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Accumulative charge separation inspired by photosynthesis
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för fotokemi och molekylärvetenskap, Kemisk fysik.
Chimie et Interdisciplinarité, Synthèse, Analyse, Modélisation, Université de Nantes.
Chimie et Interdisciplinarité, Synthèse, Analyse, Modélisation, Université de Nantes.
Chimie et Interdisciplinarité, Synthèse, Analyse, Modélisation, Université de Nantes.
Vise andre og tillknytning
2010 (engelsk)Inngår i: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 132, nr 51, s. 17977-17979Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

Molecular systems that follow the functional principles of photosynthesis have attracted increasing attention as a method for the direct production of solar fuels. This could give a major carbon-neutral energy contribution to our future society. An outstanding challenge in this research is to couple the light-induced charge separation (which generates a single electron-hole pair) to the multielectron processes of water oxidation and fuel generation. New design considerations are needed to allow for several cycles of photon absorption and charge separation of a single artificial photosystem. Here we demonstrate a molecular system with a regenerative photosensitizer that shows two successive events of light-induced charge separation, leading to high-yield accumulation of redox equivalents on single components without sacrificial agents.

sted, utgiver, år, opplag, sider
2010. Vol. 132, nr 51, s. 17977-17979
HSV kategori
Forskningsprogram
Kemi med inriktning mot kemisk fysik
Identifikatorer
URN: urn:nbn:se:uu:diva-122184DOI: 10.1021/ja104809xISI: 000285818700001PubMedID: 21138258OAI: oai:DiVA.org:uu-122184DiVA, id: diva2:309340
Tilgjengelig fra: 2010-04-07 Laget: 2010-04-07 Sist oppdatert: 2017-12-12bibliografisk kontrollert
Inngår i avhandling
1. Single and Accumulative Electron Transfer – Prerequisites for Artificial Photosynthesis
Åpne denne publikasjonen i ny fane eller vindu >>Single and Accumulative Electron Transfer – Prerequisites for Artificial Photosynthesis
2010 (engelsk)Doktoravhandling, med artikler (Annet vitenskapelig)
Abstract [en]

Photoinduced electron transfer is involved in a number of photochemical and photobiological processes. One example of this is photosynthesis, where the absorption of sunlight leads to the formation of charge-separated states by electron transfer. The redox equivalents built up by successive photoabsorption and electron transfer is further used for the oxidation of water and reduction of carbon dioxide to sugars. The work presented in this thesis is part of an interdisciplinary effort aiming at a functional mimic of photosynthesis. The goal of this project is to utilize sunlight to produce renewable fuels from sun and water. Specifically, this thesis concerns photoinduced electron transfer in donor(D)-photosensitizer(P)-acceptor(A) systems, in mimic of the primary events of photosynthesis.

The absorption of a photon typically leads to transfer of a single electron, i.e., charge separation to produce a single electron-hole pair. This fundamental process was studied in several molecular systems. The purpose of these studies was optimization of single electron transfer as to obtain charge separation in high yields, with minimum losses to competing photoreactions such as energy transfer. Also, the lifetime of the charge separated state and the confinement of the electron and hole in three-dimensional space are important in practical applications. This led us to explore molecular motifs for linear arrays based on Ru(II)bis-tridentate and Ru(II)tris-bidentate complexes.

The target multi-electron catalytic reactions of water-splitting and fuel production require a build-up of redox equivalents upon successive photoexcitation and electron transfer events. The possibilities and challenges associated with such processes in molecular systems were investigated. One of the studied systems was shown to accumulate two electrons and two holes upon two successive excitations, without sacrificial redox agents and with minimum yield losses. From these studies, we have gained better understanding of the obstacles associated with step-wise photoaccumulation of charge and how to overcome them.

sted, utgiver, år, opplag, sider
Uppsala: Acta Universitatis Upsaliensis, 2010. s. 77
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 735
Emneord
Artificial photosynthesis, Photoinduced charge separation, Electron transfer, Energy transfer, Accumulative electon transfer, Donor-acceptor, Ruthenium, Linear arrays
HSV kategori
Forskningsprogram
Kemi med inriktning mot kemisk fysik
Identifikatorer
urn:nbn:se:uu:diva-122206 (URN)978-91-554-7791-2 (ISBN)
Disputas
2010-05-21, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:15 (engelsk)
Opponent
Veileder
Tilgjengelig fra: 2010-04-28 Laget: 2010-04-07 Sist oppdatert: 2011-03-01bibliografisk kontrollert

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