Lattice energy minimizations and molecular dynamics calculations for a selected series of metal complexes with similar metal centers and ligand geometry were performed and were compared to experimental measurements of shifts in redox potentials observed when the complexes are intercalated into negatively charged Wyoming montmorillonite. An excellent correlation between computational trends and experimental trends was observed for nonequilibrium measurements. The results are not dependent on the size of the metal complex or the absolute magnitude of the interaction with the clay surface, but are related to the relative electrostatic energies of the reduced and oxidized complexes. The results are strongly influenced by the distribution of charge within the complex.