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Three different N-donors L, namely N-ethyl-N′-3-pyridyl-imidazolidine-4,5-dione-2-thione (1), N,N′-bis(3-pyridylmethyl)-imidazolidine-4,5-dione-2-thione (2), and tetra-2-pyridyl-pyrazine (3), bearing one, two and four pyridyl substituents, respectively, have been reacted with halogens X2 (X = Br, I) or interhalogens XY (X = I; Y = Cl, Br). CT σ–adducts L · nXY, bearing linear N⋯XY moieties (L = 3; X = I; Y = Br, I; n = 2), and salts containing the protonated cationic donors HnLn+ (L = 1 − 3; n = 1, 2, 4), counterbalanced by Cl−, Br−, I 3 - , Br 3 - , I 5 - , Br 5 - , I2Br−, I 3 Br 4 - , or ICl 2 - anions, have been isolated. Among the reactions products, (H1+)Cl−, (H1+)Br−, ( H 2 + ) I 3 - , ( H 2 3 2 + ) ( ICl 2 - ) 2 , and 3 · 2IBr have been characterised by single-crystal X-ray diffraction. The nature of the products has been elucidated based on elemental analysis and FT-Raman spectroscopy supported by MP2 and DFT calculations. |
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