Abstract

The production of ammonia (NH3) from atmospheric dinitrogen is one of the most important and challenging chemical transformations. In addition to NH3 being invaluable for the production of fertilizers necessary to sustain global agriculture, NH3 is also an appealing nitrogen-based fuel due to its high energy density and ease of storage and distribution. However, producing NH3 from N2 using industrial Haber-Bosch catalysts is a highly energy-intensive process. Developing efficient electrocatalysts for NH3 production from N2, and protons and electrons, could augment this energy intensive process and enable distributed facilities for on-demand NH3 production. Moreover, catalysts for the reverse reaction, NH3 oxidation, will be essential to utilize the energy stored in N-H bonds. This presentation will describe iron and chromium complexes with tetradentate phosphine ligands to catalyze N2 reduction. M-NH3 complexes supported by bidentate phosphine ligands containing non-coordinating pendant amines for the catalytic oxidation of NH3 to N2 will also be discussed. The synthesis and initial electrochemical studies of these systems will be described.

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