Abstract:
Conventional aluminum complexes are incapable of one- and two-electron
redox chemistry. As a result, despite being the most abundant metal on Earth,
aluminum is seldom used in redox catalysis—one of chemistry’s most impactful
fields. We are motivated to break this barrier to provide a green alternative to the
countless redox catalysts built around the toxic, mining-intensive platinum-group
metals. To create aluminum complexes that do desirable redox chemistry, we
coordinate redox-active α-diimine ligands to the metal center. These ligands are
stable across multiple oxidation states, allowing for multi-electron redox chemistry
for their aluminum complexes.
This thesis will report the synthesis of several α-diimine complexes of
aluminum, across various ligand substitution patterns and oxidation states. These
complexes have been characterized by combinations of X-ray diffraction,
multinuclear NMR spectroscopy, cyclic voltammetry, electron paramagnetic
resonance spectroscopy, and density functional theory. For our neutral-ligand
compounds, we will report their catalytic activity for the epoxidation of cyclohexene
by peracetic acid.