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Introducing high-valence elements into cobalt-free layered cathodes for practical lithium-ion batteries

Abstract

The elimination of Co from Ni-rich layered cathodes is considered a priority to reduce their material cost and for sustainable development of Li-ion batteries (LIBs) as Co is becoming increasingly scarce. The introduction of 1 mol% Mo into Li(Ni0.9Mn0.1)O2 delivers 234 mAh g−1 at 4.4 V. The cycling stability of a full cell featuring the Li(Ni0.89Mn0.1Mo0.01)O2 (Mo–NM90) cathode is enhanced with a modified electrolyte; retaining 86% of its initial capacity after 1,000 cycles while providing 880 Wh kgcathode−1. The grain size refinement achieved by Mo doping dissipates the deleterious strain from abrupt lattice contraction through fracture toughening and the removal of local compositional inhomogeneities. Enhanced cation ordering induced by the presence of Mo6+ also stabilizes the delithiated structure through a pillar effect. The Mo–NM90 cathode is able to deliver a high capacity with cycling stability suitable for the long service life for electric vehicles at a reduced material cost, furthering the realization of a commercially viable Co-free cathode for LIBs.

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Fig. 1: Electrochemical performances of half cells featuring undoped and doped NM90 cathodes.
Fig. 2: Comparison of primary particle morphologies of undoped and doped NM90 cathodes.
Fig. 3: Structural instability of a NM90 cathode.
Fig. 4: Structural stability of a Co-free Mo–NM90 cathode.
Fig. 5: Comparison of the long-term cycling performances of full cells featuring undoped and doped Co-free NM90 cathodes and a series of post-mortem analyses.

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All the relevant data are included in the paper and its Supplementary Information.

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Acknowledgements

This work was mainly supported by the Human Resources Development Program (number 20214000000320) of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant, funded by the Ministry of Trade, Industry and Energy of the Korean government. This work was also supported by National Research Foundation of Korea (NRF) grant funded by the Korea government Ministry of Education and Science Technology (MEST) (NRF-2018R1A2B3008794).

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G.-T.P., C.S.Y. and Y.-K.S. conceived and designed the research. G.-T.P., B.N. and S.-B.K. performed the experiments and characterization of materials. G.-T.P., C.S.Y. and Y.-K.S. analysed the data. G.-T.P., J.L., C.S.Y. and Y.-K.S. contributed to the discussion of the results. C.S.Y. and Y.-K.S. wrote the manuscript. All the authors commented on and revised the manuscript.

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Correspondence to Chong S. Yoon or Yang-Kook Sun.

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Supplementary References 1–13, Figs. 1–30 and Tables 1–5.

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Park, GT., Namkoong, B., Kim, SB. et al. Introducing high-valence elements into cobalt-free layered cathodes for practical lithium-ion batteries. Nat Energy 7, 946–954 (2022). https://doi.org/10.1038/s41560-022-01106-6

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