We use the DFT + solvent ion model as a screening mechanism to better couple atomistic information about oxidation and spin states to an understanding of the effects of compositional tuning on the thermodynamics of metal release from the (001) surface. We report on the bulk and surface structures, including the effects of de-lithiation and surface metal release to gauge the series of redox events that may take place while under standard operating conditions or exposed to aqueous environments. We create equistoichiometric compositions of general chemical formula Li( There has been a large effort to replace the toxic and flammable organic electrolytes in LIB to those that are aqueous since 1994. LIBs with aqueous electrolytes, aqueous lithium-ion batteries (ALIBs), have the potential to be safer with cheaper production costs, and up to two orders of magnitude higher ionic conductivity than their non-aqueous counterparts. Unfortunately, many of these initial batteries have low cyclability due to instability of the compounds used for the electrodes. More specifically, when lithium intercalation compounds such as LiMn 2 O 4 , LCO, and NMC, were used as the cathode, it was found that the pH of the electrolyte was important for the stability of the cathode. Therefore, the stability of these materials in aqueous environments, i.e. solubility 28 must be considered for use in the new frontier of high energy storage. Here we suggest cathode materials that have limited solubility depending on the pH range.