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Süss-Fink, Georg

Nom
Süss-Fink, Georg
Affiliation principale
Fonction
Professeur ordinaire
Email
georg.suess-fink@unine.ch
Identifiants
https://libra.unine.ch/handle/123456789/385

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  • Publication
    Accès libre
    Supramolecular cluster catalysis : facts and problems
    (2004)
    Süss-Fink, Georg 
    ;
    Therrien, Bruno 
    ;
    Vieille-Petit, Ludovic
    ;
    Tschan, Mathieu J.-L.
    ;
    Romakh, Vladimir B.
    ;
    Ward, Thomas R.
    ;
    Dadras, Massoud
    ;
    Laurenczy, Gabor
    By checking the chemistry underlying the concept of "supramolecular cluster catalysis" we identified two major errors in our publications related to this topic, which are essentially due to contamination problems. (1) The conversion of the "closed" cluster cation [H3Ru3(C6H6)(C6Me6)2(O)]+ (1) into the "open" cluster cation [H2Ru3(C6H6)(C6Me6)2 (O)(OH)]+ (2), which we had ascribed to a reaction with water in the presence of ethylbenzene is simply an oxidation reaction which occurs in the presence of air. (2) The higher catalytic activity observed with ethylbenzene, which we had erroneously attributed to the "open" cluster cation [H2Ru3(C6H6)(C6Me6)2(O)(OH)]+ (2), was due to the formation of RuO2• nH2O, caused by a hydroperoxide contamination present in ethylbenzene.
  • Publication
    Accès libre
    Isolation and single-crystal X-ray structure analysis of the catalyst–substrate host–guest complexes [C6H6⊂H3Ru3{C6H5(CH2) nOH}(C6Me6)2(O)]+ (n = 2, 3)
    (2003-11-01)
    Vieille-Petit, Ludovic
    ;
    Therrien, Bruno 
    ;
    Süss-Fink, Georg 
    ;
    Ward, Thomas R.
    The trinuclear arene-ruthenium cluster cations [H3Ru3{C6H5 (CH2)nOH}(C6Me6)2 (O)]+ (3: n=2, 4: n=3) have been synthesised from the dinuclear precursor [H3Ru2 (C6Me6)2]+ and the mononuclear complexes [{C6H5(CH2)nOH}Ru(H2O)3]2+ in aqueous solution, isolated and characterised as the hexafluorophosphate or tetrafluoroborate salts. Both 3 and 4 are derivatives of the parent cluster cation [H3Ru3 (C6H6)(C6Me6)2(O)]+ (1) which was found to catalyse the hydrogenation of benzene to give cyclohexane under biphasic conditions. The mechanism postulated for this catalytic reaction (‘supramolecular cluster catalysis’), involving the hydrophobic pocket spanned by the three arene ligands in 1, was based on the assumption that the substrate molecule benzene is hosted inside the hydrophobic pocket of the cluster molecule to form a catalyst–substrate host–guest complex in which the hydrogenation of the substrate takes place. With the analogous cluster cations 3 and 4, containing a (CH2)nOH side-arm (n=2, 3) as substituent at the benzene ligand, it was possible to isolate the cationic host–guest complexes as the hexafluorophosphate or tetrafluoroborate salts. The single-crystal X-ray structure analyses of [C6H6⊂3][PF6] and [C6H6⊂4][BF4], compared to that of [3][PF6] show that the substrate molecule benzene is indeed held inside the hydrophobic pocket of 3 and 4, the angle between the metal (Ru3) plane and the aromatic plane being 67° and 89°, respectively.
  • Publication
    Accès libre
    Mechanistic in situ High-Pressure NMR Studies of Benzene Hydrogenation by Supramolecular Cluster Catalysis with [(η6-C6H6)(η6-C6Me6)2Ru3(μ3-O)(μ2-OH)(μ2-H)2][BF4]
    (2002)
    Laurenczy, Gabor
    ;
    Faure, Matthieu
    ;
    Vieille-Petit, Ludovic
    ;
    Süss-Fink, Georg 
    ;
    Ward, Thomas R.
    In situ high-pressure NMR spectroscopy of the hydrogenation of benzene to give cyclohexane, catalysed by the cluster cation [(η6-C6H6)(η6-C6Me6)2Ru3(μ3-O)(μ2-OH)(μ2-H)2]+2, supports a mechanism involving a supramolecular host-guest complex of the substrate molecule in the hydrophobic pocket of the intact cluster molecule.