Hydrogen has emerged as one of the most promising alternative fuels, with hydrogenase enzymes gaining a large amount of attention because of their ability to reversibly reduce protons to hydrogen with high kinetic rates under mild conditions. Properly understanding this catalytic mechanism would advance the development of hydrogenase mimics that could be used in hydrogen fuel applications. [Fe(η⁵-C₅H₅)(CO)₂]₂ (Fp₂) is a model complex that has features similar to the active sites of hydrogenases, including functioning in a catalytic cycle that reduces protons to hydrogen. The intermediates in this catalytic cycle can be studied in detail in terms of structure and energy to gain insight into the catalytic cycle of hydrogenases. Density functional calculations and cyclic voltammetry were used to develop a mechanism for Fp₂ catalytically generating H₂. The proposed mechanism provides comment on essential features of hydrogenases.