Self-assembly of an Organometallic Fe9O6 Cluster from Aerobic Oxidation of (tmeda)Fe(CH2tBu)2

Substoichiometric aerobic oxidation of the high-spin organometallic compound (tmeda)Fe(CH2tBu)2 (tmeda = N,N,N’,N’- tetramethylethylenediamine) in toluene or THF solution leads to the self-assembly of a magic-sized all-ferrous oxide cluster containing the Fe9O6 subunit and bearing organometallic and diamine ligands. Mossbauer studies of the cluster and the reference complex (tmeda)Fe(OCPh3)2 are consistent with the all-ferrous assignment, and magnetometry reveal considerable antiferromagnetic coupling between Fe atoms in the cluster and frustrated antiferromagnetic interactions between clusters in the solid state.