Oxidation Catalysis with 3d Complexes Bearing Fluorinated Alkoxide Ligands

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Oxidation reactions are critically important and widespread in modern chemistry. The cheapest and most sustainable oxidant is atmospheric oxygen (O2). This research expands on prior successes in the laboratories of Professor Doerrer, Boston University and Professor Stieglitz of Roxbury Community College (RCC) in preparing new copper (Cu) catalysts. The researchers are designing and developing new catalysts that are longer lived and more selective in their reactivity. They are also designing water-soluble catalysts to avoid the use of expensive or toxic organic solvents. A new collaboration between Boston University and Roxbury Community College develops a new summer research class that brings together BU expertise in transition metal complexes and RCC experience with natural products. Roxbury Community College (RCC) is a predominantly under-represented minority institution. The research demonstrates how to incorporate sustainability concepts into challenging and important chemical reactions. Oxidation of carbon-hydrogen (C-H) bonds remains a chemical transformation with many remaining challenges. This research builds on recent success with Cu/O2 chemistry that has demonstrated the effectiveness of fluorinated alkoxide ligands in making highly reactive species for oxidizing carbon-hydrogen bonds. The fluorinated, chelating O-donor ligands are developed to determine the effect of chelate ring size and overall metal complex charge on the oxidation reactions by {CunO2} moieties. The researchers then determine the potential breadth of this chemical formulation for oxidation catalysts. Finally, the researchers build on recent work with more earth-abundant metals from the middle of the d-block - chromium, manganese, and iron - using the fluorinated alkoxide ligands in water, a more sustainable solvent. A new collaboration between Boston University and Roxbury Community College develops a new summer research class that brings together BU expertise in transition metal complexes and RCC experience with natural products. This collaboration enhances the capacities of RCC to train under-represented minority students for science careers, while exposing them to research at an highly research intensive university.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.