The synthesis of weak chemical bonds with minimal chemical overpotential is an overlooked and under studied challenge in synthesis. This is particularly relevant in the synthesis of nitrogen-hydrogen bonds relevent to ammonia synthesis where many intermediates such as metal-dinitrogen, metal nitrido, diazenides have low driving forces, often below the thermodynamic threshold for H2 formation. Our laboratory has been exploring new routes to the synthesis of N-H bond by proton coupled electron transfer. Specific examples include exploration of metal complexes that have sufficien driving force to cleavage H<sub>2</sub> but generate weak M-H bonds that promote subsequent N-H bond formation as well as photocatalytic methods involving weak acids and an appropriate stoichiometric H-atom donor. My presentation will focus on our progress with these various strategies both in the synthesis of NH3 and the oxidation of ammonia to its elements as well as broader applications of proton coupled electron transfer as a fundamental transformation in organometallic chemistry.

Approaches to the synthesis of weak chemical bonds and application to the synthesis and oxidation of ammonia

2019 Fall National Meeting

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