Wei-Hsiang ChenYu-Ting WengYu-Cheng LuHsi ChenPo-Ya ChangHwo-Shuenn SheuSenthil-Kumar ParthasarathiNAE-LIH WU2024-10-012024-10-012024-12-1503787753https://www.scopus.com/record/display.uri?eid=2-s2.0-85203627494&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/721697Herein, we demonstrate a novel and feasible strategy to stabilize the LiNi0.83Co0.12Mn0.05O2 (NCM) structure via the in-situ formation of a superficial spinel layer with potassium (K) doping. While K+ doped NCM is not new, the formation of the protective spinel layer gives surprising results with even a trace amount of doping, which is unique and novel, and nowhere reported. The structural transformation from layered to spinel on the surface region of NCM is achieved with a K-doping level of 0.05 mol% (NCM-0.05K) and the formed spinel layer acted as a protective pillar for stabilizing the host structure, leading to substantially improved electrochemical performance. The X-ray photoelectron spectra demonstrate a large increase in nickel (Ni2+) distribution after cycling for pristine but almost no change for the NCM-0.05K, suggesting a stable preformed spinel layer. The above results reveal that the K+ doping can strongly reduce the Ni4+ to stable Ni2+ under the spinel phase formation and improves cell performances in terms of specific capacity, capacity retention, rate capability, and Li+ diffusivity. The internal micro-cracking of host NCM is also effectively suppressed by the low amount of K doping. Excessive K-doping, in contrast, leads to a reduction in (de)lithiation rate and greater polarization.falseCycling stabilityK-dopingLithium-ion transportNi-rich cathoderate performanceSurface stabilization[SDGs]SDG7[SDGs]SDG11In-situ formation of spinel protective layer through extremely low K-doping for enhanced performance of Ni-rich layered cathodesjournal article10.1016/j.jpowsour.2024.2354462-s2.0-85203627494