NDLI: Oxo-molybdenum and oxo-tungsten complexes of Schiff bases relevant to molybdoenzymes

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Oxo-molybdenum and oxo-tungsten complexes of Schiff bases relevant to molybdoenzymes

Content Provider	Royal Society of Chemistry (RSC)
Author	Lyashenko, Ganna Mösch-Zanetti, Nadia C. Baumgartner, Judith Saischek, Gerald Judmaier, Martina E. Belaj, Ferdinand Volpe, Manuel Jancik, Vojtech Herbst-Irmer, Regine
Copyright Year	2009
Abstract	A series of octahedral dioxomolybdenum(VI) complexes of the type [MoO2L2] {L = 4-Ar-pent-2-en-ol; Li−Pr2Ph with Ar = 2,6-diisopropylphenyl (1); LMe2Ph with Ar = 2,6-dimethylphenyl (2), LMePh with Ar = 2-methylphenyl (3) and with Ar = phenyl (4)} and dioxotungsten(VI) compounds [WO2L2] {Li-Pr2Ph (5); LMe2Ph (6) and LMePh (7)} with Schiff bases have been synthesized as models for oxotransferases. Spectroscopic characterization in solution shows with the sterically encumbered ligands Li-Pr2Ph and LMe2Ph isomerically pure products whereas the ligand with only one substituent in ortho position at the aromatic ring LMePh revealed a dynamic mixture of three isomers as confirmed by variable temperature NMR spectroscopy. Single crystal X-ray diffraction analyses of compounds 1, 2 and 4 showed them to be in the N,N-trans conformation consistent with the larger steric demand at nitrogen. Oxygen atom transfer (OAT) properties towards trimethylphosphine were investigated leading to the isolation of two mononuclear molybdenum(IV) compounds [MoO(PMe3)(LMe2Ph)2] (8) and [MoO(PMe3)(LMePh)2] (9) as confirmed by spectroscopic and crystallographic means. The kinetics of OAT between complex [MoO2(LMe2Ph)2] (2) and PMe3 was investigated by UV/Vis spectroscopy under pseudo-first-order conditions revealing single-step reactions with Eyring values of ΔH≠ = +60.79 kJ mol−1 and ΔS≠ = −112 J mol−1K−1 and a first-order dependence of phosphine consistent with a slow nucleophilic attack of the phosphine showing the octahedral geometries of this system to be unfavorable for OAT. Compound 1 showed no OAT reactivity towards PMe3 emphasizing the influence of sterical properties. Furthermore, the reactivity of the reduced compounds [MoO(PMe3)(LMe2Ph)2] (8) and [MoO(PMe3)(LMePh)2] (9) towards molecular oxygen was investigated leading, in the case of 8, to the substitution of PMe3 by O2 under formation of the peroxo compound [MoO(O2)(LMe2Ph)2] (10). In contrast, the analogous reaction employing 9 led to oxidation forming the dioxo compound [MoO2(LMePh)2] (3).
Starting Page	5655
Ending Page	5665
Page Count	11
File Format	HTM / HTML PDF
ISSN	14779226
Volume Number	0
Issue Number	29
Journal	Dalton Transactions
DOI	10.1039/b820629e
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Schiff Eyring Phenyl group Ligand Substituent Nuclear magnetic resonance spectroscopy Single crystal X-ray crystallography Chemical structure Nitrogen Trimethylphosphine Molybdenum FB Vis Spectroscopy Correlation and dependence Phosphine Nucleophile Oxygen
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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