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Catalyst-solvent interactions in a dinuclear Ru-based water oxidation catalyst
Stockholm University, Faculty of Science, Department of Organic Chemistry.ORCID iD: 0000-0002-7249-7437
Stockholm University, Faculty of Science, Department of Organic Chemistry. Nuclear Materials Authority, Egypt.
Stockholm University, Faculty of Science, Department of Organic Chemistry.
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2016 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 45, no 47, p. 19024-19033Article in journal (Refereed) Published
Abstract [en]

Photocatalytic water oxidation represents a key process in conversion of solar energy into fuels and can be facilitated by the use of molecular transition metal-based catalysts. A novel straightforward approach for covalent linking of the catalytic units to other moieties is demonstrated by preparation of a dinuclear complex containing two [Ru(pdc)(pic)(3)]-derived units (pdc = 2,6-pyridinedicarboxylate, pic = 4-picoline). The activity of this complex towards chemical and photochemical oxidation of water was evaluated and a detailed insight is given into the interactions between the catalyst and acetonitrile, a common co-solvent employed to increase solubility of water oxidation catalysts. The solvent-induced transformations were studied by electrochemical and spectroscopic techniques and the relevant quantitative parameters were extracted.

Place, publisher, year, edition, pages
2016. Vol. 45, no 47, p. 19024-19033
National Category
Organic Chemistry
Research subject
Organic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-139388DOI: 10.1039/c6dt03789eISI: 000390082900029PubMedID: 27853776OAI: oai:DiVA.org:su-139388DiVA, id: diva2:1072221
Funder
Swedish Research CouncilKnut and Alice Wallenberg FoundationCarl Tryggers foundation Available from: 2017-02-07 Created: 2017-02-06 Last updated: 2019-12-12Bibliographically approved
In thesis
1. Ru-Based Water Oxidation Catalysts: Development and Mechanistic Studies
Open this publication in new window or tab >>Ru-Based Water Oxidation Catalysts: Development and Mechanistic Studies
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Oxidation of water constitutes one of the most challenging processes in artificial photosynthesis, which aims at storing solar energy in the form of chemical bonds of high-energy fuels. To facilitate this process, efficient and durable water oxidation catalysts have to be developed and integrated into the complete photosynthetic cells. Importantly, the intricate complexity of such devices requires the catalyst not only to be highly efficient and robust, but also operate through a well-defined mechanism.

This thesis describes the development and mechanistic studies of new water oxidation catalysts based on ruthenium. The first part of the thesis describes the synthesis of a dinuclear ruthenium-based catalyst active for both chemical and light-driven water oxidation. This catalyst displayed a pronounced influence of the acetonitrile co-solvent on the redox properties, which was studied in detail by electrochemical methods. In the second part, a new benzimidazole-based mononuclear catalyst was evaluated. The activity of the catalyst was studied for chemical and light-driven water oxidation, and insight into the operating mechanism was provided with the help of density functional theory calculations. In the third part of the thesis, a new mononuclear ruthenium-based catalyst was prepared and evaluated for electrochemically-driven water oxidation. This catalyst displayed activity similar to that of the current state-of-the-art water oxidation catalyst, while eliminating its main drawback, that is incomplete activation. The redox properties of the new catalyst were studied in detail by electrochemical and spectroscopic techniques, providing insight into the origins of its improved performance. Finally, in the fourth part of the thesis, a heterogeneous nanoparticulate catalyst immobilized on a solid support is described. The catalyst displayed high activity and stability during chemical and light-driven water oxidation, which was attributed to the small average particle size and efficient anchoring of the catalyst to the heterogeneous support via an oxidatively-stable linker.

Place, publisher, year, edition, pages
Stockholm: Department of Organic Chemistry, Stockholm University, 2018. p. 73
Keywords
ruthenium, catalysis, water oxidation, artificial photosynthesis
National Category
Organic Chemistry
Research subject
Organic Chemistry
Identifiers
urn:nbn:se:su:diva-160718 (URN)978-91-7797-466-6 (ISBN)978-91-7797-467-3 (ISBN)
Public defence
2018-12-05, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 3: Manuscript.

Available from: 2018-11-12 Created: 2018-10-18 Last updated: 2018-11-02Bibliographically approved

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Shatskiy, AndreyAbdel-Magied, Ahmed F.Rabten, WangchukLaine, Tanja M.Sun, JunliangAndersson, Pher G.Kärkäs, Markus D.Johnston, Eric V.Åkermark, Björn
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