%0 Journal Article %A Yanying Lu %A Tianyu Zhu %A Eric J McShane %A Bryan D McCloskey %A Guoying Chen %B Small %D 2022 %G eng %N 12 %P 2105833 %R 10.1002/smll.202105833 %T Single‐Crystal LiNixMnyCo1−x−yO2 Cathodes for Extreme Fast Charging %U https://onlinelibrary.wiley.com/toc/16136829/18/12 %V 18 %8 03/2022 %! Small %X
Ni-rich layered LiNixMnyCo1−x−yO2 (NMCs, x ≥ 0.8) are poised to be the dominating cathode materials for lithium-ion batteries for the foreseeable future. Conventional polycrystalline NMCs, however, suffer from severe cracking along the grain boundaries of primary particles and capacity loss under high charge and/or discharge rates, hindering their implementation in fast-charging electric vehicular (EV) batteries. Single-crystal (SC) NMCs are attractive alternatives as they eliminate intergranular cracking and allow for grain-level surface optimization for fast Li transport. In the present study, the authors report synthetic approaches to produce SC LiNi0.8Co0.1Mn0.1O2 (NMC811) samples with different morphologies: Oct-SC811 with predominating (012)-family surface and Poly-SC811 with predominating (104)-family surface. Poly-SC811, representing the first experimentally synthesized NMC811 single crystals with (104) surface, delivers superior performance even at the ultra-high rate of 6 C. Through detailed X-ray analysis and electron microscopy characterization, it is shown that the enhanced performance originates from better chemical and structural stabilities, faster Li+ diffusion kinetics, suppressed side reactions with electrolyte, and excellent cracking resistance. These insights provide important design guidelines in the future development of fast-charging NMC-type cathode materials.