Mononuclear and polynuclear copper(I) complexes with a new N,N',S-donor ligand and with structural analogies to the copper thionein core.
2007
The N,N‘,S-donor ligand 4-methoxy-3,5-dimethyl-2-((3-(2-(methylthio)phenyl)-1H-pyrazol-1-yl)methyl)pyridine (L) was prepared from 2-(chloromethyl)-4-methoxy-3,5-dimethylpyridine hydrochloride and 3-(2-(methylthio)phenyl)-1H-pyrazole. The Cu(I) complexes [Cu2(L)2CH3CN][Cu(L)CH3CN](BF4)3 (1), [Cu(L)PPh3]BF4 (2), and [Cu6(L)2(C6F5S)6] (3) were prepared and characterized by X-ray crystallography (PPh3 = triphenylphosphine, C6F5S- = pentafluorothiophenolate). The unit cell of compound 1 consists of cocrystallized mononuclear and dinuclear entities in which all of the copper atoms exhibit distorted tetrahedral coordination. Compound 2 is monomeric with L bound in the κ3-N,N‘,S mode and a PPh3 molecule that completes the coordination environment. Compound 2 presents a fluxional behavior in CDCl3 solution due to the boat inversion of the six-membered N,N‘ chelate ring (ΔH⧧ = +43.6(3) kJ mol-1, ΔS⧧ = −16(1) J mol-1 K-1). Crystallization of 3 in acetonitrile leads to a polynuclear structure that contains a CH3CN mo...
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