New hybrid bis (phosphine)(pyrazole) borate tripodal ligands ([PhBP t Bu2 (pz')]-) are reported that support pseudotetrahedral iron in the oxidation states+ 1,+ 2,+ 3, and+ 4. The higher oxidation states are stabilized by a terminal Fe⋮ NR linkage. Of particular interest is the generation and thorough characterization of an S= 1 FeIV⋮ NR+ imide cation using this new ligand system. The latter species can be observed electrochemically and ...