Known for their incredible selectivity, activity, and stability under physiological conditions, enzymes set a high bar for synthetic catalysts to achieve. While synthetic small-molecule active site mimics can achieve impressive levels of catalytic activity, most fall short of their enzyme counterparts, with true enzyme-like activity proving difficult to accomplish. Research demonstrating the significance of the secondary coordination sphere suggests that by synthesizing the secondary coordination sphere interactions around a small-molecule mimic, enzyme-like catalysis can be achieved. We chose to mimic dopamine beta monooxygenase (DβM) due to its desirable selectivity and oxygen-activating reactivity. Our metallopolymer system is designed with a copper center surrounded by a larger polymer framework that models the proteinaceous microenvironment in a way that is both scalable and tunable. We have begun synthesis and benchmarking of a series of small molecule copper complexes chosen for their ease of synthesis and effectiveness in various oxidation reactions. We have also begun modification of these complexes with vinyl moieties to allow for straightforward attachment to our polymer scaffolds via thiol-ene click chemistry. Looking forward, we will study the selectivity, activity, and stability of our metallopolymer systems with a range of oxidation reactions and compare to small molecule controls.

Copper-containing metallopolymers towards enabling enzyme-like activity

ACS Spring Meeting 2021

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