@phdthesis{Kunz2018,
  author    = {Kunz, Valentin},
  title     = {Supramolecular Approaches for Water Oxidation Catalysis with Ruthenium Complexes},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-154820},
  school      = {Universit{\"a}t W{\"u}rzburg},
  year      = {2018},
  abstract  = {The catalytic splitting of water into its elements is an important reaction to establish hydrogen as a solar fuel. The bottle-neck of this process is considered to be the oxidative half reaction generating oxygen, and good catalysts are required to handle the complicated redox chemistry involved. As can be learned from nature, the incorporation of the catalytically active species into an appropriate matrix can help to improve the overall performance. Thus, the aim of the present thesis was to establish novel supramolecular approaches to improve water oxidation catalysis using the catalytically active {Ru(bda)} fragment as key motive (bda = 2,2'-bipyridine-6,6'-dicarboxylate). First, the synthesis of ruthenium catalysts gathering three {Ru(bda)} water oxidation subunits in a macrocyclic fashion is described. By using bridging bipyridine ligands of different lengths, metallosupramolecular macrocycles with distinct sizes have been obtained. Interestingly, an intermediate ring size has been proven to be optimal for the catalytic water oxidation. Detailed kinetic, spectroscopic, and theoretical studies helped to identify the reaction mechanism and to rationalize the different catalytic activities. Furthermore, solubilizing side chains have been introduced for the most active derivative to achieve full water solubility. Secondly, the {Ru(bda)} fragment was embedded into supramolecular aggregates to generate more stable catalytic systems compared to a homogeneous reference complex. Therefore, the catalyst fragment was equipped with axial perylene bisimide (PBI) ligands, which facilitate self-assembly. Moreover, the influence of the different accessible aggregate morphologies on the catalytic performance has been investigated.},
  subject      = {Ruthenium Komplexe},
  language  = {en}
}
@phdthesis{MezaChincha2021,
  author    = {Meza Chincha, Ana Lucia},
  title     = {Catalytic Water Oxidation with Functionalized Ruthenium Macrocycles},
  doi       = {10.25972/OPUS-20962},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-209620},
  school      = {Universit{\"a}t W{\"u}rzburg},
  year      = {2021},
  abstract  = {In light of the rapidly increasing global demand of energy and the negative effects of climate change, innovative solutions that allow an efficient transition to a carbon-neutral economy are urgently needed. In this context, artificial photosynthesis is emerging as a promising technology to enable the storage of the fluctuating energy of sunlight in chemical bonds of transportable "solar fuels". Thus, in recent years much efforts have been devoted to the development of robust water oxidation catalysts (WOCs) leading to the discovery of the highly reactive Ru(bda) (bda: 2,2'-bipyridine-6,6'-dicarboxylic acid) catalyst family. The aim of this thesis was the study of chemical and photocatalytic water oxidation with functionalized Ruthenium macrocycles to explore the impact of substituents on molecular properties and catalytic activities of trinuclear macrocyclic Ru(bda) catalysts. A further objective of this thesis comprises the elucidation of factors that influence the light-driven water oxidation process with this novel class of supramolecular WOCs.},
  subject      = {Rutheniumkomplexe},
  language  = {en}
}
@phdthesis{Schindler2022,
  author    = {Schindler, Dorothee},
  title     = {Water Oxidation with Multinuclear Ruthenium Catalysts},
  doi       = {10.25972/OPUS-23309},
  url       = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-233093},
  school      = {Universit{\"a}t W{\"u}rzburg},
  year      = {2022},
  abstract  = {In terms of the need of environmentally benign renewable and storable energy sources, splitting of water into hydrogen and oxygen by using sunlight is a promising approach. Hereby, water oxidation catalysts (WOCs) are required to perform the water oxidation comprising the transfer of four electrons to provide the reducing equivalents for producing hydrogen. The class of Ru(bda) (bda = 2,2'-bipyridine-6,6'-dicarboxylate) catalysts has proven to be efficient for this reaction. In this thesis, ligand exchange processes in Ru(bda) complexes have been analyzed and the formation of multinuclear macrocyclic WOCs was studied. Based on the knowledge acquired by these studies, new multinuclear cyclic Ru(bda) complexes have been synthesized and their catalytic efficiencies in homogeneous water oxidation have been investigated. Going one step further for setting up functional devices, molecular WOCs have been immobilized on conducting or semiconducting supporting materials. Direct anchoring on carbon nanotubes generated a promising materials for further applications.},
  subject      = {Rutheniumkomplexe},
  language  = {en}
}