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- Fryxelius, Jacob, 1974-
(författare)
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Design and Synthesis of Ligands for High-Valent Metal Oxidation Catalysts
- 2006
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This thesis describes several approaches towards the design of a water oxidation catalyst. Different aspects of coordination and water oxidation chemistry are adressed and result in various syntheses of ligands and their metal complexes.
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- Magnuson, Ann, et al.
(författare)
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High-valent Ruthenium-Manganese Complexes for Solar Energy Production.
- 2001
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Ingår i: PS2001 Proceedings.
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Konferensbidrag (refereegranskat)abstract
- We present progress in the development of artificial photosynthesis, as a means to harvesting and storage of solar energy. The plan is to compose molecular systems that combine known photochemistry with emerging functional model compounds. A photochemical device for solar energy conversion contains a photosensitizer, an electron acceptor system and a donor system that prevents charge recombination. Our goal is to utilize water as sacrificial electron donor, which will allow a net production of reducing equivalents, and the ultimate production of fuel. The only light-driven molecular catalyst for water oxidation exists in Photosystem II (PSII), which has a tetranuclear Mn-cluster in the active site. Here we present several Mn-compounds, that we have developed for the purpose of creating water-oxidizing catalysts. Our idea is to link Ru-tris(bipyridine) derivatives, which mimicks the function of the primary donor in PS II, with manganese complexes, mimicking the tetra-Mn cluster on the PSII donor side. We have constructed a number of heteronuclear complexes, containing a Ru-photosensitizer and various Mn-complexes. The compounds have been characterized with regards to their photophysical and photochemical properties, redox potentials and structure. The most promising compounds are capable of undergoing several electron transfers from the Mn-complex to the photosensitizer, leaving 3 to 4 oxidizing equivalents on the Mn. In the latest development, we have constructed ligands that stabilize higher oxidation states in Mn, in order to promote formation of Mn(V) which many believes is an intermediate in the water oxidation mechanism.
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- Thapper, Anders, et al.
(författare)
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Synthesis and Reactivity Studies of Model Complexes for Molybdopterin-Dependent Enzymes
- 2000
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Ingår i: Journal of Inorganic Biochemistry. - 1873-3344. ; 79:1-4, s. 67-74
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Tidskriftsartikel (refereegranskat)abstract
- The molybdenum cofactor (Moco)-containing enzymes are divided into three classes that are named after prototypical members of each family, viz. sulfite oxidase, DMSO reductase and xanthine oxidase. Functional or structural models have been prepared for these three prototypical enzymes: (i) The complex [MoO2(mnt)2]2− (mnt2−=1,2-dicyanoethylenedithiolate) has been found to be able to oxidize hydrogen sulfite to HSO4− and is thus a functional model of sulfite oxidase. Kinetic and computational studies indicate that the reaction proceeds via attack of the substrate at one of the oxo ligands of the complex, rather than at the metal. (ii) The coordination geometries of the mono-oxo [Mo(VI)(O-Ser)(S2)2] entity (S2=dithiolene moiety of molybdopterin) found in the crystal structure of R. sphaeroides DMSO reductase and the corresponding des-oxo Mo(IV) unit have been reproduced in the complexes [M(VI)O(OSiR3)(bdt)2] and [M(VI)O(OSiR3)(bdt)2] (M=Mo,W; bdt=benzene dithiolate). (iii) A facile route has been developed for the preparation of complexes containing a cis-Mo(VI)OS molybdenum oxo, sulfido moiety similar to that detected in the oxidized form of xanthine oxidase.
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