Unraveling the mechanism of biomimetic hydrogen fuel production A computational study

[FeFe] hydrogenase enzymes can reversibly catalyze the conversion of protons into molecular hydrogen. The active site of the [FeFe] hydrogenase enzyme has inspired many biomimetic catalysts to produce molecular hydrogen. A fundamental understanding of the reaction mechanism of the enzyme could help in designing better biomimetic catalysts. The active site of the [FeFe] hydrogenase enzyme is buried inside the protein. The transport of electrons and protons to the active site of the protein is crucial for an efficient catalytic cycle. In this thesis we used computational techniques to understand the transport process as well as the reaction mechanism of the enzyme and the catalysts and finally provides a guideline in choosing various ligands for designing a biomimetic catalyst. Classical molecular dynamics, QM/MM and DFT-MD are used in this study for an elaborative understanding of electron transfer, proton transfer and reaction mechanism.