The chemical oxidation and subsequent group transfer activity of the unusual diiron imido complexes Fe((i)PrNPPh2)3Fe≡NR (R = tert-butyl ((t)Bu), 1; adamantyl, 2) was examined. Bulk chemical oxidation of 1 and 2 with Fc[PF6] (Fc = ferrocene) is accompanied by fluoride ion abstraction from PF6(-) by the iron center trans to the Fe≡NR functionality, forming F-Fe((i)PrNPPh2)3Fe≡NR ((i)Pr = isopropyl) (R = (t)Bu, 3; adamantyl, 4). Axial halide ligation in 3 and 4 significantly disrupts the Fe-Fe interaction in these complexes, as is evident by the >0.3 Å increase in the intermetallic distance in 3 and 4 compared to 1 and 2. Mössbauer spectroscopy suggests that each of the two pseudotetrahedral iron centers in 3 and 4 is best described as Fe(III) and that one-electron oxidation has occurred at the tris(amido)-ligated iron center. The absence of electron delocalization across the Fe-Fe≡NR chain in 3 and 4 allows these complexes to readily react with CO and (t)BuNC to generate the Fe(III)Fe(I) complexes F-Fe((i)PrNPPh2)3Fe(CO)2 (5) and F-Fe((i)PrNPPh2)3Fe((t)BuNC)2 (6), respectively. Computational methods are utilized to better understand the electronic structure and reactivity of oxidized complexes 3 and 4.
This research output has an Altmetric Attention Score of 3. This is our high-level measure of the quality and quantity of online attention that it has received. This Attention Score, as well as the ranking and number of research outputs shown below, was calculated when the research output was last mentioned on 31 May 2014.
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