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Attachment of a Hydrogen-Bonding Carboxylate Side Chain to an FeFe -Hydrogenase Model Complex : Influence on the Catalytic Mechanism
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- Gao, Weiming (author)
- Stockholms universitet,Institutionen för organisk kemi
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- Sun, Junliang (author)
- Stockholms universitet,Avdelningen för strukturkemi
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- Åkermark, Torbjörn (author)
- KTH,Tillämpad elektrokemi
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- (creator_code:org_t)
- Weinheim : Wiley, 2010
- 2010
- English.
- In: Chemistry - A European Journal. - Weinheim : Wiley. - 0947-6539 .- 1521-3765. ; 16:8, s. 2537-2546
- Journal article (peer-reviewed)
Abstract
Subject headings
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- Azapropanedithiolate (adt)-bridged model complexes of [FeFe]-hydrogenase bearing a carboxylic acid functionality have been designed with the aim of decreasing the potential for reduction of protons to hydrogen. Protonation of the bisphosphine complexes 4-6 has been studied by in situ IR and NMR spectroscopy, which revealed that protonation with triflic acid most likely takes place first at the N-bridge for complex 4 but at the Fe Fe bond for complexes 5 and 6. Using an excess of acid, the diprotonated species could also be observed, but none of the protonated species was sufficiently stable to be isolated in a pure state. Electrochemical studies have provided an insight into the catalytic mechanisms under strongly acidic conditions, and have also shown that complexes 3 and 6 are electro-active in aqueous solution even in the absence of acid, presumably due to hydrogen bonding. Hydrogen evolution, driven by visible light, has been observed for three-component systems consisting of [Ru(bpy)(3)](2+), complex 1, 2, or 3, and ascorbic acid in CH3CN/D2O solution by on-line mass spectrometry.
Subject headings
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
Keyword
- electrochemistry
- electron transfer
- enzyme model
- iron-hydrogenase
- proton reduction
- active-site models
- fe-only hydrogenase
- coupled electron-transfer
- iron hydrogenase
- electrochemical properties
- structure/function
- relationships
- proton reduction
- generation
- activation
- ligands
- Chemistry
- Kemi
- Organic chemistry
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- ref (subject category)
- art (subject category)
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