Department of Chemical & Biological Sciences, University of Huddersfield, Queensgate, Huddersfield, UK HD1 3DH.
Dalton Trans. 2011 Aug 7;40(29):7610-6. doi: 10.1039/c1dt10634a. Epub 2011 Jun 24.
A series of 1-alkyl-4-aryl-1,2,3-triazoles (1-methyl-4-phenyl-1,2,3-triazole (1a); 1-propyl-4-phenyl-1,2,3-triazole (1b); 1-benzyl-4-phenyl-1,2,3-triazole (1c); 1-propyl-4-p-tolyl-1,2,3-triazole (1d)) have been prepared through a one-pot procedure involving in situ generation of the alkyl azide from a halide precursor followed by copper catalysed alkyne/azide cycloaddition (CuAAC) with the appropriate aryl alkyne. Cationic Re(I) complexes [Re(bpy)(CO)(3)(1a-d)]PF(6) (2a-d) were then prepared by stirring [Re(bpy)(CO)(3)Cl] with AgPF(6) in dichloromethane in the presence of ligands 1a-d. X-ray crystal structures were obtained for 2a and 2b. In the solid state, 2a adopts a highly distorted geometry, which is not seen for 2b, in which the plane of the triazole ligand tilts by 13° with respect to the Re-N bond as a result of a π-stacking interaction between the Ph substituent and one of the rings of the bpy ligand. This π-stacking interaction also results in severe twisting of the bpy ligand. Infrared spectra of 2a-d exhibit ν(CO) bands at ∼2035 and ∼1926 cm(-1) suggesting that these ligands are marginally better donors than pyridine (ν(CO) = 2037, 1932 cm(-1)). The complexes are luminescent in aerated dichloromethane at room temperature with emission maxima at 542 to 552 nm comparable to that of the pyridine analogue (549 nm) and blue shifted relative to the parent chloride complex. Long luminescent lifetimes are observed for the triazole complexes (475 to 513 ns) in aerated dichloromethane solutions at room temperature.
通过一锅法制备了一系列 1-烷基-4-芳基-1,2,3-三唑(1-甲基-4-苯基-1,2,3-三唑(1a);1-丙基-4-苯基-1,2,3-三唑(1b);1-苯甲基-4-苯基-1,2,3-三唑(1c);1-丙基-4-对甲苯基-1,2,3-三唑(1d)),方法涉及卤化物前体原位生成烷基叠氮化物,然后通过铜催化的炔烃/叠氮化物环加成(CuAAC)与合适的芳基炔烃反应。然后通过搅拌[Re(bpy)(CO)(3)(1a-d)]PF 6(2a-d)在二氯甲烷中用 AgPF 6 制备阳离子 Re(I)配合物[Re(bpy)(CO)(3)Cl]与配体 1a-d。获得了 2a 和 2b 的晶体结构。在固态中,2a 采用高度扭曲的几何形状,而 2b 则不存在,其中三唑配体相对于 Re-N 键倾斜 13°,这是由于 Ph 取代基与 bpy 配体的一个环之间的π堆积相互作用所致。这种π堆积相互作用还导致 bpy 配体严重扭曲。2a-d 的红外光谱在∼2035 和∼1926 cm-1 处显示出ν(CO)带,表明这些配体比吡啶(ν(CO)= 2037、1932 cm-1)略微更好的供体。在室温下,在有氧的二氯甲烷中,这些配合物具有发光性,发射最大值在 542 至 552 nm 之间,与吡啶类似物(549 nm)相当,并相对于母体氯化物配合物发生蓝移。在有氧的二氯甲烷溶液中,三唑配合物在室温下具有长的发光寿命(475 至 513 ns)。