Remote site deprotonation of the coordinated tripodal ligand, tris((2-benzimidazolyl)methyl)amine, was examined using electronic spectroscopy and electrochemistry techniques. The solid-state structures [CoH(3)1(tba)(NCS)](+) and [CoH(2)1(tba)(NCS)] are reported. These complexes crystallized in the triclinic space group P (1) over bar [a = 13.3043(2) Angstrom, b = 13.8019(2) Angstrom, c = 14.1322(2) Angstrom, alpha = 63.6670(10)degrees, beta = 68.0590(10)degrees, gamma = 81.8960degrees; Z= 2] and the monoclinic space group P2(1)/n [a = 15.3530(9) Angstrom, b = 11.0645(6) Angstrom, c = 19.1319(10) Angstrom, beta = 105.6750(10)degrees; Z = 4], respectively. Preliminary results suggest that selective and reversible deprotonation of coordinated benzimidazolyl ligands can tune the reduction potential of several isostructural cobalt(II) complexes.