Further structural optimization and property calculations were performed with the VASP code on a selection of CASTEP optimized refined structures using the PBEsol+U (U Ni = 6 eV) with a cutoff energy of 550 eV and a k-point spacing of 0.05 2π Å -1 on gamma-centered Monkhorst-Pack grids. A maximum force tolerance of 0.01 eV Å -1 was applied during geometry optimization. The PAW pseudopotentials (version PBE 5.4) of Li_sv, Ni_pv and O were used unless otherwise stated. Lattice dynamics calculations were performed on the known phases in the Li-Ni-O phase diagrams and the lowest energy structure in each hypothetical composition with the ground magnetic ordering using the Phonopy package with the finite-displacement method at an increased cutoff energy of 800 eV and a tighter force tolerance of 0.001 eV Å -1 during geometry optimization (Table ). Non-analytical term corrections were applied on all oxides to treat the long range electrostatic interactions. The thermodynamic stability of a selection of structures were evaluated with other functionals (PBE+U 40 , LDA+U , SCAN and HSE06 ) using the VASP code and Hubbard U for Ni was kept at 6 eV. All structures were optimized in the same functional as the that for the final static calculations. The screening parameter 𝜔 = 0.207 Å -1 was consistently used for all HSE06 calculations. The energy cutoff for different functionals were specified in Table . The PAW pseudopotentials (version LDA 5.4) of Li_sv, Ni_pv and O were used for the LDA+U calculations. For the thermodynamically stable phases, the atomic chemical potentials ranges that a target phase is stable were determined using CPLAP. The average voltages and voltage profiles were calculated using the ferromagnetic (FM) ordering spin arrangements using the PBEsol+U functional, since the magnetic ordering generally gives small differences to the calculated voltages. The band gaps were obtained from the HSE06 calculations. The climbing image NEB (cNEB) method was used to study Li-ion The ase , pymatgen 50 packages were used for manipulating structures and general analysis.