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One-step calcination synthesis of interface-coherent crystallized and surface-passivated LiNi0.5Mn1.5O4 for high-voltage lithium-ion battery

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Abstract

LiNi0.5Mn1.5O4 (LNMO) with a spinel crystal structure presents a compelling avenue towards the development of economic cobalt-free and high voltage (∼ 5 V) lithium-ion batteries. Nevertheless, the elevated operational voltage of LNMO gives rise to pronounced interfacial interactions between the distorted surface lattices characterized by Jahn–Teller (J–T) distortions and the electrolyte constituents. Herein, a localized crystallized coherent LaNiO3 and surface passivated Li3PO4 layer is deposited on LNMO via a one-step calcination process. As evidenced by transmission electron microscopy (TEM), time-of-flight secondary ion mass spectrometry (ToF-SIMS) and density functional theory (DFT) calculation, the epitaxial growth of LaNiO3 along the LNMO lattice can effectively stabilize the structure and inhibit irreversible phase transitions, and the Li3PO4 surface coating can prevent the chemical reaction between HF and transition metals without sacrificing the electrochemical activity. In addition, the ionic conductive Li3PO4 and atomic wetting inter-layer enables fast charge transfer transport property. Consequently, the LNMO material enabled by the lattice bonding and surface passivating features, demonstrates high performance at high current densities and good capacity retention during long-term test. The rational design of interface coherent engineering and surface coating layers of the LNMO cathode material offers a new perspective for the practical application of high-voltage lithium-ion batteries.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22209075 and 12004145), the Key Science and Technology Plan Project of Ji’an City (No. 20211-015311), and the Natural Science Foundation of Jiangsu Province (No. BK20200800). All the computations were performed on the high-performance computing platform of Jinggangshan University and Shanghai University.

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Authors and Affiliations

  1. College of Materials Science and Engineering, Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Nanjing Forestry University, Nanjing, 210037, China

    Min Xu, Bifu Sheng, Junjie Lu, Minfeng Chen, Jizhang Chen & Xiang Han

  2. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Materials, Xiamen University, Xiamen, 361005, China

    Yong Cheng & Ming-Sheng Wang

  3. College of Mathematics and Physics, Jinggangshan University, Ji’an, 343009, China

    Bo Liu

  4. School of Materials Science and Engineering, Shanghai University, Shanghai, 200444, China

    Siqi Shi

  5. Western Digital Corporation, 951 Sandisk Dr, Milpitas, CA, 95035, USA

    Peng Wang

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  1. Min Xu
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  2. Bifu Sheng
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  3. Yong Cheng
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Correspondence to Bo Liu, Jizhang Chen or Xiang Han.

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One-step calcination synthesis of interface-coherent crystallized and surface-passivated LiNi0.5Mn1.5O4 for high-voltage lithium-ion battery

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Xu, M., Sheng, B., Cheng, Y. et al. One-step calcination synthesis of interface-coherent crystallized and surface-passivated LiNi0.5Mn1.5O4 for high-voltage lithium-ion battery. Nano Res. 17, 4192–4202 (2024). https://doi.org/10.1007/s12274-023-6361-z

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