Dissertation

Biomimetic models of [NiFe] hydrogenase for electrocatalytic hydrogen evolution

Author: Gezer, G.
Date: 10 October 2017
Links: Thesis in Leiden Repository

The growing demand of energy indicates that global energy resources in the form of fossil fuels will not be sufficient in the future. In order to solve potential future energy problems development of a sustainable hydrogen economy is highly desirable. Researchers are looking for new and cleaner ways for the production of dihydrogen gas. The structure and function of hydrogenases have raised the attention of synthetic chemists in the past decades, since new catalysts for proton reduction may be developed by using biomimetic, functional models of hydrogenases. Three types of hydrogenases are known, being the [FeFe], [Fe] and [NiFe] hydrogenases.A significant amount of data has been gathered over the years concerning the enzyme redox states and the reaction mechanism for the reversible heterolytic splitting of dihydrogen at the [NiFe] hydrogenase active site. The [NiFeSe] hydrogenases form a subclass of the [NiFe] hydrogenases, in which one of the cysteines (Cys) in the active site of the enzyme is replaced by selenocysteine (Sec). This thesis deals with the synthesis and characterization of new structural and functional models of the nickel-containing enzymes [NiFe] and [NiFeSe] hydrogenases for electrocatalytic hydrogen evolution.

electrocatalysis