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Attachment of a Hydrogen-Bonding Carboxylate Side Chain to an FeFe -Hydrogenase Model Complex: Influence on the Catalytic Mechanism
KTH, Skolan för kemivetenskap (CHE), Kemiteknik, Tillämpad elektrokemi.
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2010 (Engelska)Ingår i: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 16, nr 8, s. 2537-2546Artikel i tidskrift (Refereegranskat) 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 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.

Ort, förlag, år, upplaga, sidor
2010. Vol. 16, nr 8, s. 2537-2546
Nyckelord [en]
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
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Kemi
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URN: urn:nbn:se:kth:diva-19317DOI: 10.1002/chem.200902278ISI: 000275685800026Scopus ID: 2-s2.0-77049106133OAI: oai:DiVA.org:kth-19317DiVA, id: diva2:337364
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VetenskapsrådetKnut och Alice Wallenbergs Stiftelse
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QC 20110114Tillgänglig från: 2010-08-05 Skapad: 2010-08-05 Senast uppdaterad: 2017-12-12Bibliografiskt granskad

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