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Visible light-driven water oxidation catalyzed by mononuclear ruthenium complexes
KTH, School of Chemical Science and Engineering (CHE), Chemistry.
KTH, School of Chemical Science and Engineering (CHE), Chemistry.ORCID iD: 0000-0003-1662-5817
KTH, School of Chemical Science and Engineering (CHE), Chemistry.
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.ORCID iD: 0000-0002-4521-2870
2013 (English)In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 306, 129-132 p.Article in journal (Refereed) Published
Abstract [en]

A series of mononuclear ruthenium water oxidation catalysts (WOCs) [Ru(bda)L-2] (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid; L = N-cyclic aromatic ligands) were investigated in three-component light-driven water oxidation systems composed of photosensitizers, a sacrificial electron acceptor, and WOCs. A high turnover number of 579 for water oxidation was achieved in the homogeneous system using complex 4 ([Ru(bda)(4-Br-pyridine)(2)]) as the WOC, and a high quantum efficiency of 17% was found which is a new record for visible light-driven water oxidation in homogeneous systems.

Place, publisher, year, edition, pages
2013. Vol. 306, 129-132 p.
Keyword [en]
Photochemistry, Homogeneous catalysis, Water oxidation, Ruthenium, Quantum yield
National Category
Other Chemistry Topics
Identifiers
URN: urn:nbn:se:kth:diva-129437DOI: 10.1016/j.jcat.2013.06.023ISI: 000323865500013Scopus ID: 2-s2.0-84881158429OAI: oai:DiVA.org:kth-129437DiVA: diva2:652931
Funder
Swedish Energy Agency
Note

QC 20131002

Available from: 2013-10-02 Created: 2013-09-30 Last updated: 2017-12-06Bibliographically approved
In thesis
1. Artificial Photosynthesis: Molecular Catalysts for Water Oxidation
Open this publication in new window or tab >>Artificial Photosynthesis: Molecular Catalysts for Water Oxidation
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Artificial photosynthesis provides a promising solution to the future sustainable energy system. Water is the only suitably sufficient protons and electrons supplier by the reaction of water oxidation. However, this reaction is both kinetically and thermodynamically demanding, leading to a sluggish kinetics unless the introduction of a catalyst.The theme of this thesis is to design, synthesize and evaluate molecular catalysts for water oxidation. This thesis consists of seven parts:The first chapter presents a general introduction to the field of homogenous catalysis of water oxidation, including catalysts design, examination and mechanistic investigation.The second chapter investigates the electronic and noncovalent-interaction effects of the ligands on the activities of the catalysts.In the third chapter, halogen substitutes are introduced into the axial ligands of the ruthenium catalysts. It is proved that the hydrophobic effect of the halogen atom dramatically enhanced the reactivity of the catalysts.Chapter four explores a novel group of ruthenium catalysts with imidazole-DMSO pair of axial ligands, in which the DMSO is proved to be crucial for the high efficiency of the catalysts.Chapter five describes the light-driven water oxidation including the three-component system and the sensitizer-catalyst assembled system. It is found that the common Ru(bpy)32+ dye can act as an electron relay and further benefit the electron transfer as well as the photo-stability of the system.In chapter six, aiming to the future application, selected ruthenium catalysts have been successfully immobilized on electrodes surfaces, and the electrochemical water oxidation is achieved with high efficiency.Finally, in the last chapter, a novel molecular catalyst based on the earth abundant metal ―nickel has been designed and synthesized. The activities as well as the mechanism have been explored.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. 82 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:40
Keyword
artificial photosynthesis, water oxidation, ruthenium complexes, nickel complexes, cerium, photo-catalysts, photosensitizer, electrochemistry, immobilization.
National Category
Organic Chemistry Physical Chemistry
Research subject
Chemistry; Energy Technology
Identifiers
urn:nbn:se:kth:diva-173622 (URN)978-91-7595-659-6 (ISBN)
Public defence
2015-10-13, F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Swedish Energy Agency
Note

QC 20150916

Available from: 2015-09-16 Created: 2015-09-15 Last updated: 2015-09-16Bibliographically approved

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Duan, LeleSun, Licheng

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