Synthesis and reactivity of silyl iron hydride via Si H bond activation

The preligand pyridine-2-amino(methyl)-dimethylsilane (1) was used to synthesize silyl iron hydride. Iron(II) hydride FeH(N(κN-C5H4N)Me(SiMe2))(PMe3)3 (2) was obtained through the reaction of 1 and Fe(PMe3)4 via the activation of one Si H bond and the coordination of nitrogen atom of pyridine. The substitution reaction of complex 2 with haloalkane (CH3I and EtBr) delivered complexes FeX(N(κN-C5H4 N)Me(SiMe2))(PMe3)3 (X = I (3); Br (4)). Complex 2 reacting with acetylacetone resulted in the formation of Fe(acac)(N(κN-C5H4N)Me(SiMe2))(PMe3)3 (5). However, the insertion products Fe(η3-OCOH)(N(κN-C5H4N)Me(SiMe2))(PMe3)3 (6) and Fe(η3-Ph-NCOH)(N(κN-C5H4N)Me(SiMe2))(PMe3)3 (7) were formed through the insertion of the unsaturated bonds into Fe H bond. Complex 6 could also be synthesized through the substitution reaction of 2 with HCOOH. The molecular structures of complexes 2 and 4–7 were determined by single crystal X-ray diffraction.