Synthesis and reactivity of pyridinediimine iron complexes: for the breakdown of carbon dioxide

The increase of greenhouse gases in our atmosphere, particularly carbon dioxide (CO2), has been recognized by the scientific, industrial, and political communities. The increase in CO2 concentration has been connected to negative effects on our environment (global warming). Despite the negative associations of CO2, chemists can synthesize useful organic products and fuel from it. Ideally, the two electron reduction of CO2 to CO can provide one of the two products of synthesis gas (CO and H2), which is used in the Fischer-Tropsch process to produce diesel fuel. This thesis aims to convert CO2 to CO, using a cheap and abundant metal, Fe. The research presented herein focuses on the redox-active capability of pyridinediimine (PDI) ligands and their promotion of the CO2-to-CO conversion on Fe(II). Furthermore, the chemical and electrochemical release of CO on Fe(II) has shown to complete the CO2-to-CO cycle. Additional studies with varying Lewis acids and Lewis bases located within the secondary coordination sphere of the PDIFe complex will be discussed. These studies demonstrated the electronic effects on the reduction-oxidation potential of the CO release in PDIFe(CO)2 complexes