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Attachment of a hydrogen-bonding carboxylate side chain to an [FeFe]-hydrogenase model complex: Influence on the catalytic mechanism
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för fysikalisk kemi, oorganisk kemi och strukturkemi, Avdelningen för strukturkemi.
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för fysikalisk kemi, oorganisk kemi och strukturkemi, Avdelningen för strukturkemi.
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2010 (engelsk)Inngår i: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 16, nr 8, s. 2537-2546Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

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 46 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 FeFe 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.

sted, utgiver, år, opplag, sider
Weinheim: Wiley-VCH Verlag GmbH & Co. KGaA , 2010. Vol. 16, nr 8, s. 2537-2546
Emneord [en]
electrochemistry;electron transfer;enzyme model;iron-hydrogenase;proton reduction
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Identifikatorer
URN: urn:nbn:se:su:diva-43569DOI: 10.1002/chem.200902278ISI: 000275685800026OAI: oai:DiVA.org:su-43569DiVA, id: diva2:358031
Tilgjengelig fra: 2010-10-20 Laget: 2010-10-20 Sist oppdatert: 2017-12-12bibliografisk kontrollert

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