spectacularly. In particular, we found that the Qeq scheme can return inappropriately highand in some instances unphysical -charges. Such is the case for the MOFs populating the cluster of blue points (cluster II) below the parity line in Figure (h). The spurious charges assigned in these materials arise for different reasons. For example, in EBOTOF (Figure , lower panel on the right), Al metals are coordinated to highly electronegative atoms such as F, which represents a particular bonding environment for which Qeq fails. Similarly, abnormal Qeq charges are assigned in MOFs where Na, Ga, or In metals are present, such as in AYUWUM (Figure , lower left panel). Ongari et al. noticed similar abnormalities in their study. As to why Qeq fails in this regard, and EQeq does not, stems from the fact that Qeq uses a neutral charge-centre to express the Taylor series expansion in electric energy, while EQeq considers the Taylor series expansion around charge-positive metal cations. The neutral charge-centring is not able to accurately reproduce DDEC charges in alkali metals such as Na, but more generally it appears to fail for MOFs containing metals with a single electron in their outer orbital, At this point, it is clear that the choice of the FF has a very strong impact on the adsorption behaviour, often leading to profound differences in the isotherms for the same material, depending on the parameters used in molecular simulations. Our results further emphasise that using simplified charge equilibration schemes in application to a heterogeneous database of materials is likely to result in unreliable predictions, which can further lead to significant scattering in the results and a lack of confidence in the rankings.