uu.seUppsala University Publications
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Accumulative charge separation inspired by photosynthesis
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science, Chemical Physics.
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.
Show others and affiliations
2010 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 132, no 51, 17977-17979 p.Article in journal (Refereed) 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.

Place, publisher, year, edition, pages
2010. Vol. 132, no 51, 17977-17979 p.
National Category
Chemical Sciences
Research subject
Chemistry with specialization in Chemical Physics
Identifiers
URN: urn:nbn:se:uu:diva-122184DOI: 10.1021/ja104809xISI: 000285818700001PubMedID: 21138258OAI: oai:DiVA.org:uu-122184DiVA: diva2:309340
Available from: 2010-04-07 Created: 2010-04-07 Last updated: 2011-03-01Bibliographically approved
In thesis
1. Single and Accumulative Electron Transfer – Prerequisites for Artificial Photosynthesis
Open this publication in new window or tab >>Single and Accumulative Electron Transfer – Prerequisites for Artificial Photosynthesis
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
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.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2010. 77 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 735
Keyword
Artificial photosynthesis, Photoinduced charge separation, Electron transfer, Energy transfer, Accumulative electon transfer, Donor-acceptor, Ruthenium, Linear arrays
National Category
Physical Chemistry
Research subject
Chemistry with specialization in Chemical Physics
Identifiers
urn:nbn:se:uu:diva-122206 (URN)978-91-554-7791-2 (ISBN)
Public defence
2010-05-21, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2010-04-28 Created: 2010-04-07 Last updated: 2011-03-01Bibliographically approved

Open Access in DiVA

No full text

Other links

Publisher's full textPubMed

Authority records BETA

Karlsson, Susanne

Search in DiVA

By author/editor
Karlsson, Susanne
By organisation
Chemical Physics
In the same journal
Journal of the American Chemical Society
Chemical Sciences

Search outside of DiVA

GoogleGoogle Scholar

doi
pubmed
urn-nbn

Altmetric score

doi
pubmed
urn-nbn
Total: 736 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf