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Dinuclear Manganese Complexes for Artificial Photosynthesis: Synthesis and Properties
Stockholm University, Faculty of Science, Department of Organic Chemistry.
2005 (English)Doctoral thesis, comprehensive summary (Other academic)
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.

Place, publisher, year, edition, pages
Stockholm: Institutionen för organisk kemi , 2005. , 49 p.
Keyword [en]
Crystal Structure, Artificial photosynthesis, Manganese complex
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-396ISBN: 91-7155-018-6 (print)OAI: oai:DiVA.org:su-396DiVA: diva2:193361
Public defence
2005-03-18, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 12 A, Stockholm, 10:00
Opponent
Supervisors
Available from: 2005-02-24 Created: 2005-02-24Bibliographically approved
List of papers
1. Light-indused multistep oxidation of dinuclear manganese complexes for artificial photosyntesis
Open this publication in new window or tab >>Light-indused multistep oxidation of dinuclear manganese complexes for artificial photosyntesis
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2004 In: Journal of Inorganic Biochemistry, ISSN 0162-0134, Vol. 98, no 5, 733-745 p.Article in journal (Refereed) Published
Identifiers
urn:nbn:se:su:diva-23603 (URN)
Note
Part of urn:nbn:se:su:diva-396Available from: 2005-02-24 Created: 2005-02-24Bibliographically approved
2. Synthesis, Structure and Redox Chemistry of a Dinuclear Manganese Complex with a Novel Unsymmetric N5O2 Ligand
Open this publication in new window or tab >>Synthesis, Structure and Redox Chemistry of a Dinuclear Manganese Complex with a Novel Unsymmetric N5O2 Ligand
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Manuscript (Other academic)
Identifiers
urn:nbn:se:su:diva-23604 (URN)
Note
Part of urn:nbn:se:su:diva-396Available from: 2005-02-24 Created: 2005-02-24 Last updated: 2010-01-13Bibliographically approved
3. Light Induced Magnanese Oxidation and Long-lived Charge Separation in a Mn2II,II-RuII-acceptor triad
Open this publication in new window or tab >>Light Induced Magnanese Oxidation and Long-lived Charge Separation in a Mn2II,II-RuII-acceptor triad
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Manuscript (Other academic)
Identifiers
urn:nbn:se:su:diva-23605 (URN)
Note
Part of urn:nbn:se:su:diva-396Available from: 2005-02-24 Created: 2005-02-24 Last updated: 2010-01-13Bibliographically approved
4. Bridging-mode changes in response to manganese oxidation in two binuclear manganese complexes: implications for photosynthetic water-oxidation
Open this publication in new window or tab >>Bridging-mode changes in response to manganese oxidation in two binuclear manganese complexes: implications for photosynthetic water-oxidation
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Article in journal (Refereed) Submitted
Identifiers
urn:nbn:se:su:diva-23606 (URN)
Note
Part of urn:nbn:se:su:diva-396Available from: 2005-02-24 Created: 2005-02-24Bibliographically approved
5. A New, Dinuclear High Spin Manganese(III) Complex with Bridging Phenoxy and Methoxy Groups. Structure and Magnetic Properties
Open this publication in new window or tab >>A New, Dinuclear High Spin Manganese(III) Complex with Bridging Phenoxy and Methoxy Groups. Structure and Magnetic Properties
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2006 (English)In: Inorganic Chemistry Communications, ISSN 1387-7003, E-ISSN 1879-0259, Vol. 9, no 12, 1195-1198 p.Article in journal (Refereed) 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

Keyword
Manganese complex, X-ray structure, Magnetic properties
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-23607 (URN)10.1016/j.inoche.2006.07.025 (DOI)
Available from: 2005-02-24 Created: 2005-02-24 Last updated: 2017-12-13Bibliographically approved
6. The Effect of Phenolates in the Mn(salen)-Catalyzed Epoxidation Reaction
Open this publication in new window or tab >>The Effect of Phenolates in the Mn(salen)-Catalyzed Epoxidation Reaction
2005 (English)In: Tetrahedron Letters, ISSN 0040-4039, E-ISSN 1359-8562, Vol. 46, no 33, 5597-5600 p.Article in journal (Refereed) 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.

Place, publisher, year, edition, pages
Elsevier Ltd, 2005
Keyword
Asymmetric catalysis; Manganese; Schiff bases; Oxygenations; Reaction mechanisms
National Category
Organic Chemistry
Identifiers
urn:nbn:se:su:diva-23608 (URN)10.1016/j.tetlet.2005.06.008 (DOI)
Note
Part of urn:nbn:se:su:diva-396Available from: 2005-02-24 Created: 2005-02-24 Last updated: 2017-12-13Bibliographically approved

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