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Synthesis, Characterization, and Studies of Coordination-Polymeres With Isomeric Pyridylcyanoximes: Route to Metal Ribbons With Very Short TI...TI Separations
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DOI：10.1021/cg3000763.png)
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Abstract
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Two isomeric pyridylcyanoximes, H(3PCO) and H(4PCO), containing nitrogen atoms of the heterocycle at 3- and 4-positions, respectively, were synthesized and thoroughly characterized using IR (including N-15 labeling), UV-visible, H-1,C-13 one- and two-dimensional NMR spectroscopy, and X-ray analysis. The H(3PCO) exists as a mixture of syn- and anti-isomers in solutions, contrary to H(4PCO) which is present only as an antiisomer. Both compounds have planar geometry in the solid state and form elegant zigzag chains via H-bonding between the oxime group and the N-atom of the heterocycle. The H(3PCO) and H(4PCO) upon addition of a base form colored conjugated and solvatochromic anions in solutions. The reaction of the hot aqueous solution of TI2CO3 with solid isomeric pyridylcyanoximes leads to TIL, which were characterized by elemental analyses, IR spectroscopy, and X-ray analysis. Both complexes represent three-dimensional coordination polymers of different complexities where cyanoxime anions act as bridging ligands. Thallium(I) atoms in TI(3PCO) and TI(4PCO) form infinite, planar metal ribbons with unusually short intermetallic distances: 3.705 angstrom in TI(3PCO) and 3.635 angstrom in TI(4PCO) respectively, which are close to that in metallic thallium (3.465 angstrom). The latter compound has the second shortest TI...TI thallophillic interaction reported in the literature thus far. Both yellow TI(3PCO) and orange TI(4PCO) are insulators at ambient conditions: R similar to I X 10(11) Ohm.
Keywords:
MOLECULAR-STRUCTURE
2/4-NITROPHENOXIDE COMPLEXES
STRUCTURAL SYSTEMATICS
SECONDARY INTERACTIONS
ELECTRICAL-CONDUCTION
2-ELECTRON TRANSFER
CRYSTAL-STRUCTURES
PLATINUM
TL
TRANSITION
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