Analyzing the structural characteristics of the aluminium pairs reveals that the changes in chemical shifts do not follow a consistent pattern based on the position or distance of the additional aluminium atom. The effect of adding an Al atom is significant across both next-nearest-neighbour (NNN) and next-next-nearest-neighbour (NNNN) aluminium pairs. Also, there is no clear correlation between the interatomic distance separating aluminium atoms and the effect on the chemical shift. The lack of clear-cut distance dependency, in this distance range, may be due to the inherent complexity of the MFI structure, however, a similarly large effect of the rather distant NNNN pairs have been also reported recently for a simpler framework (CHA). These rtmesults indicate that the magnitude of the Al chemical shift is very sensitive even to a rather minor perturbation, due to introduction of additional aluminium as far as 8 Å away, reflecting the nuanced interactions within the zeolite framework over rather large distances.