Dinitrogen Coordination to a High-Spin Diiron(I/II) Species
Résumé
Dinitrogen coordination to iron centers underpins industrial and biological fixation in the Haber-Bosch process and by the FeM cofactors in the nitrogenase enzymes. The latter employ local high-spin metal centers; however, iron-dinitrogen coordination chemistry remains dominated by low-valent states, contrasting the enzyme systems. Here, we report a high-spin mixed-valent cis-(mu-1,2-dinitrogen)diiron(I/II) complex [(FeBr)(2)(mu-N-2)L-bis](-) (2), where [L-bis](-) is a bis(beta-diketiminate) cyclophane. Field-applied Mossbauer spectra, dc and ac magnetic susceptibility measurements, and computational methods support a delocalized S=(7)/(2) Fe2N2 unit with D=-5.23 cm(-1) and consequent slow magnetic relaxation.
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