Biological systems capable of performing oxidative cleavage of C-H bonds have generated much interest for the insight they provide into the design of inexpensive, environmentally friendly catalytic materials. Mixed nitrogen-donor ligands such as bispicen derivatives (N2/Py2) may serve as a suitable model for the histidine-rich coordination environment of the copper active sites of lytic polysaccharide monooxygenase and particulate methane monooxygenase. The synthesis, characterization, and reactivity of mononuclear copper(II) complexes supported by a series of bispicen ligand derivatives are reported. The formation of copper-oxygen intermediate species using H2O2 as the oxidant is explored and their reactivity toward external hydrocarbon substrates is investigated through a variety of spectroscopic and chromatographic techniques. The impact of introducing different substitutions onto the ligand framework on the electronic structure of the complex was evaluated through a combined spectroscopic and theoretical approach. This talk will focus on our current understanding of the reactivity of these mononuclear complexes toward external substrates.

Modeling copper active sites in biology: Synthesis and reactivity of bioinspired mononuclear copper(II) complexes

2019 Fall National Meeting

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