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Ruthenium-manganese...
Ruthenium-manganese complexes for artificial photosynthesis : Factors controlling intramolecular electron transfer and excited-state quenching reactions
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- Abrahamsson, M. L. A. (författare)
- Uppsala universitet,Fysikalisk-kemiska institutionen
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- Berglund, Helena (författare)
- Uppsala universitet,Lund University,Lunds universitet,Biodiversitet,Biologiska institutionen,Naturvetenskapliga fakulteten,Biodiversity,Department of Biology,Faculty of Science,Fysikalisk-kemiska institutionen
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Tran, A. (författare)
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Philouze, C. (författare)
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Berg, K. E. (författare)
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- Raymond-Johansson, M. K. (författare)
- Uppsala universitet,Fysikalisk-kemiska institutionen
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Sun, Licheng C. (författare)
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Akermark, B. (författare)
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- Styring, Stenbjörn (författare)
- Lund University,Lunds universitet,Biokemi och Strukturbiologi,Centrum för Molekylär Proteinvetenskap,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Biochemistry and Structural Biology,Center for Molecular Protein Science,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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- Hammarström, Leif (författare)
- Uppsala universitet,Fysikalisk-kemiska institutionen
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(creator_code:org_t)
- 2002-02-22
- 2002
- Engelska.
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 41:6, s. 1534-1544
- Relaterad länk:
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http://dx.doi.org/10...
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https://urn.kb.se/re...
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https://doi.org/10.1...
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https://lup.lub.lu.s...
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https://urn.kb.se/re...
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Abstract
Ämnesord
Stäng
- Continuing our work toward a system mimicking the electron-transfer steps from manganese to P-680(+) in photosystem II (PS II), we report a series of ruthenium(II)-manganese(II) complexes that display intramolecular electron transfer from manganese(II) to photooxidized ruthenium(III). The electron-transfer rate constant (k(ET)) values span a large range, 1 X 10(5)-2 x 10(7) s(-1), and we have investigated different factors that are responsible for the variation. The reorganization energies determined experimentally (lambda = 1.5-2.0 eV) are larger than expected for solvent reorganization in complexes of similar size in polar solvents (typically lambda approximate to 1.0 eV). This result indicates that the inner reorganization energy is relatively large and, consequently, that at moderate driving force values manganese complexes are not fast donors. Both the type of manganese ligand and the link between the two metals are shown to be of great importance to the electron-transfer rate. In contrast, we show that the quenching of the excited state of the ruthenium(II) moiety by manganese(II) in this series of complexes mainly depends on the distance between the metals. However, by synthetically modifying the sensitizer so that the lowest metal-to-ligand charge transfer state was localized on the nonbridging ruthenium(II) ligands, we could reduce the quenching rate constant in one complex by a factor of 700 without changing the bridging ligand. Still, the manganese(II)-ruthenium (III) electrontransfer rate constant was not reduced. Consequently, the modification resulted in a complex with very favorable properties.
Ämnesord
- NATURVETENSKAP -- Biologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences (hsv//eng)
- NATURVETENSKAP -- Biologi -- Ekologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences -- Ecology (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Nyckelord
- oxygen-evolving complex
- ray-absorption spectroscopy
- photosystem-ii
- acceptor molecules
- water-oxidation
- s-0 state
- delocalization
- ligand
- model
- evolution
- Physical chemistry
Publikations- och innehållstyp
- ref (ämneskategori)
- art (ämneskategori)
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