ArticleDalton transactions (Cambridge, England : 2003)2012
Nickel-iron dithiolates related to the deactivated [NiFe]-hydrogenases.
Article in Dalton transactions (Cambridge, England : 2003), 2012. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 1 paper.
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1 citing paper in PubMed.
- Synthesis and vibrational spectroscopy of (57)Fe-labeled models of [NiFe] hydrogenase: first direct observation of a nickel-iron interaction.Chemical communications (Cambridge, England) · 2014Article
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2 authors.
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Abstract
Described herein are preparations of synthetic models for the deactivated Ni(II)Fe(II) states of the [NiFe]-hydrogenases. Iodination of the S = ½ species [(dppe)Ni(pdt)Fe(CO)(3)](+) afforded the diamagnetic iodo complex [(dppe)Ni(pdt)IFe(CO)(3)](+). Crystallographic analysis of this species confirmed the presence of square-pyramidal Ni linked to an octahedral Fe centre. The NiFe separation of 3.018 Å indicated the absence of metal-metal bonding. This complex could be reduced to give (dppe)Ni(pdt)Fe(CO)(3) and, in the presence of iodide, decarbonylated to afford (dppe)Ni(pdt)FeI(2). Derivatives of the type [(diphosphine)Ni(dithiolate)XFe(CO)(2)L](+) (X = Cl, Br, I) were prepared by halogenation of mixed-valence precursors [(diphosphine)Ni(dithiolate)Fe(CO)(2)L](+) (diphosphine = dppe, dcpe; L = tertiary phosphine or CO). The Fe(CO)(2)(PR(3))-containing derivatives are more robust than the related tricarbonyl derivatives. Exploiting this greater stability, we characterised examples of chloride and bromide derivatives. Related fluorides could be prepared by F(-) abstraction from BF(4)(-). Spectroscopic evidence is presented for the hydroperoxide [(dppe)Ni(pdt)(OOH)Fe(CO)(2)L](+), which represents a model for the Ni-SU state.
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