The MFI structure was obtained from the IZA database. To determine the optimal unit cell dimensions for the models with aluminium, one aluminium atom was substituted at the T12 site (Si/Al = 95). To generalize the model for both low and high water loadings, 7 water molecules were introduced into the structure. The unit cell dimensions obtained from the IZA database were uniformly scaled by factors ranging from 0.96 to 1.06, and molecular dynamics (MD) simulations were performed at a temperature of 350 K (see Section 2.2). A cubic fit of the unit cell volume versus average energy revealed the lowest energy configuration, corresponding to a unit cell volume of 5301 Å 3 . The optimized lattice parameters were determined to be a = 20.20 Å, b = 19.85 Å, and c = 13.22 Å, and these parameters were used for all orthorhombic MFI unit cells in this study. Further details can be found in Section S1 in ESI †.