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Oxygen evolving reactions catalysed by synthetic manganese complexes: A systematic screening
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fotokemi och molekylärvetenskap, Molekylär biomimetik.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fotokemi och molekylärvetenskap, Molekylär biomimetik.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fotokemi och molekylärvetenskap, Molekylär biomimetik.
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fotokemi och molekylärvetenskap, Molekylär biomimetik.
2007 (engelsk)Inngår i: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, nr 38, s. 4258-4261Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

A set of six multinuclear manganese complexes was screened for the ability to catalyse reactions yielding O(2) under coherent experimental conditions; we identify a much larger number of manganese compounds than previously known that catalyse oxygen formation.

sted, utgiver, år, opplag, sider
2007. nr 38, s. 4258-4261
HSV kategori
Identifikatorer
URN: urn:nbn:se:uu:diva-11551DOI: 10.1039/b710761gISI: 000249705100004PubMedID: 17893814OAI: oai:DiVA.org:uu-11551DiVA, id: diva2:39320
Tilgjengelig fra: 2007-09-27 Laget: 2007-09-27 Sist oppdatert: 2017-12-11
Inngår i avhandling
1. Mimicking Nature – Synthesis and Characterisation of Manganese Complexes of Relevance to Artificial Photosynthesis
Åpne denne publikasjonen i ny fane eller vindu >>Mimicking Nature – Synthesis and Characterisation of Manganese Complexes of Relevance to Artificial Photosynthesis
2009 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

The development of efficient catalyst for water oxidation is of paramount importance to artificial photosynthesis, but before this can be achieved a deeper understanding of this reaction is essential. In nature this reaction occurs in a tetranuclear Mn-cluster which serves as the work-horse of oxygenic photosynthesis. This thesis summarises my efforts at developing molecular systems capable of mimicking this complex employing a biomimetic approach.

Three different approaches towards this goal are described here-in. The first section describes a screening study, in which a number of manganese complexes were tested to see whether or not they were capable of catalysing the formation of dioxygen when treated with different oxidants (Papers I). For those reactions in which dioxygen formation was observed the reactions were repeated in labelled water and the incorporation of labelled O-atoms was studied by mass spectrometry. This allowed us to determine to what extent water was the source of the evolved dioxygen (Papers II-III).

In Chapter three a reported catalyst and a derivative thereof is studied in depth. The influence of changes to the ligand on the oxygen–oxygen bond forming reaction could unfortunately not be reliably addressed, because of the instability of the complexes under “catalytic” conditions. Nevertheless, the study allowed us to revise the “carboxylate shift”-mechanism suggested in the literature (Papers IV-V).

Chapter four describes the continuation of my work on ligands featuring the carboxylate ligand motif first introduced in Chapter three. In this study ligands containing multiple binding pockets were designed and synthesised (Paper VI).

A better understanding of the mechanism in the natural water oxidising enzyme will facilitate the design of biomimetic complexes, this is discussed in Chapter five. In this work model complexes (Paper VII) are used to study the mechanism by which natures own water oxidising catalyst performs this reaction.

sted, utgiver, år, opplag, sider
Uppsala: Acta Universitatis Upsaliensis, 2009. s. 101
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 674
Emneord
Manganese, biomimetic, artificial photosynthesis, water splitting, homogeneous catalysis
HSV kategori
Forskningsprogram
fysikalisk kemi
Identifikatorer
urn:nbn:se:uu:diva-108526 (URN)978-91-554-7614-4 (ISBN)
Disputas
2009-11-06, Polhemsalen, Ångströmslaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:00 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2009-10-15 Laget: 2009-09-21 Sist oppdatert: 2018-01-13bibliografisk kontrollert

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