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Reactions of [FeFe]-hydrogenase models involving the formation of hydrides related to proton reduction and hydrogen oxidation
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.ORCID iD: 0000-0002-4521-2870
2013 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 42, no 34, 12059-12071 p.Article in journal (Refereed) Published
Abstract [en]

[FeFe]-hydrogenases are enzymes in nature that catalyze the reduction of protons and the oxidation of H-2 at neutral pH with remarkably high activities and incredibly low overpotential. Structural and functional biomimicking of the active site of [FeFe]-hydrogenases can provide helpful hints for elucidating the mechanism of H-2 evolution and uptake at the [FeFe]-hydrogenase active site and for designing bio-inspired catalysts to replace the expensive noble metal catalysts for H-2 generation and uptake. This perspective focuses on the recent progress in the formation and reactivity of iron hydrides closely related to the processes of proton reduction and hydrogen oxidation mediated by diiron dithiolate complexes. The second section surveys the bridging and terminal hydride species formed from various diiron complexes as well as the intramolecular proton transfer. The very recent progress in H-2 activation by diiron dithiolate models are reviewed in the third section. In the concluding remarks and outlook, the differences in structure and catalytic mechanism between the synthetic models and the native [FeFe]-H(2)ase active site are compared and analyzed, which may cause the need for a significantly larger driving force and may lead to lower activities of synthetic models than the [FeFe]-H(2)ases for H-2 generation and uptake.

Place, publisher, year, edition, pages
2013. Vol. 42, no 34, 12059-12071 p.
Keyword [en]
Fe-Only Hydrogenases, Active-Site, Iron Hydrogenase, Desulfovibrio-Desulfuricans, Terminal Hydride, Electrochemical Properties, Organometallic Complex, Functional Models, Bridging Hydride, Synthetic Models
National Category
Chemical Sciences
URN: urn:nbn:se:kth:diva-127785DOI: 10.1039/c3dt51371hISI: 000322780000001ScopusID: 2-s2.0-84881454998OAI: diva2:645989
Knut and Alice Wallenberg Foundation

QC 20130906

Available from: 2013-09-06 Created: 2013-09-05 Last updated: 2013-09-06Bibliographically approved

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