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Synthesis, structures and electrochemical properties of nitro- and amino-functionalized diiron azadithiolates as active site models of Fe-only hydrogenases
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2004 (English)In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 10, no 18, 4474-4479 p.Article in journal (Refereed) Published
Abstract [en]

Complex [{(mu-SCH2)(2)N(4-NO2C6H4)}Fe-2(CO)(6)] (4) was prepared by the reaction of the dianionic intermediate [(mu-S)(2)Fe-2(CO)(6)](2-) and N,N-bis(chloromethyl)-4-nitroaniline as a biomimetic model of the active site of Fe-only hydrogenase. The reduction of 4 by Pd-C/H-2 under a neutral condition afforded complex [{(mu-SCH2)(2)N(4-NH2C6H4)}Fe-2(CO)(6)] (5) in 67% yield. Both complexes were characterized by IR, H-1 and C-13 NMR spectroscopy and MS spectrometry. The molecular structure of 4, as determined by X-ray analysis, has a butterfly 2Fe2S core and the aryl group on the bridged-N atom slants to the Fe(2) site. Cyclic voltammograms of 4 and 5 were studied to evaluate their redox properties. It was found that complex 4 catalyzed electrochemical proton reduction in the presence of acetic acid. A plausible mechanism of the electrocatalytic proton reduction is discussed.

Place, publisher, year, edition, pages
2004. Vol. 10, no 18, 4474-4479 p.
Keyword [en]
bioinorganic chemistry, cluster compounds, diiron azaditholate, iron only hydrogenase, redox chemistry, iron hydrogenase, desulfovibrio-desulfuricans, complexes, chemistry, dinuclear, exchange, coordination, photosensitizer, evolution, ligands
URN: urn:nbn:se:kth:diva-23767ISI: 000224146800010OAI: diva2:342466
QC 20100525Available from: 2010-08-10 Created: 2010-08-10Bibliographically approved

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