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Low-Coordinate Iron Hydride Chemistry at an N,N,C-Heteroscorpionate Platform. | LitMetric
Locally high-spin iron hydrides are proposed to play a critical role as intermediates in iron-molybdenum cofactor (FeMoco)-catalyzed N fixation. Inspired by these biological systems, we report herein our initial investigations into low-coordinate iron hydride chemistry supported by our N,N,C-heteroscorpionate ligands. Those ligands with smaller steric profiles are unable to completely suppress the formation of a binuclear [Fe(μ-H)] complex; however, the incorporation of more substantial steric bulk allows for the isolation of a rare example of a terminal, high-spin ( = 2) Fe hydride. Fourier transform infrared spectroscopy suggests an unusually weak Fe-H bond in the latter molecule. Mössbauer spectroscopies, coupled with density functional theory calculations, highlights the substantial influence of the terminal hydride ligand on Fe isomer shift.
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