During the addition of further electrons, Pauli repulsion gradually destabilizes the POV6 core (Table , where K is given as an example). The expansion of the electron cloud of the core even pushes the oppositely charged counterions from the core. Nevertheless, the change of V-O bond length (Fig. ) shows that for both monovalent (K as an example is given) and divalent cations the increase of the distance between the atoms in the POV6 is not significant and does not exceed 5% (for the system with K cations) and 9% (for the system with Mg cations) compared to the V-O bond length in the pristine POV6 with all vanadium atoms in the V V oxidation state. Therefore, the main difference between the various types of counterions is the number of electrons that can be taken up by V addenda atoms of the POV6 core, and thus the generated magnetic state of the overall bisligated POV6 structure.