Condensation of ortho-phenylene diamines with an unsymmetrical 2,6Ј-bipyridyl-2ЈЈ-pyridyl α-diketone (2) affords helical ligands 3a and 3b that self-assemble in the presence of copper (i)
The tetra-substituted TTF-type donors 4,4Ј,5,5Ј-tetrakis(2-pyridylethylsulfanyl)tetrathiafulvalene (1) and 4,4Ј,5,5Ј-tetrakis(2-pyrazylethylsulfanyl)tetrathiafulvalene (2) were prepared and characterized. These donors show a redox behaviour that is comparable with similar unsubstituted TTF donors, with a small increase of the redox potentials due to the electron-withdrawing effect of the pyridine and pyrazine groups. Single crystal X-ray diffraction analyses show structures with a strong segregation of TTF and azo moieties. The
Condensation of 1,2-diamino-4,5-bis(n-alkoxy)arenes with an oligopyridyl-type alpha-diketone afforded a series of long-chain pyridine-quinoxaline hybrids. These were evaluated for their ability to self-assemble with tetrahedral Cu(I) and Ag(I) to form dimeric, double-decker amphiphillic complexes having a flattened metallocyclophane topology. Detailed NOESY and T1 relaxation time experimentation showed that the configuration of the dicopper(I) complexes corresponds to inversion (meso) symmetry, which leads to an extended molecular shape, wherein the alkoxy chains of the individual ligand components lie on opposite sides of the metallocyclophane core, as opposed to the same side. Preliminary measurements show that the disilver(I) complexes having nC12H25 and nC18H37 chains exhibit reversible melting processes and undergo two endothermic transitions each, at 189/237 and 59/80 degrees C, respectively.
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