Core-shell positive electrode materials with a core:shell mass ratio of 2:1 and 4:1 were synthesized in a two-step reaction. Powder X-ray diffraction, SEM and spatial EDS measurements were used to characterize the core and shell phases in the precursors and lithiated products. It was determined using EDS that the precursor and lithiated products are both core-shell and the two phases can be easily resolved with laboratory grade XRD equipment. Two phase Rietveld refinement was completed on the core-shell lithiated products. The results of these refinements in conjunction with contour plots of the lattice parameters within the Li-Ni-Mn oxide layered single phase region were used to position the core and shell of each sample on the Li-Ni-Mn-O phase diagram as a function of the amount of Li 2 CO 3 used in synthesis. The shell phase retained an approximately fixed amount of Li while the Li content of the core phase increased as the overall Li content of the core-shell sample increased. Both the core and shell were electrochemically active. A specific capacity of 220 mAh/g was achieved in a core shell material between 2.5-4.6 V vs. Li/Li + . © The Author ( There has been an extraordinary effort to synthesize and characterize different materials for the positive electrode of lithium-ion batteries.1,2 A primary motivation of this research is to improve the performance of lithium-ion cells to meet requirements for electric vehicle (EVs) and grid storage applications. As the choices of positive electrode materials move away from current commercial staples such as LiFePO 4 5 the cell must be charged to higher potentials, sometimes as high as 4.8 V vs. Li/Li + , to access the additional reversible capacity. At higher potentials, degradation of the electrolyte through oxidation on the positive electrode may vastly reduce the lifetime of the cell. For the high energy density of new materials to be fully utilized, oxidation of the electrolyte must be minimized. Otherwise, these materials are of little commercial interest for EVs and grid storage where lifetime requirements of decades of useful service would be difficult to achieve.The rate of parasitic reactions that degrade the electrolyte at the positive electrode's surface are affected by the composition of the electrolyte, the potential of the positive electrode, the composition of the positive electrode and many other parameters in the construction and operation of the cell. Commonly, researchers are addressing this by improving electrolyte formulations via additives and solvent blends.6,7 A complementary approach is examining the positive electrode surface composition and its effect on the degradation of the electrolyte. [8][9][10][11][12] Rowe et al. 13 showed via high precision charger measurements that the columbic efficiency and charge end point capacity slippage were dependent on the composition of the positive electrode of various LiNi-Mn layered oxides. Samples in that study were cycled up to 4.6 V vs. Li/Li + with the same additive-free electrolyte formulation. ...