Synthesis, characterization, and H/D exchange of μ-hydride-containing [FeFe]-hydrogenase subsite models formed by protonation reactions of (μ-TDT)Fe2(CO)4(PMe3)2 (TDT = SCH2SCH2S) with protic acids

Dalton Transactions : an International Journal of Inorganic Chemistry
Li-Cheng SongYuan-Qiang Guo

Abstract

As [FeFe]-hydrogenase models, the first thiodithiolate (TDT) ligand-containing μ-hydride complexes [(μ-TDT)Fe2(CO)4(PMe3)2(μ-H)](+)Y(-) (2-7, Y = Cl, ClO4, PF6, BF4, CF3CO2, CF3SO3) have been prepared by protonation reactions of (μ-TDT)Fe2(CO)4(PMe3)2 (1) with the corresponding HY acids. While the protonation reactions are monitored by in situ(1)H and (31)P{(1)H} NMR spectroscopy to show the isomer type and stability of 2-7, the structures of the isolated 2-7 are characterized by elemental analysis, spectroscopy and for some of them by X-ray crystallography. Although the H/D exchange of μ-hydride complex 7 (Y = CF3SO3) with D2 or D2O has been proved not to occur under the studied conditions, the H/D exchange of 7 with DCl gives the μ-deuterium complex [(μ-TDT)Fe2(CO)4(PMe3)2(μ-D)](+)[CF3SO3](-) (8) in a nearly quantitative yield. To our knowledge, 8 is the first crystallographically characterized μ-deuterium-containing butterfly [2Fe2S] complex produced by H/D exchange reaction.

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Citations

Feb 16, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Hassan Abul-FutouhWolfgang Weigand
Jul 5, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·J Patrick ShuppMichael J Rose
Oct 11, 2016·Chemistry : a European Journal·Hassan Abul-FutouhWolfgang Weigand
Oct 28, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Takehiko ShimamuraTsutomu Mizuta

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