Crack-Free Nickel-Rich Single-Crystal LiNi0.8Co0.1Mn0.1O2 Thick Dry Electrode Fabrication for Application in High-Performance Lithium-Ion Batteries

Abstract The development of high-energy-density lithium-ion batteries (LIBs) is crucial to meet the increasing demands of electric vehicles (EVs), hybrid electric vehicles (HEVs), portable electronics, and large-scale energy storage systems. In this context, dry electrode fabrication has emerged as a sustainable and cost-effective alternative to conventional slurry-based processing, particularly for high-loading thick electrodes. However, intensive calendaring required in dry thick electrode processing induces significant mechanical stress, often leading to particle cracking in nickel-rich layered oxide cathodes and consequent electrochemical degradation. Herein, we systematically investigated the mechanical robustness and electrochemical performance of single-crystal S-LiNi0.8Co0.1Mn0.1O2 (S-NCM811) cathodes fabricated via a dry electrode route. The single-crystal S-NCM811 demonstrates superior structural integrity with significantly reduced particle cracking after calendaring, as confirmed by SEM analysis. Electrochemical evaluations reveal enhanced lithium-ion transport kinetics, lower charge-transfer resistance, and improved porosity in S-NCM811 compared to its polycrystalline counterpart. As a result, the S-NCM811 dry thick electrode achieves a high-capacity retention of 91.5% at 0.5 C after 50 cycles at a high mass loading of ∼35 mg cm–2, as compared to P-NCM811, which retained only 63.4% of its initial capacity after subsequent cycles. This work highlights the critical role of crystal morphology in mitigating mechanical degradation during dry processing and provides valuable insights into the design of robust nickel-rich cathodes for next-generation high-energy-density LIBs.