Because of the pressing need for sustainable energy sources, H<sub>2</sub> has received increased attention as an environmentally benign energy source. Hydrogenases, metalloenzymes that catalyze the reversible oxidation of H<sub>2</sub>, are ubiquitous throughout nature. However, synthetic efforts to replicate hydrogenases have struggled with low efficiency, short life spans, and the need for high catalyst loading. This arises, in part, because of the limited understanding of the enzymatic mechanism. The mechanism of [NiFe]-hydrogenase, the most prevalent family of hydrogenases in nature, has been the focus of significant research efforts since the crystallographic determination of the active site in 1995, however the understanding of metal center, in particular the role of the iron, remains poorly understood. It has been determined that the redox chemistry happens solely at the Ni-center, however the Fe-center is necessary. In previous synthetic systems, the Ni(II) precursor has shown limited catalytic activity compared to the Ni(II)-Fe(II) complex, while the Fe(II) precursor was catalytically inert, further demonstrating the important, yet secondary, role of the Fe-center. This poster will discuss the synthesis and characterization of a series of tetradentate sulfur ligands and their corresponding Ni(II) complexes as precursors for a series of [NiFe]-hydrogenase mimics. The reactivity of the Ni(II) complexes will also be discussed.

Synthesis and characterization of novel nickel(II) complexes as precusors to [NiFe]-hydrogenase mimetic compounds

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