The purpose of our project is to synthesize multiple α –diimine ligands that have the potential to be redox active in transition metal complexes. We propose that iron complexes of these various ligands can be tuned electronically to be selective for the reduction of either protons or carbon dioxide. Specifically, complexes in which reduction occurs at the ligand will be more prone to bind carbon dioxide, whereas, complexes in which the iron center is reduced will favor reaction with protons. In order to analyze reduction potentials of the various ligands, we synthesized zinc complexes of the general formula Zn(α –diimine)Cl2 because redox activity will most likely occur at the ligand, as zinc will remain in the 2+ oxidation state. The zinc complexes were synthesized and characterized by 1H NMR spectroscopy and X-ray crystallography, and we determined the reduction potentials of the complexes using cyclic voltammetry. Based on these reduction potentials, we synthesized iron carbonyl complexes of the form Fe(α –diimine)(CO)3, in which the α –diimine ligands have a range of reduction potentials. We will present the characterization of these complexes by NMR and IR spectroscopies, as well as X-ray crystallography. Based on comparison of α –diimine bond lengths in the zinc and iron complexes, we propose that the ligand is in a reduced form. In the iron complexes, the α –diimine C-C bond is shortened and the C-N bonds lengthened compared to those in the zinc complexes. We will also present the electrochemical properties of the iron carbonyl complexes and their reactivity with small molecules.

Structural, electrochemical, and catalytic properties of zinc and iron complexes of redox active α-diimine ligands

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

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.