Molecular catalytic system for efficient water splitting

Abstract

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 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.

Water splittingTurnover numberTurnover frequencySolar fuelOxygen evolving catalystOverpotentialArtificial leaf