Synthesis of Fuels and Value-Added Nitrogen-Containing Compounds from N2.

摘要

Our first support from the AFOSR enabled investigations for our research group to explore new paradigms for the interconversion of ammonia and hydrazine with its elements, N2 and H2. Our research is potentially transformative to synthesize these important fuels and energy storage media under batch type conditions compatible with sources of renewable hydrogen. Our efforts are significant for reducing the carbon footprint associated with the synthesis of many nitrogen-based propellants and fuels. Our program identified of the role of hydrogen atom transfer (HAT) as a new method for making and breaking N-H bonds and its influence on the reversible cleavage of strong N-N bonds. Our AFOSR funded program has also definitely established that redox-active ligands -- those that can undergo reversible one electron transfer events with a transition metal -- have a transformative impact on the thermochemistry associated with N-H bonds in important nitrogen-containing intermediates relevant to catalytic cycles for N2 fixation with earth abundant metals. Our findings have provided new catalysis concepts to be explored in developing and understanding the molecular dynamics of catalysis involving N2, hydrazine and ammonia.