Thermodynamically Stable Dual-Modified LiF&FeF layer Empowering Ni-Rich Cathodes with Superior Cyclabilities.

Pushing the limit of cutoff potentials allows nickel-rich layered oxides to provide greater energy density and specific capacity whereas reducing thermodynamic and kinetic stability. Herein, a one-step dual-modified method is proposed for in situ synthesizing thermodynamically stable LiF&FeF coating on LiNi Co Mn O surfaces by capturing lithium impurity on the surface to overcome the challenges suffered. The thermodynamically stabilized LiF&FeF coating can effectively suppress the nanoscale structural degradation and the intergranular cracks. Meanwhile, the LiF&FeF coating alleviates the outward migration of O (α<2), increases oxygen vacancy formation energies, and accelerates interfacial Li diffusion. Benefited from these, the electrochemical performance of LiF&FeF modified materials is improved (83.1% capacity retention after 1000 cycles at 1C), even under exertive operational conditions of elevated temperature (91.3% capacity retention after 150 cycles at 1C). This work demonstrates that the dual-modified strategy can simultaneously address the problems of interfacial instability and bulk structural degradation and represents significant progress in developing high-performance lithium-ion batteries (LIBs).