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

Abstract

Air Force Materiel Command REPORT DOCUMENTATION PAGEForm Public reporting burden for this collection of information is estimated to average 1 hour per response, including the time for reviewing instructions, searching existing data sources, gathering and maintaining the data needed, and completing and reviewing this collection of information. Send comments regarding this burden estimate or any other aspect of this collection of information, including suggestions for reducing this burden to Department of Defense, Washington Headquarters Services, Directorate for Information Our first support from the AFRSO 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 AFSRO 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.Ammonia, hydrazine, N2, H2, renewable hydrogen, nitrogen-based, hydrogen atom transfer ( Executive Summary. 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, N 2 and H 2 . If successful, such research would be transformative as these important fuels and energy storage media could be synthesized under batch type conditions compatible with sources of renewable hydrogen. Thus, our efforts would be significant in reducing the carbon footprint associated with the synthesis of many nitrogen-based propellants and fuels. Key to our program has been the recognition 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 N 2 fixation. Earth abundant transition metals such as vanadium, titanium and molybdenum...