Y., Hwang, J. et al. Reactive boride infusion stabilizes Ni-rich cathodes for lithium-ion batteries. Nat Energy 6, 362–371 (2021). https://doi.org/10.1038/s41560-021-00782-0

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