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Redox chemistry of ...
Redox chemistry of a dimanganese(II,III) complex with an unsymmetric ligand : Water binding, deprotonation and accumulative light-induced oxidation
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- Anderlund, Magnus F. (author)
- Uppsala universitet,Institutionen för fotokemi och molekylärvetenskap
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- Högblom, Joakim (author)
- 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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- Shi, Wei (author)
- Uppsala universitet,Institutionen för fotokemi och molekylärvetenskap
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- Huang, Ping (author)
- Uppsala universitet,Institutionen för fotokemi och molekylärvetenskap
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Eriksson, Lars (author)
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Weihe, Högni (author)
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- Styring, Stenbjörn (author)
- Uppsala universitet,Institutionen för fotokemi och molekylärvetenskap
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Åkermark, Björn (author)
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- Lomoth, Reiner (author)
- Uppsala universitet,Institutionen för fotokemi och molekylärvetenskap
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- Magnuson, Ann (author)
- Uppsala universitet,Institutionen för fotokemi och molekylärvetenskap
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(creator_code:org_t)
- 2006-12-06
- 2006
- English.
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In: European Journal of Inorganic Chemistry. - : Wiley. - 1434-1948 .- 1099-1948 .- 1099-0682. ; :24, s. 5033-5047
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Abstract
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- A dinuclear manganese complex {[(Mn2L)-L-II,IIII(mu-OAc)(2)]-ClO4} has been synthesised, where L is the dianion of 2-{[bis-(pyrid-2-ylmethyl)amino]methyl}-6-{[(3,5-di-tert-butyl-2- hydroxybenzyl)(pyrid-2-ylmethyl)amino]methyl)-4-methylphenol, an unsymmetric binucleating ligand with two coordinating phenol groups. The two manganese ions, with a Mn-Mn distance of 3.498 angstrom, are bridged by the two bidentate acetate ligands and the 4-methylphenolate group of the ligand, resulting in a N3O3 and N2O4 donor set of Mn-II and Mn-II, respectively. Electrochemically [Mn2(II,III)L(mu-OAc)(2)](+) is reduced to [(Mn2L)-L-II,II(mu-OAc)(2)] at E-1/2(1)=-0.53 V versus Fc(+/0) and oxidised to [(Mn2L)-L-III,III(mu-OAC)(2)](2+) at E-1/2(2)=0.38 V versus Fc(+/0). All three redox states have been characterised by EPR, IR and UV/Vis spectroscopy. Subsequent oxidation of [(Mn2L)-L-II,III(mu-OAc)(2)](2+) [E-1/2(3)=0.75 V vs. Fc(+/0)] in dry acetonitrile results in an unstable primary product with a lifetime of about 100 ins. At high scan rates quasireversible voltammetric behaviour is found for all three electrode processes, with particularly slow electron transfer for the II,III/II,II [k(o)(1) = 0.002 cms(-1) and III,III/II,III [k(o)(2) = 0.005 cms(-1)] couples, which can be rationalised in terms of major distortions of the Mn-II centres. In aqueous media the bridging acetates are replaced by water-derived ligands. Deprotonation of these stabilises higher valence states, and photo-induced oxidation of the manganese complex results in a (Mn2L)-L-IlI,IV complex with oxo or hydroxo bridging ligands, which is further oxidised to an EPR-silent product. These results demonstrate that a larger number of metal-centred oxidations can be compressed in a narrow potential range if build up of charge is avoided by charge-compensating reactions.
Subject headings
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
- NATURVETENSKAP -- Biologi (hsv//swe)
- NATURAL SCIENCES -- Biological Sciences (hsv//eng)
Keyword
- manganese
- bioinorganic chemistry
- ligand exchange
- EPR spectroscopy
- IR spectroscopy
- Chemistry
- Kemi
- EPR spectroscopy
- ligand exchange
- manganese
- bioinorganic chemistry
- IR spectroscopy
Publication and Content Type
- ref (subject category)
- art (subject category)
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- By the author/editor
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Anderlund, Magnu ...
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Högblom, Joakim
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Shi, Wei
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Huang, Ping
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Eriksson, Lars
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Weihe, Högni
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show more...
-
Styring, Stenbjö ...
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Åkermark, Björn
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Lomoth, Reiner
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Magnuson, Ann
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show less...
- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Biological Scien ...
- Articles in the publication
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European Journal ...
- By the university
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Uppsala University
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Lund University