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• W1966451155 endingPage "4249" @default.
• W1966451155 startingPage "4243" @default.
• W1966451155 abstract "This study describes the characterization of a mixed-valence RuII/NiI complex, a structural model for the Ni–L state of the [NiFe]hydrogenases. One-electron oxidation of (cymene)Ru(μ-pdt)Ni(diphos) ([1]0, diphos = dppe, C2H4(PPh2)2; [2]0, diphos = dcpe, C2H4(P(C6H11)2)2] affords the mixed-valence cations [(cymene)Ru(pdt)Ni(diphos)]+ ([1]+ and [2]+). Crystallographic and spectroscopic measurements indicate that these cations are described as RuII/NiI. Although [1]0 and [1]+ are very similar structurally, the following changes are notable: the Ni–P distances elongate upon oxidation, and the Ru–Ni distance changes insignificantly. The molecular and electronic structures of the Ni center in [1]+ approaches that observed in the [NiFe]hydrogenases. Density functional theory calculations indicate that [1]0 is best described as RuII/Ni0, consistent with its oxidation to RuII/NiI in [1]+. The fast electron self-exchange rate of 107 M–1 s–1 between [1]0 and [1]+ suggests minor reorganization, more consistent with a Ni0/NiI oxidation state change than a NiI/NiII couple. In solution, [1]+ slowly converts to [H1]+ and [1-H]+, with the latter being a complex of the thioaldehyde SCHCH2CH2S arising from C–H activation of the pdt backbone. Treatment of [1]+ with the H-atom abstracting reagent 2,2,6,6-tetramethylpiperidine-1-oxy also gives [1-H]+." @default.
• W1966451155 created "2016-06-24" @default.
• W1966451155 creator A5005070123 @default.
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• W1966451155 date "2014-03-31" @default.
• W1966451155 modified "2023-09-26" @default.
• W1966451155 title "Ni^I/Ru^II Model for the Ni–L State of the [NiFe]Hydrogenases: Synthesis, Spectroscopy, and Reactivity" @default.
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• W1966451155 doi "https://doi.org/10.1021/ic500389p" @default.
• W1966451155 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/24684697" @default.
• W1966451155 hasPublicationYear "2014" @default.
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