This dissertation covers the exciting field of hydrogenase model compounds. Due to the increasing energy demand on our planet, it is necessary to pursue new ways to satisfy this demand. One possibility is the generation of hydrogen as in natural hydrogenases. Of particular interest is the possibility to avoid expensive precious metals such as platinum, which is still the mainly used catalyst in industry, but instead to employ cheap earth-abundant metals as catalysts. The syntheses and characterisation of two new [FeFe]-hydrogenase model compounds based on a [3Fe2S] cluster bridged with diphosphines is presented. One compound is bridged by methylene, which is the simplest case and a second compound is bridged by the electron-rich ferrocene subunit. It is especially important to differentiate between electrochemical and photochemical properties. For this reason, a substantial part of this work concentrates on irradiation experiments and investigations with cyclic voltammetry with variable parameters. To prove the hydrogen evolution, electrolysis with headspace-GC analysis has been performed as well. Additionally, more advanced investigations such as Mössbauer spectroscopy or measurements in the field of ultrafast vibrational spectroscopy with collaborations in Salzburg and Amsterdam have been performed. The work presented here has built a foundation for the application of novel iron-based catalyst systems developed for bioinspired generation of hydrogen. Parts of this work have already been published.