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

by Julius Scholz
Doctoral thesis
Date of Examination:2017-06-26
Date of issue:2017-11-03
Advisor:Prof. Dr. Christian Jooß
Referee:Prof. Dr. Christian Jooß
Referee:Prof. Dr. Sven Schneider
Referee:Prof. Dr. Franc Meyer
Referee:Prof. Dr. Vasily Moshnyaga
Referee:Prof. Dr. Inke Siewert
Referee:Dr. Martin Wenderoth
Persistent Address: http://dx.doi.org/10.53846/goediss-6564

 

 

Files in this item

Name:Dissertation_Scholz.pdf
Size:41.1Mb
Format:PDF
Description:Dissertation

The following license files are associated with this item:

Abstract

English

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
 
Statistik