For Fe(bpac)Ni(CN)4 a stronger binding is expected in HS because of the d 8 electron count and the distorted octahedral ligand field (the d z 2 is singly occupied in HS and doubly occupied in LS). In HS, N2 and CO bind in a top on apical configuration, while H2 adopts a side on Kubas configuration. The CO2 molecules are located horizontally on top of the metal and parallel to the phenyl rings with the O(CO2)-Ni-C(CN) bond angle of 74.5 • . In LS, the bond distances increase for all molecules. N2 and CO2 maintain their orientation. H2 adopts a tilted configuration as in the IS case of Mn and Fe, and CO also adopts a tilted configuration.