Chalcogenide-capped triiron clusters [Fe3(CO)9(μ3-E)2], [Fe3(CO)7(μ3-CO)(μ3-E)(μ-dppm)] and [Fe3(CO)7(μ3-E)2(μ-dppm)] (E = S, Se) as proton-reduction catalysts
Chalcogenide-capped triiron clusters [Fe3(CO)7(μ3-CO)(μ3-E)(μ-dppm)] and [Fe3(CO)7(μ3-E)2(μ-dppm)] (E = S, Se) have been examined as proton-reduction catalysts. Protonation studies show that [Fe3(CO)9(μ3-E)2] are unaffected by strong acids. Mono-capped [Fe3(CO)7(μ3-CO)(μ3-E)(μ-dppm)] react with HBF4.Et2O but changes in IR spectra are attributed to BF3 binding to the face-capping carbonyl, while bicapped [Fe3(CO)7(μ3-E)2(μ-dppm)] are protonated but in a process that is not catalytically important. DFT calculations are presented to support these protonation studies. Cyclic voltammetry shows that [Fe3(CO)9(μ3-Se)2] exhibits two reduction waves, and upon addition of strong acids, proton-reducti…
Asymmetric hydrogenation of an α-unsaturated carboxylic acid catalyzed by intact chiral transition metal carbonyl clusters – diastereomeric control of enantioselectivity
Twenty clusters of the general formula [(μ-H)2Ru3(μ3-S)(CO)7(μ-P–P*)] (P–P* = chiral diphosphine of the ferrocene-based Walphos or Josiphos families) have been synthesised and characterised. The clusters have been tested as catalysts for asymmetric hydrogenation of tiglic acid [trans-2-methyl-2-butenoic acid]. The observed enantioselectivities and conversion rates strongly support catalysis by intact Ru3 clusters. A catalytic mechanism involving an active Ru3 catalyst generated by CO loss from [(μ-H)2Ru3(μ3-S)(CO)7(μ-P–P*)] has been investigated by DFT calculations. peerReviewed
Synthesis and characterization of chiral phosphirane derivatives of [(μ-H)4Ru4(CO)12] and their application in the hydrogenation of an α,β-unsaturated carboxylic acid
Abstract Ruthenium clusters containing the chiral binaphthyl-derived mono-phosphiranes [(S)-([1,1′-binaphthalen]-2-yl)phosphirane] (S)-1a, [(R)-(2′-methoxy-1,1′-binaphthyl-2-yl)phosphirane] (R)-1b, and the diphosphirane [2,2′-di(phosphiran-1-yl)-1,1′-binaphthalene] (S)-1c have been synthesized and characterized. The clusters are [(μ-H)4Ru4(CO)11((S)-1a)] (S)-2, [(μ-H)4Ru4(CO)11((R)-1b)] (R)-3, 1,1-[(μ-H)4Ru4(CO)10((S)-1c)] (S)-4, [(μ-H)4Ru4(CO)11((S)-binaphthyl-P(s)(H)Et)] (S,Sp)-5, [(μ-H)4Ru4(CO)11((S)-binaphthyl-P(R)(H)Et)] (S,Rp)-6, [(μ-H)4Ru4(CO)11((R)-binaphthyl-P(s)(H)Et)] (R,Sp)-7, [(μ-H)4Ru4(CO)11((R)-binaphthyl-P(R)(H)Et)] (R,Rp)-8 and the phosphinidene-capped triruthenium cluster …
Diastereomeric control of enantioselectivity: evidence for metal cluster catalysis
Enantioselective hydrogenation of tiglic acid effected by diastereomers of the general formula [(μ-H)2Ru3(μ3-S)(CO)7(μ-P–P*)] (P–P* = chiral Walphos diphosphine ligand) strongly supports catalysis by intact Ru3 clusters. A catalytic mechanism involving Ru3 clusters has been established by DFT calculations. peerReviewed
Water oxidation catalyzed by molecular di- and nonanuclear Fe complexes: importance of a proper ligand framework.
The synthesis of two molecular iron complexes, a dinuclear iron(III,III) complex and a nonanuclear iron complex, based on the di-nucleating ligand 2,2-(2-hydroxy-5-methyl-1,3-phenylene)bis(1H-benzo[d]imidazole-4-carboxylic acid) is described. The two iron complexes were found to drive the oxidation of water by the one-electron oxidant [Ru(bpy)(3)](3+). Funding Agencies|Knut and Alice Wallenberg Foundation; Swedish Research Council [621-2013-4872]; Carl Trygger Foundation; DFG (Metal Sites in Biomolecules: Structures, Regulation and Mechanisms) [IRTG 1422]; Swedish Energy Agency
CCDC 1043618: Experimental Crystal Structure Determination
Related Article: Ahmed F. Abdel-Magied, Yusuf Theibich, Amrendra K. Singh, Ahibur Rahaman, Isa Doverbratt, Arun K. Raha, Matti Haukka, Michael G. Richmond, Ebbe Nordlander|2020|Dalton Trans.|49|4244|doi:10.1039/C9DT04799A
CCDC 1962572: Experimental Crystal Structure Determination
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CCDC 1962571: Experimental Crystal Structure Determination
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CCDC 1531251: Experimental Crystal Structure Determination
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CCDC 1962575: Experimental Crystal Structure Determination
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CCDC 993899: Experimental Crystal Structure Determination
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CCDC 1981159: Experimental Crystal Structure Determination
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CCDC 1962574: Experimental Crystal Structure Determination
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CCDC 966406: Experimental Crystal Structure Determination
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CCDC 1043620: Experimental Crystal Structure Determination
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CCDC 1043617: Experimental Crystal Structure Determination
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CCDC 993900: Experimental Crystal Structure Determination
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CCDC 1473054: Experimental Crystal Structure Determination
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CCDC 1531250: Experimental Crystal Structure Determination
Related Article: Ahmed F. Abdel-Magied, Maitham H. Majeed, Manuel F. Abelairas-Edesa, Arne Ficks, Radwa M. Ashour, Ahibur Rahaman, William Clegg, Matti Haukka, Lee J. Higham, Ebbe Nordlander|2017|J.Organomet.Chem.|849-850|71|doi:10.1016/j.jorganchem.2017.05.031
CCDC 1962573: Experimental Crystal Structure Determination
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CCDC 1473051: Experimental Crystal Structure Determination
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CCDC 1531252: Experimental Crystal Structure Determination
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CCDC 1043616: Experimental Crystal Structure Determination
Related Article: Ahmed F. Abdel-Magied, Yusuf Theibich, Amrendra K. Singh, Ahibur Rahaman, Isa Doverbratt, Arun K. Raha, Matti Haukka, Michael G. Richmond, Ebbe Nordlander|2020|Dalton Trans.|49|4244|doi:10.1039/C9DT04799A
CCDC 1981173: Experimental Crystal Structure Determination
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CCDC 1043619: Experimental Crystal Structure Determination
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