Nitrogenase is the complex metalloenzyme responsible for biological dinitro
gen reduction. This reaction represents the single largest contributor to t
he reductive portion of the global nitrogen cycle. Recent developments in u
nderstanding the mechanism of the Mo-based nitrogenase are reviewed. Topics
include how nucleotide binding and hydrolysis are coupled to electron tran
sfer and substrate reduction, how electrons are accumulated and transferred
within the MoFe-protein, and how substrates bind and are reduced at the ac
tive site metal cluster.