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Artificial Water Sp...
Artificial Water Splitting: Ruthenium Complexes for Water Oxidation
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- Duan, Lele, 1982- (författare)
- KTH,Organisk kemi,Licheng Sun's group
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- Sun, Licheng, Professor (preses)
- KTH,Organisk kemi
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- Beller, Matthias, Professor (opponent)
- Leibniz-Institut für Katalyse e. V., Albert-Einstein-Str. 29 a, 18059 Rostock, Germany
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(creator_code:org_t)
- ISBN 9789175010830
- Stockholm : KTH Royal Institute of Technology, 2011
- Engelska 80 s.
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Serie: Trita-CHE-Report, 1654-1081 ; 2011:48
- Relaterad länk:
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https://kth.diva-por... (primary) (Raw object)
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https://urn.kb.se/re...
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Abstract
Ämnesord
Stäng
- This thesis concerns the development and study of Ru-based water oxidation catalysts (WOCs) which are the essential components for solar energy conversion to fuels. The first chapter gives a general introduction about the field of homogenous water oxidation catalysis, including the catalytic mechanisms and the catalytic activities of some selected WOCs as well as the concerns of catalyst design. The second chapter describes a family of mononuclear Ru complexes [Ru(pdc)L3] (H2pdc = 2,6-pyridinedicarboxylic acid; L = pyridyl ligands) towards water oxidation. The negatively charged pdc2− dramatically lowers the oxidation potentials of Ru complexes, accelerates the ligand exchange process and enhances the catalytic activity towards water oxidation. A Ru aqua species [Ru(pdc)L2(OH2)] was proposed as the real catalyst. The third chapter describes the analogues of [Ru(terpy)L3]2+ (terpy = 2,2′:6′,2′′-terpyridine). Through the structural tailor, the ligand effect on the electrochemical and catalytic properties of these Ru complexes was studied. Mechanistic studies suggested that these Ru-N6 complexes were pre-catalysts and the Ru-aqua species were the real WOCs. The forth chapter describes a family of fast WOCs [Ru(bda)L2] (H2bda = 2,2′-bipyridine-6,6′-dicarboxylic acid). Catalytic mechanisms were thoroughly investigated by electrochemical, kinetic and theoretical studies. The main contributions of this work to the field of water oxidation are (i) the recorded high reaction rate of 469 s−1; (ii) the involvement of seven-coordinate Ru species in the catalytic cycles; (iii) the O-O bond formation pathway via direct coupling of two Ru=O units and (iv) non-covalent effects boosting up the reaction rate. The fifth chapter is about visible light-driven water oxidation using a three component system including a WOC, a photosensitizer and a sacrificial electron acceptor. Light-driven water oxidation was successfully demonstrated using our Ru-based catalysts.
Ämnesord
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
Nyckelord
- water oxidation
- ruthenium
- electrochemistry
- DFT calculation
- photoelectrochemistry
- negatively charged ligand
- catalyst
Publikations- och innehållstyp
- vet (ämneskategori)
- dok (ämneskategori)
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