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Oxygen evolution at functionalized carbon surfaces: A strategy for immobilization of molecular water oxidation catalysts
KTH, Skolan för kemivetenskap (CHE), Kemi, Organisk kemi.
KTH, Skolan för informations- och kommunikationsteknik (ICT), Mikroelektronik och tillämpad fysik, MAP.
KTH, Skolan för kemivetenskap (CHE), Kemi, Organisk kemi.ORCID-id: 0000-0002-4521-2870
2012 (Engelska)Ingår i: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 48, nr 80, s. 10025-10027Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

A molecular Ru(ii) water oxidation catalyst was immobilized on a conductive carbon surface through a covalent bond, and its activity was maintained at the same time. The method can be applied to other materials and may inspire development of artificial photosynthesis devices.

Ort, förlag, år, upplaga, sidor
2012. Vol. 48, nr 80, s. 10025-10027
Nyckelord [en]
Mononuclear Ruthenium Complexes, Electrolysis, Chemistry, Azide
Nationell ämneskategori
Kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-103519DOI: 10.1039/c2cc35379bISI: 000308653800022PubMedID: 22945420Scopus ID: 2-s2.0-84866391677OAI: oai:DiVA.org:kth-103519DiVA, id: diva2:561052
Forskningsfinansiär
VetenskapsrådetKnut och Alice Wallenbergs Stiftelse
Anmärkning

QC 20121017

Tillgänglig från: 2012-10-17 Skapad: 2012-10-15 Senast uppdaterad: 2020-03-09Bibliografiskt granskad
Ingår i avhandling
1. Mononuclear Ruthenium Complexes that Catalyze Water to Dioxgen Oxidation
Öppna denna publikation i ny flik eller fönster >>Mononuclear Ruthenium Complexes that Catalyze Water to Dioxgen Oxidation
2012 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

The theme of this thesis is the development of mononuclear Ru-based complexes that are capable of catalyzing the water oxidation (or O2-evolving) reaction, e.g. 2 H2O → O2 + 4 H+ + 4 e. Several families of mononuclear Ru water oxidation catalysts were designed and prepared. They feature with anionic ancillary ligands that contain carboxylate or phenolate donors. The properties of the catalysts were investigated in various aspects including coordination geometry, electrochemical behavior, and ligand exchange. All catalysts showed outstanding catalytic activity towards water oxidation in the presence of cerium(IV) ammonium nitrate as a sacrificial oxidant. High-valent Ru intermediates involved in the reactions were characterized both experimentally and theoretically. The kinetics of catalytic water oxidation was examined based on one catalyst and a prevailing catalytic pathway was proposed. The catalytic cycle involved a sequence of oxidation steps from RuII−OH2 to RuV=O species and O−O bond formation via water-nucleophilic-attack to the RuV=O intermediate. By comparing properties and catalytic performance of Ru catalysts herein with that of previously reported examples, the effect of anionic ancillary ligands was clearly elucidated in the context of catalytic water oxidation. Aiming to further application in an envisaged artificial photosynthesis device, visible light-driven water oxidation was conducted and achieved primarily in a homogeneous three-component system containing catalyst, photosensitizer, and sacrificial electron acceptor. Moreover, one model Ru catalyst was successfully immobilized on ordinary glass carbon surface through a facile and widely applicable method.

Ort, förlag, år, upplaga, sidor
Stockholm: KTH Royal Institute of Technology, 2012. s. 101
Serie
Trita-CHE-Report, ISSN 1654-1081 ; 2012:55
Nyckelord
Ruthenium complex, Homogeneous catalysis, Water oxidation, O2 evolution, anionic ligand, Molecular catalyst, Electrocatalysis, Kinetics, Artificial photosynthesis, Light-driven, Immobilization of catalyst
Nationell ämneskategori
Organisk kemi Oorganisk kemi Energisystem
Identifikatorer
urn:nbn:se:kth:diva-104765 (URN)978-91-7501-517-0 (ISBN)
Disputation
2012-11-30, F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (Engelska)
Opponent
Handledare
Anmärkning

QC 20121112

Tillgänglig från: 2012-11-12 Skapad: 2012-11-12 Senast uppdaterad: 2019-12-20Bibliografiskt granskad

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