Aluminum-Stabilized Low-Spin Iron(II) Hydrido Complexes of 1,4,7-Trimethyl-1,4,7-triazacyclononane
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We investigated herein the reactions of (Me3tacn)FeCln (1a: n = 3, 1b: n = 2) with common aluminum hydride reagents and a bulky dihydridoaluminate {Li(ether)2}{Al(OC6H3-2,6-tBu2)}(μ-H)2, which yielded the diamagnetic hydrido complexes 2–4 containing Fe(II) and Al(III). In particular, the use of divalent 1b afforded excellent isolated yields. The structures of 2–4 were determined using spectroscopic and crystallographic analyses. The crystal structures showed distorted octahedral Fe centers and fairly short Fe–Al distances [2.19–2.24 Å]. The structures of cation moiety 2 and neutral complex 4 were further probed using DFT calculations, which indicated a stable low-spin Fe(II) state and strongly electron-donating nature of the (Me3tacn)FeH3 fragment toward the Al(III) center.
