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 the development of molecular M-N2 and M-NH3 complexes using earth-abundant transition metals, supported by bidentate and multidentate phosphine ligands containing non-coordinating pendant amines, to catalyze N2 reduction and NH3 oxidation reactions. The synthesis, catalytic reactivity, and initial electrochemical studies of these systems will be described.

Transition metal complexes for N2 reduction and NH3 oxidation: Strategies for making and breaking N≡N and N-H bonds

254th National Meeting (2017)

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