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首页> 外文期刊>Chemistry: A European journal >Experimental and theoretical approaches toward anion-responsive tripod-lanthanide complexes: Mixed-donor ligand effects on lanthanide complexation and luminescence sensing profiles
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Experimental and theoretical approaches toward anion-responsive tripod-lanthanide complexes: Mixed-donor ligand effects on lanthanide complexation and luminescence sensing profiles

机译：阴离子反应性三脚架镧系元素络合物的实验和理论方法：混合给体配体对镧系元素络合物和发光传感曲线的影响

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摘要

A new series of tripods were designed to form anion-responsive, luminescent lanthanide complexes. These tripods contain pyridine, thiazole, pyrazine, or quinoline chromophores combined with amide carbonyl oxygen and tertiary nitrogen atoms. Crystallographic and EXAFS studies of the 10-coordinated tripod-La(NO3)(3) complexes revealed that each La3+ cation was cooperatively coordinated by one tetradentate tripod and three bidentate NO3- anions in the crystal and in CH3CN. Quantum chemical calculations indicated that the aromatic nitrogen plays a significant role in lanthanide complexation. The experimentally determined stability constants of complexes of the tripod with La(NO3)(3), Eu(NO3)(3), and Tb(NO3)(3) were in good agreement with the theoretically calculated interaction energies. Complexation of each tripod with lanthanide triflate gave a mixture of several lanthanide complex species. Interestingly, the addition of a coordinative NO3- or Cl- anion to the mixture significantly influenced the lanthanide complexation profiles. The particular combination of tripod and a luminescent Eu3+ center gave anion-selective luminescence enhancements. Pyridine-containing tripods exhibited the highest NO3- anion-selective luminescence and thus permit naked-eye detection of the NO3- anion.
机译：设计了一系列新的三脚架，以形成对阴离子敏感的发光镧系元素络合物。这些三脚架包含吡啶，噻唑，吡嗪或喹啉发色团，并结合了酰胺羰基氧和叔氮原子。晶体学和EXAFS研究10配位的三脚架La（NO3）（3）配合物表明，每个La3 +阳离子由晶体和CH3CN中的一个四齿三脚架和三个二齿NO3-阴离子协同配位。量子化学计算表明，芳族氮在镧系元素络合中起重要作用。实验确定的三脚架与La（NO3）（3），Eu（NO3）（3）和Tb（NO3）（3）的配合物的稳定常数与理论计算的相互作用能高度吻合。每个三脚架与三氟化镧镧系元素的络合得到几种镧系元素络合物的混合物。有趣的是，向混合物中添加配位NO3-或Cl-阴离子显着影响了镧系元素的络合曲线。三脚架和发光的Eu3 +中心的特定组合增强了阴离子选择性发光。含吡啶的三脚架表现出最高的NO3-阴离子选择性发光，因此可以肉眼检测NO3-阴离子。

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