The reversible redn. of protons to form hydrogen gas is known to be catalyzed by the active-site of the diiron hydrogenase, [FeFe]-H2ase. The N2S2Ni (square planar), N2S2-Co(NO) and -Fe(NO) (square pyramidal) compds. are particularly interesting as the cis-dithiolates are noted for their nucleophilicity toward a diverse variety of electrophiles and their ability to lower the redn. potentials on coordination with M(CO)x. In this project a series of [FeFe]-H2ase active site model compds. are shown to form stable addu...