Professor Adam Fiedler of Marquette University is supported by the Chemical Catalysis (CAT) Program in the Division of Chemistry to design and synthesize transition metal complexes that mimic the function of metalloenzymes. More specifically, the PI is mainly targeting Fe(II) complexes with polyimidazole ligands to mimic the 3His motif found in several iron oxygenases which use O2 to cleave the C-C bonds of pollutants. Complexes with a range of electronic and steric properties will be prepared using a flexible synthetic approach, and their ability to catalyze dioxygenation reactions will be explored under various conditions. An array of spectroscopic and computational tools will be used to obtain detailed geometric- and electronic-structure descriptions of the resulting complexes. In addition, the PI will employ a series of biologically-relevant ligands with non-coordinating groups capable of forming intramolecular hydrogen-bonds, thereby providing insight into second-sphere interactions that are known to be significant in enzymatic function.
Metal-containing dioxygenases are capable of incorporating oxygen atoms into hydrocarbons, thus initiating their degradation process. The proposed research will have a significant environmental remediation impact, in that it could potentially lead to complexes that are capable of facilitating the aerobic degradation of single and multi-ring hydrocarbons which are a major class of environmental pollutants. Research opportunities will be provided to students from underrepresented and low-income groups through outreach programs already administered at Marquette University, and laboratory experiments on environmental remediation and oxidation catalysis will be prepared for pre-college and undergraduate science laboratory programs.
