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Visible light-driven water oxidation catalyzed by mononuclear ruthenium complexes
KTH, Skolan för kemivetenskap (CHE), Kemi.
KTH, Skolan för kemivetenskap (CHE), Kemi.ORCID-id: 0000-0003-1662-5817
KTH, Skolan för kemivetenskap (CHE), Kemi.
KTH, Skolan för kemivetenskap (CHE), Kemi, Organisk kemi.ORCID-id: 0000-0002-4521-2870
2013 (Engelska)Ingår i: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 306, s. 129-132Artikel i tidskrift (Refereegranskat) 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.

Ort, förlag, år, upplaga, sidor
2013. Vol. 306, s. 129-132
Nyckelord [en]
Photochemistry, Homogeneous catalysis, Water oxidation, Ruthenium, Quantum yield
Nationell ämneskategori
Annan kemi
Identifikatorer
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, id: diva2:652931
Forskningsfinansiär
Energimyndigheten
Anmärkning

QC 20131002

Tillgänglig från: 2013-10-02 Skapad: 2013-09-30 Senast uppdaterad: 2017-12-06Bibliografiskt granskad
Ingår i avhandling
1. Artificial Photosynthesis: Molecular Catalysts for Water Oxidation
Öppna denna publikation i ny flik eller fönster >>Artificial Photosynthesis: Molecular Catalysts for Water Oxidation
2015 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Stockholm: KTH Royal Institute of Technology, 2015. s. 82
Serie
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:40
Nyckelord
artificial photosynthesis, water oxidation, ruthenium complexes, nickel complexes, cerium, photo-catalysts, photosensitizer, electrochemistry, immobilization.
Nationell ämneskategori
Organisk kemi Fysikalisk kemi
Forskningsämne
Kemi; Energiteknik
Identifikatorer
urn:nbn:se:kth:diva-173622 (URN)978-91-7595-659-6 (ISBN)
Disputation
2015-10-13, F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (Engelska)
Opponent
Handledare
Forskningsfinansiär
Energimyndigheten
Anmärkning

QC 20150916

Tillgänglig från: 2015-09-16 Skapad: 2015-09-15 Senast uppdaterad: 2019-12-20Bibliografiskt granskad

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Totalt: 564 träffar
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