Ni-Rich Li[Ni_<i>x</i>Mn_<i>y</i>Co_{1–<i>x</i>–<i>y</i>}]O₂ Single Crystals as Superior Fast Charge Cathodes for Lithium-Ion Batteries

The utilization of single-crystal (SC) Li[Ni _<i>x</i> Mn _<i>y</i> Co_{1-<i>x</i>-<i>y</i>} ]O₂ (NMC) cathodes has facilitated unparalleled performance in commercial high-energy lithium-ion batteries (LIBs). In the current study, we evaluate the application of SC cathodes in fast charge (FC)-LIBs where particle cracking is a predominant failure mechanism. Ni-rich SC-NMC samples with various compositions, sizes, and shapes are synthesized and investigated for their influence on FC performance. We reveal the necessity of utilizing smaller SCs (<1 μm) as larger sizes (>2 μm) experience significant particle-level lithium concentration gradients under FC conditions. To improve lithium transport and minimize side reactivities, we strategically expose the (104) crystal facets on the surface. Exceptional performance was observed on an optimized SC-LiNi_0.80Mn_0.05Co_0.15O₂, delivering a discharge capacity of 165 mAh/g even after 150 cycles at 6C charge. Our study not only demonstrates the promise of SC-NMC but also provides the key insights for the design and optimization of advanced cathodes for FC-LIBs.