The lattice structural dynamics of active materials within Li-ion batteries, contingent upon their state of charge (SoC), introduce challenges associated with volume expansion or contraction in a both particle and electrode levels1-2. This phenomenon induces mechanical fractures and alters electrode thickness, particularly problematic for high-Ni cathodes characterized by pronounced c-lattice changes during cycling, leading to substantial mechanochemical degradation and hindrance to long-term cycle retention3-4. This study proposes a resilient framework employing multi-wall carbon nanotubes to decorate the surface of active particles, imparting recoverable characteristics to high-Ni cathode materials. This surface framework, endowed with the capacity to absorb mechanical energy, effectively preserves the original secondary particle shape throughout multiple charge cycles, mitigating the serve propagation of cracking. Additionally, the control of particle shape alterations results in a noteworthy reduction of over 50% in electrode thickness changes. The consequential impact of this elastic framework particle engineering is exemplified by outstanding performance, even in a carbon-additive-free electrode with a density of 20 mg/cm². The battery exhibits superior cycle life, retaining 85% of its initial capacity after 500 cycles in a pouch cell. This advancement establishes a universal paradigm for the systematic design of Li-ion batteries with markedly extended cycle life, presenting a transformative prospect for robust and enduring energy storage W. Li, E. M. Erickson, A. Manthiram, Nat. Energy 5 , 26-34 (2020). J. Langdon, A. Manthiram, Energy Stor. Mater. 37 , 143-160 (2021). W. Li, H. Y. Asl, Q. Xie, A. Manthiram, J. Am. Chem. Soc. 141 , 5097-5101 (2019). X.-H. Meng, T. Lin, H. Mao, J.-L. Shi, H. Sheng, Y.-G. Zou, M. Fan, K. Jiang, R.-J. Xiao, D. Xiao, J. Am. Chem. Soc. 144 , 11338-11347 (2022).
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