Table shows the 11 new systems performed with explorative searches according to the pair-wise minimum separations from Table . Further property calculations (e.g. band gaps, average voltages) were performed on dynamically stable structures (see Figure ) with distances to the convex hull of the Li-Ni-O phase diagram within 100 meV atom -1 (i.e. E above_hull < 100 meV atom - 1 ) from PBEsol+U calculations, as the chosen energy range generally covers that for experimental synthesizable structures. From Overall, there is a consistent energy (E above_hull ) ordering of phases predicted using the PBEsol+U and HSE06 functionals. The HSE06 functional tends to better describe the electronic structures for a wider range of materials in different chemical environments and hence their results are generally more reliable. Assuming only cationic redox during delithiation, the average voltages, theoretical capacities and theoretical energy densities for dynamically stable phases are benchmarked against experimentally known phases (Table ). The two Li 2 NiO 2 phases have the highest theoretical energy densities, suggesting that they are potentially good cathode candidates. Unfortunately, the practical performance of I-Li 2 NiO 2 is poor, as it was found to experience an irreversible structural change and a significant capacity loss during the first charge-discharge cycle. The 1T-Li 2 NiO 2 , on the other hand, was reported to be stable over 100 cycles between 1.7-4.0 V, despite the voltage hysteresis. Below half lithiation, the 1T-Li 2 NiO 2 becomes the layered LiNiO 2 , and its practical performance is limited due to the existing issues with cycling LiNiO 2 (e.g. the anisotropic lattice change and the various phase transformations during the lithium deintercalation). For layered intercalation cathode materials, volume reductions (>5%) are commonly observed when >75% of Li have been extracted from the structures. The cell volume change at different Li contents has contributions from: (1) steric factors (e.g. the number of Li that are required to sterically sustain the interlayer spacing); (2) electrostatic factors (e.g. strength of Van der Waals interactions vs other coulombic interactions). The experimental percentage volume reduction for the layered LiNiO 2 to the H3 phase (approaching a dilute limit of Li) is around 7%, which is close to the calculated result. The preference for the Ni to adopt in the square planar coordination is therefore not greatly driven by the crystal field stabilization energy (CSFE) but other (long range) electrostatic interactions between the ions. ), suggesting that the structural feature of layers of tetrahedral Li + and octahedral Ni 2+ is associated with poorer electronic conductivity.