Ab Initio Calculation of Surface Orientation Effect on Slab Stability and Morphology of Spinel LiNi0.5Mn1.5O4 Embedded in a Thermodynamic Framework

Herein, we perform ab initio computations to assess the influence of surface orientation on the stability and morphology of spinel LiNi0.5Mn1.5O4 within a thermodynamic framework. The validity of our computations is confirmed through a comparison with the experimental results. We examine the behavior of LiNi0.5Mn1.5O4 crystals in response to differing reaction conditions, thereby presenting novel insights to advance the development of more stable LiNi0.5Mn1.5O4 cathodes. Despite the limited number of surfaces analyzed, our findings contribute significant evidence to the ongoing debate concerning the most stable plane. This encourages a shift in focus from merely identifying the most stable plane to understanding the conditions that lead to its stability.