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.
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