In the search for sustainable energy solutions, the idea of artificial photosynthesis has been proposed as an approach with which to use water and sunlight to produce hydrogen. Key in the... Show moreIn the search for sustainable energy solutions, the idea of artificial photosynthesis has been proposed as an approach with which to use water and sunlight to produce hydrogen. Key in the development of hydrogen production technologies is the splitting of water using a water oxidation catalyst. In this thesis, the water splitting catalytic process was investigated using a number of different computational techniques. Computationally, the water splitting catalytic process has traditionally been considered statically as a number of snapshots, and in vacuum. The traditional approaches also often include a number of correction factors for the charge carriers in the reaction. But because catalytic processes are dynamic, a novel approach was also developed in this thesis. With this approach, one can examine the dynamic transition from one catalytic intermediate to another, in a fully solvated environment. In optimising water oxidation catalysts it is important to consider the interaction with the surrounding environment, and how this can impact the catalytic reaction. Furthermore, in the new approach all the charge carriers–protons and electrons–are included in a dynamic simulation. These techniques give us a better idea of the things needed in the optimisation of water oxidation catalysts. Show less
The aim of this dissertation is to construct and explore artificial oxygen evolving complexes that are synthetically accessible, stable, functionally robust and efficient. To achieve this, a class... Show moreThe aim of this dissertation is to construct and explore artificial oxygen evolving complexes that are synthetically accessible, stable, functionally robust and efficient. To achieve this, a class of mono metal water splitting catalysts is introduced in this manuscript and exploitation of these complexes in homogeneous catalysis and in electrochemical studies with surface immobilized catalyst assemblies has been discussed. The catalysts are comprised of a single centre ruthenium or iridium metal core coordinated to a dinitrogen ligand and stabilized by a cyclic conjugated hydrocarbon. Homogeneous catalytic water oxidation is performed with a chemical oxidant as catalyst activator. For electro-assisted experiments, the catalyst complexes are functionalized with carboxylic or phosphonic acid linker units on the dinitrogen ligand that serve as anchoring sites for deposition on conducting oxide electrodes. The electrochemical water splitting systems with molecular catalysts have potential application in e.g. rooftop devices to make personalized energy carriers. The proposed __Artificial Leaf__ will soon be the future outcome of the present day technology and efforts in this field. Cheap and easy accessible hydrogen will not only serve as fuel for transportation but also as driving force for green power generation. Show less
