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We have exploited the capacity of the "(SiP(iPr)(3))Fe(I)" scaffold to accommodate additional axial ligands and characterized the mononuclear S = ½ H(2) adduct complex (SiP(iPr)(3))Fe(I)(H(2)). EPR and ENDOR data, in the context of X-ray structural results, revealed that this complex provides a highly unusual example of an open-shell metal complex that binds dihydrogen as a ligand. The H(2) ligand at 2 K dynamically reorients within the ligand-binding pocket, tunneling among the energy minima created by strong interactions with the three Fe-P bonds.

A Nonclassical Dihydrogen Adduct of S = 1/2 Fe(I)

A Nonclassical Dihydrogen Adduct of S = ¹/₂ Fe(I)