Extended metal atom chain complexes (EMAC) that contain metal to metal bonds have utility as the smallest models of molecular wires. One current challenge is there is a limit to the diversity of M-M bonded, trimetallic EMAC and this is especially true for iron. Known trimetallic EMAC of this type are primarily supported by one ligand, dipyridylamine. We are working to expand this area of research using 2,6-bis(trimethylsilylamino)pyridine (H2L) to support clusters of 1st-row transition metals. This ligand is highly modular and is strongly donating due to its dianionic charge. Using this ligand we have synthesized the first linear (179°) triiron(II) complex that contains short Fe-Fe contacts. We have investigated this complex by X-ray diffraction, 1H NMR including Evan’s method, and cyclic voltammetry. The triferrous core is supported by three deprotonated ligands which surround the Fe chain in a trigonal coordination environment and the Fe-Fe distance (2.437 Å) suggests a significant bonding interaction. Preliminary magnetic measurements indicate an S = 6 ground state, likely arising from ferromagnetic coupling. This ligand also supports a tricobalt congener that is linear with trigonal coordination about each metal. This complex is unique amongst tricobalt EMAC in that it is the first with the Co(II) in a trigonal coordination environment, a so called lantern complex. As expected, the Co-Co bonds are shorter ( Å) but this complex has an intermediate spin that suggests more complicated magnetic behavior. Another unique feature of these complexes is the crystallographic symmetry along the M-M-M core as well as the absence of ligands binding axially on the terminal metal ions. These complexes represent an opportunity to investigate the properties of linearly combined metal-metal bonds without the complication of axially coordinated ligands and are an important addition to the field of extended metal atom chain compounds.

Novel linear, trimetallic lantern complexes of Fe(II) and Co(II) supported by 2,6-bis(trimethylsilylamino)pyridine: Structural, magnetic, and electrochemical properties

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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