A new double betaine 1,1′-（propane-1,3-diyl）dipyridinium-4-carboxylate L has been synthesized. Reaction of 1, 1′-（propane-1,3-diyl）dipyridinium-4-carboxylate tetrahydrate 1 with Co（ClO4）2-6H2O leads to the for...A new double betaine 1,1′-（propane-1,3-diyl）dipyridinium-4-carboxylate L has been synthesized. Reaction of 1, 1′-（propane-1,3-diyl）dipyridinium-4-carboxylate tetrahydrate 1 with Co（ClO4）2-6H2O leads to the formation of a new Co（Ⅱ） coordination compound, namely [Co（H2O）6]-2H2O-2L-2ClO4 2. The crystal structures of 1 and 2 have been determined by single-crystal X-ray diffraction method. Crystal data for 1. monoclinic, space group C2/c, a = 18.945（4）, b = 7.700（2）, c = l 1.888（2）A,β = 101.67（3）°, V = 1698.3（6） A^3, Z = 4, F（000） = 760.0, Dc = 1.402 g/cm^3, the final R = 0.0607 and wR = 0.1607 for 950 observed reflections （1 〉 2σ（I））; and those for 2： monoclinic, space group P21/c, a = 17.982（1）, b = 15.879 （1）, c = 7.0716（5）/A,β= 100.675（1）°, V= 1984.3（3） ,A^3 Z= 4, F（000） = 1010.0, Dc = 1.631 g/cm^3, the final R = 0.0316 and wR = 0.0896 for 3784 observed reflections （1 〉20（I））. Crystal structure analysis indicates that in 1, molecules of L in a ＂V-shaped＂ conformation are linked to chains sustained by O-H…O hydrogen bonds between carboxylate groups and solvent water molecules. The chains are joined by O-H…O and C-H…O hydrogen bonds to further expand into a three-dimensional structure. For 2, molecules of L in a ＂Z-shaped＂ conformation are linked by hydrogen bonds between carboxylate groups and aqua ligands to form a chain of loops running down the b axis. The （2D→2D） polythreading in compound 2 represents the mode of parallel interpenetration of 2D sheets, having polyrotaxane character.展开更多
Reaction of 4,4’-(1,4-phenylene)bis(5-acetyl-6-methyl-2-thioxo-1,2-dihydropyridine-3-carbonitrile) (1) with methyl iodide afforded the 4,4’-(1,4-phenylene)bis(5-acetyl-6-methyl-2-(methylthio)nicotinonitrile) (2). Th...Reaction of 4,4’-(1,4-phenylene)bis(5-acetyl-6-methyl-2-thioxo-1,2-dihydropyridine-3-carbonitrile) (1) with methyl iodide afforded the 4,4’-(1,4-phenylene)bis(5-acetyl-6-methyl-2-(methylthio)nicotinonitrile) (2). The reaction of 2 with hydrazine hydrate followed by diazotization reaction af-forded the 1,1’-(1,4-phenylenebis(3-amino-6-methyl-1H-pyrazolo[3,4-b]pyridine-4,5-diyl))bis(e-than-1-one) (3) and 1,1’-(1,4-phenylenebis(3-(chlorodiazenyl)-6-methyl-1H-pyrazolo[3,4-b]-pyridine-4,5-diyl))bis(ethan-1-one) (4) respectively. On the other hand, reaction of 4 with malononitrile, 2-cyanoethanethioamide, ethyl acetoacetate, acetyl acetone, ethyl benzoylacetate, diethylmalonate, ethyl cyanoacetate and phenacylbromide aiming to build up pyrazolotriazine or pyrazole ring on the ring system of 4. Structures of all newly synthesized heterocyclic compounds in the present study were confirmed by considering the data of IR, 1H NMR, mass spectra as well as that of elemental analyses.展开更多
基金This work was financially supported by Liuhui Center for Applied Mathematics, Nankai University and Tianjin University (No. H10114)
文摘A new double betaine 1,1′-（propane-1,3-diyl）dipyridinium-4-carboxylate L has been synthesized. Reaction of 1, 1′-（propane-1,3-diyl）dipyridinium-4-carboxylate tetrahydrate 1 with Co（ClO4）2-6H2O leads to the formation of a new Co（Ⅱ） coordination compound, namely [Co（H2O）6]-2H2O-2L-2ClO4 2. The crystal structures of 1 and 2 have been determined by single-crystal X-ray diffraction method. Crystal data for 1. monoclinic, space group C2/c, a = 18.945（4）, b = 7.700（2）, c = l 1.888（2）A,β = 101.67（3）°, V = 1698.3（6） A^3, Z = 4, F（000） = 760.0, Dc = 1.402 g/cm^3, the final R = 0.0607 and wR = 0.1607 for 950 observed reflections （1 〉 2σ（I））; and those for 2： monoclinic, space group P21/c, a = 17.982（1）, b = 15.879 （1）, c = 7.0716（5）/A,β= 100.675（1）°, V= 1984.3（3） ,A^3 Z= 4, F（000） = 1010.0, Dc = 1.631 g/cm^3, the final R = 0.0316 and wR = 0.0896 for 3784 observed reflections （1 〉20（I））. Crystal structure analysis indicates that in 1, molecules of L in a ＂V-shaped＂ conformation are linked to chains sustained by O-H…O hydrogen bonds between carboxylate groups and solvent water molecules. The chains are joined by O-H…O and C-H…O hydrogen bonds to further expand into a three-dimensional structure. For 2, molecules of L in a ＂Z-shaped＂ conformation are linked by hydrogen bonds between carboxylate groups and aqua ligands to form a chain of loops running down the b axis. The （2D→2D） polythreading in compound 2 represents the mode of parallel interpenetration of 2D sheets, having polyrotaxane character.
文摘Reaction of 4,4’-(1,4-phenylene)bis(5-acetyl-6-methyl-2-thioxo-1,2-dihydropyridine-3-carbonitrile) (1) with methyl iodide afforded the 4,4’-(1,4-phenylene)bis(5-acetyl-6-methyl-2-(methylthio)nicotinonitrile) (2). The reaction of 2 with hydrazine hydrate followed by diazotization reaction af-forded the 1,1’-(1,4-phenylenebis(3-amino-6-methyl-1H-pyrazolo[3,4-b]pyridine-4,5-diyl))bis(e-than-1-one) (3) and 1,1’-(1,4-phenylenebis(3-(chlorodiazenyl)-6-methyl-1H-pyrazolo[3,4-b]-pyridine-4,5-diyl))bis(ethan-1-one) (4) respectively. On the other hand, reaction of 4 with malononitrile, 2-cyanoethanethioamide, ethyl acetoacetate, acetyl acetone, ethyl benzoylacetate, diethylmalonate, ethyl cyanoacetate and phenacylbromide aiming to build up pyrazolotriazine or pyrazole ring on the ring system of 4. Structures of all newly synthesized heterocyclic compounds in the present study were confirmed by considering the data of IR, 1H NMR, mass spectra as well as that of elemental analyses.
