Chemical-Mechanical Effects in Ni-Rich Cathode Materials

The implementation of Ni-rich cathodes with high energy density has been critically restrained by stress corrosion. Herein, crack-free LiNbO₃-coated LiNi_0.88Co_0.10Mn_0.02O₂, as theoretically predicted, demonstrates highly reversible lithiation/delithiation. Mechanically, the phase transition (H1 → H2 → H3) is significantly alleviated by the excogitation of the interfacial force invoked by the LiNbO₃ coating layer, as verified by X-ray absorption spectroscopy and extended X-ray absorption near-edge structure spectroscopy. Meanwhile, the stabilities of the crystal structure are remarkably strengthened by the strong Nb–O bond activated by Nb⁵⁺ doping that is confirmed by Rietveld refinement of X-ray diffraction and differential capacitance curves. Chemically, the interface shielding effect is conducive to protecting the electrode against electrolyte corrosion along with subsequent transition-metal dissolution, ultimately rendering a faster/highly convertible lithium-ion diffusion. Greatly, the excellent electrochemical properties (74% capacity retention after 300 cycles at 2 C within 2.5–4.3 V) and structural stability (the morphology remains intact after 500 cycles at 5 C within 2.5–4.3 V) are successfully achieved. Given this, this elaborate work might inaugurate a potential avenue for rationally tuning the structure/interface evolution toward Ni-rich materials.