The structure determination program was first validated using a smaller system, in the cost of DFT geometry optimization when compared to MgCl2/TiCl4 binary systems. The addition of donor molecules significantly increased the total electron count and slowed down the convergence of geometry optimization due to their softness. With this distinction in mind, hereafter, "most stable structure" must be understood as the lowest energy structures discovered during our explorations, which may not necessarily represent the global minima in the parameter space. Nevertheless, two out of the three GA runs resulted in the same most stable structures for both DEP and DE. More importantly, stable structures consistently exhibited similar structural characteristics, leading us to believe that the conclusions drawn from the limited datasets are at least qualitatively accurate. Visual analysis of the four most stable structures of each system (Figure ) shows significant differences among compositions. As stated in our previous studies, The frequency and nature of edges is an important aspect of the morphology of nanoplates due to their strong impact on the adsorption capabilities. They can occur between same or different surface types and at various angles (Figure ), which dictate the coordination of the Mg 2+ cations placed at the edges. Particularly, right and acute edges are composed of a Mg 2+ cation coordinating to three or fewer Cl -anions from the bulk, which is very difficult to be stabilized without cooperative adsorption including chelation. Among many different patterns, a prominent one in ID-containing systems was a small {110} terrace followed by a {100}