Understanding the Surface Structure of LiNi0.45Mn1.55O4 Spinel Cathodes with Aberration-Corrected HAADF STEM

In order for Li-ion batteries to mature to a level useful for integration into the current or future energy infrastructure, basic problems such as cyclability, cost and rate capability must be overcome. LiNi0.5Mn1.5O4 (LNM), a spinel cathode material, has the advantage of being both cost-effective and a high-rate capable material, but it is plagued with cyclability problems. In the LNM system the main contributor to cycling degradation is the high operating voltage which leads to solid-electrolyte interphase (SEI) formation. We find that excess-Mn doping of this material (LiNi0.5-XMn1.5+XO4 where x=0.05) leads to increased cyclability through natural passivation [1]. To understand the exact role that excess Mn plays in the passivation of this cathode material, it is crucial to determine the surface’s atomic structure. This is because the surface structure determines how reactive the cathode will be with the electrolyte during oxidation and reduction cycles.