NDLI: Attachment of a Hydrogen-Bonding Carboxylate Side Chain to an [FeFe]-Hydrogenase Model Complex: Influence on the Catalytic Mechanism

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Attachment of a Hydrogen-Bonding Carboxylate Side Chain to an [FeFe]-Hydrogenase Model Complex: Influence on the Catalytic Mechanism

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Eriksson, Lars Sun, Licheng Akermark, Björn Gao, Weiming Sun, Junliang Akermark, Torbjörn Li, Mingrun
Description	Author Affiliation: Gao W ( Department of Organic Chemistry, Arrhenius Laboratory, Stockholm University, 10691 Stockholm, Sweden.)
Abstract	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 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 $CH_{3}CN/D_{2}O$ solution by on-line mass spectrometry.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	8
Volume Number	16
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2010-02-22
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Carboxylic Acids Chemistry Hydrogenase Iron-Sulfur Proteins Organometallic Compounds Binding Sites Catalysis Crystallography, X-Ray Electrochemistry Hydrogen Bonding Metabolism Magnetic Resonance Spectroscopy Models, Molecular Molecular Structure Spectrophotometry, Infrared Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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