Catalysts that efficiently interconvert between electrical energy and chemical bonds (fuels) are needed for sustainable, secure energy. Oxidation of ammonia by molecular complexes is a burgeoning area of research that poses crucial scientific challenges that must be addressed. Understanding the thermodynamics of the elementary steps in which the N-H bond is cleaved can contribute to improved reactivity. We have focused on the design of molecular catalysts for oxidation of NH3 to give N2, using aryloxy radicals to abstract H atoms from M-NH3 complexes. A key challenge is balancing the need for cleavage of N-H bonds and the formation of an N-N bond. Computational studies closely coupled with experimental studies have been pivotal to progress, as they provide an atomistic picture and give energetics for intermediates that have not been observed experimentally. We show how using both experimental and theoretical methods have advanced our understanding of catalytic oxidation of NH3.

Oxidation of ammonia by molecular complexes

ACS Spring 2022

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