Hybrid systems of molecular ruthenium catalyst anchored on oxide films for water oxidation: Functionality of the interface

von Julius Scholz
Dissertation
Datum der mündl. Prüfung:2017-06-26
Erschienen:2017-11-03
Betreuer:Prof. Dr. Christian Jooß
Gutachter:Prof. Dr. Christian Jooß
Gutachter:Prof. Dr. Sven Schneider
Gutachter:Prof. Dr. Franc Meyer
Gutachter:Prof. Dr. Vasily Moshnyaga
Gutachter:Prof. Dr. Inke Siewert
Gutachter:Dr. Martin Wenderoth
Zum Verlinken/Zitieren: http://dx.doi.org/10.53846/goediss-6564

 

 

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Englisch

The scope of the presented thesis is the realization and detailed analysis of a hybrid system for photoelectrochemical watersplitting with La$_{0.6}$Sr$_{0.4}$MnO$_3$ (LSMO) as photoabsorber and immobilized molecular bis(bipyridyl)pyrazolate diruthenium (Ru$_2$-bbp) catalyst. As a first step towards a full functioning photochemical device, the functionality of the hybrid assembly was elucidated electrochemically since the basic requirements for a photochemical device, such as stability and band alignment need to be also fulfilled for an electrochemical cell. The results herein focused on two main parts: (I) the role of LSMO as a solid support in terms of background activity and stability involving first models for the water oxidation mechanism and strategies to tailor the stability; (II) the behavior of the Ru$_2$-bbp complex upon immobilization on a model oxide electrode including the functionality of the anchoring via acid functionalities and possible destabilization pathways. In these studies the method of rotating ring-disk electrodes (RRDE) played a key role and their advancements enabled in depth analysis on the activity and stability.
Keywords: water oxidation; artificial photosynthesis; rotating ring-disk electrode; manganite; perovskite; X-ray photoemission spectroscopy; immobilization; structural control; stability
 
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