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Dinuclear Manganese Complexes for Artificial Photosynthesis: Synthesis and Properties
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
2005 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

This thesis deals with the synthesis and characterisation of a series of dinuclear manganese complexes. Their ability to donate electrons to photo-generated ruthenium(III) has been investigated in flash photolysis experiments followed by EPR-spectroscopy. These experiment shows several consecutive one-electron transfer steps from the manganese moiety to ruthenium(III), that mimics the electron transfer from the oxygen evolving centre in photosystem II.

The redox properties of these complexes have been investigated with electro chemical methods and the structure of the complexes has been investigated with different X-ray techniques. Structural aspects and the effect of water on the redox properties have been shown.

One of the manganese complexes has been covalently linked in a triad donor-photosensitizer-acceptor (D–P–A) system. The kinetics of this triad has been investigated in detail after photo excitation with both optical and EPR spectroscopy. The formed charge separated state (D–P–A+) showed an unusual long lifetime for triad based on ruthenium photosensitizers.

The thesis also includes a study of manganese-salen epoxidation reactions that we believe can give an insight in the oxygen transfer mechanism in the water oxidising complex in photosystem II.

sted, utgiver, år, opplag, sider
Stockholm: Institutionen för organisk kemi , 2005. , s. 49
Emneord [en]
Crystal Structure, Artificial photosynthesis, Manganese complex
HSV kategori
Identifikatorer
URN: urn:nbn:se:su:diva-396ISBN: 91-7155-018-6 (tryckt)OAI: oai:DiVA.org:su-396DiVA, id: diva2:193361
Disputas
2005-03-18, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 12 A, Stockholm, 10:00
Opponent
Veileder
Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24bibliografisk kontrollert
Delarbeid
1. Light-indused multistep oxidation of dinuclear manganese complexes for artificial photosyntesis
Åpne denne publikasjonen i ny fane eller vindu >>Light-indused multistep oxidation of dinuclear manganese complexes for artificial photosyntesis
Vise andre…
2004 Inngår i: Journal of Inorganic Biochemistry, ISSN 0162-0134, Vol. 98, nr 5, s. 733-745Artikkel i tidsskrift (Fagfellevurdert) Published
Identifikatorer
urn:nbn:se:su:diva-23603 (URN)
Merknad
Part of urn:nbn:se:su:diva-396Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24bibliografisk kontrollert
2. Synthesis, Structure and Redox Chemistry of a Dinuclear Manganese Complex with a Novel Unsymmetric N5O2 Ligand
Åpne denne publikasjonen i ny fane eller vindu >>Synthesis, Structure and Redox Chemistry of a Dinuclear Manganese Complex with a Novel Unsymmetric N5O2 Ligand
Vise andre…
Manuskript (Annet vitenskapelig)
Identifikatorer
urn:nbn:se:su:diva-23604 (URN)
Merknad
Part of urn:nbn:se:su:diva-396Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24 Sist oppdatert: 2010-01-13bibliografisk kontrollert
3. Light Induced Magnanese Oxidation and Long-lived Charge Separation in a Mn2II,II-RuII-acceptor triad
Åpne denne publikasjonen i ny fane eller vindu >>Light Induced Magnanese Oxidation and Long-lived Charge Separation in a Mn2II,II-RuII-acceptor triad
Vise andre…
Manuskript (Annet vitenskapelig)
Identifikatorer
urn:nbn:se:su:diva-23605 (URN)
Merknad
Part of urn:nbn:se:su:diva-396Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24 Sist oppdatert: 2010-01-13bibliografisk kontrollert
4. Bridging-mode changes in response to manganese oxidation in two binuclear manganese complexes: implications for photosynthetic water-oxidation
Åpne denne publikasjonen i ny fane eller vindu >>Bridging-mode changes in response to manganese oxidation in two binuclear manganese complexes: implications for photosynthetic water-oxidation
Vise andre…
Artikkel i tidsskrift (Fagfellevurdert) Submitted
Identifikatorer
urn:nbn:se:su:diva-23606 (URN)
Merknad
Part of urn:nbn:se:su:diva-396Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24bibliografisk kontrollert
5. A New, Dinuclear High Spin Manganese(III) Complex with Bridging Phenoxy and Methoxy Groups. Structure and Magnetic Properties
Åpne denne publikasjonen i ny fane eller vindu >>A New, Dinuclear High Spin Manganese(III) Complex with Bridging Phenoxy and Methoxy Groups. Structure and Magnetic Properties
Vise andre…
2006 (engelsk)Inngår i: Inorganic Chemistry Communications, ISSN 1387-7003, E-ISSN 1879-0259, Vol. 9, nr 12, s. 1195-1198Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

A new μ-phenoxy-μ-metoxy di-manganese(III) complex with the trisphenolic ligand, 2,6-bis[((2-hydroxybenzyl)(2-pyridylmethyl)amino)methyl]-4-methylphenol, was isolated as a perchlorate salt. The X-ray structure shows that the two manganese(III) ions are in a distorted octrahedral enviroment with approximately perpendicular Jahn–Teller axes. Investigation of the molar magnetic susceptibility reveals a ferromagnetic coupling between the two high-spin manganese(III) ions. Fitting of the data led to g = 2 and J = 12.5 cm−1

Emneord
Manganese complex, X-ray structure, Magnetic properties
HSV kategori
Identifikatorer
urn:nbn:se:su:diva-23607 (URN)10.1016/j.inoche.2006.07.025 (DOI)
Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24 Sist oppdatert: 2017-12-13bibliografisk kontrollert
6. The Effect of Phenolates in the Mn(salen)-Catalyzed Epoxidation Reaction
Åpne denne publikasjonen i ny fane eller vindu >>The Effect of Phenolates in the Mn(salen)-Catalyzed Epoxidation Reaction
2005 (engelsk)Inngår i: Tetrahedron Letters, ISSN 0040-4039, E-ISSN 1359-8562, Vol. 46, nr 33, s. 5597-5600Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

By addition of 2,4,6-tri-tert-butylphenolate in the Mn(salen) catalyzed epoxidation of cis-alkenes with iodosobenzene, essentially pure trans-epoxides can be obtained.

sted, utgiver, år, opplag, sider
Elsevier Ltd, 2005
Emneord
Asymmetric catalysis; Manganese; Schiff bases; Oxygenations; Reaction mechanisms
HSV kategori
Identifikatorer
urn:nbn:se:su:diva-23608 (URN)10.1016/j.tetlet.2005.06.008 (DOI)
Merknad
Part of urn:nbn:se:su:diva-396Tilgjengelig fra: 2005-02-24 Laget: 2005-02-24 Sist oppdatert: 2017-12-13bibliografisk kontrollert

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