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首页> 外文期刊>Chemistry: A European journal >Quest for Environmentally Benign Ligands for Actinide Separations: Thermodynamic, Spectroscopic, and Structural Characterization of U-VI Complexes with Oxa-Diamide and Related Ligands
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Quest for Environmentally Benign Ligands for Actinide Separations: Thermodynamic, Spectroscopic, and Structural Characterization of U-VI Complexes with Oxa-Diamide and Related Ligands

机译：寻求用于Ben系元素分离的环境友好的配体：U-VI与氧杂二酰胺和相关配体的配合物的热力学，光谱学和结构表征

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摘要

Complexation of U-VI with N,N,N',N'-tetramethyl-3-oxa-glutaramide (TMOGA) and N,N-dimethyl 3-oxa-glutaramic acid (DMOGA) was Studied in comparison with their dicarboxylate analogue, oxydiacetic acid (ODA). Thermodynamic parameters including stability constants, enthalphy. and entropy of complexation, were determined by spectrophotometry, potentiometry and calorimetry. Single-crystal X-ray diffraction, EXAFS spectroscopy. FT-IR absorption spectroscopy, and laser-induced luninescence spectroscopy were used to obtain structural information on the U-VI complexes. Like ODA, TMOGA and DMOGA form tridentate U-VI complexes, with three oxygen atoms (the amide. ether, and/or carboxylate oxygen) coordinating to the linear UO22+ ion through the equatorial plane. The stability constants, enthalphy, and entropy of complexation all decrease in the order ODA>DMOGA>TMOGA, showing that the complexation is entropy driven and the substitution of a carboxylate group with an amide group reduces the strength of complexation with U-VI due to the decrease in the entropy of complexation. The trend in the thermodynamic stability of the complexes correlates very well with the structural and spectroscopic data obtained by single-crystal X-ray diffraction, FT-IR spectroscopy. and laser-induced luminescence spectroscopy.
机译：研究了U-VI与N，N，N'，N'-四甲基-3-氧杂-戊二酰胺（TMOGA）和N，N-二甲基3-氧杂-戊二酸（DMOGA）的络合，并比较了它们的二羧酸盐类似物，氧二乙酸（ODA）。热力学参数包括稳定性常数，焓。分光光度法，电位法和量热法测定络合度和络合熵。单晶X射线衍射，EXAFS光谱。使用FT-IR吸收光谱和激光诱导的月光光谱来获得有关U-VI配合物的结构信息。像ODA一样，TMOGA和DMOGA形成三齿U-VI络合物，其中三个氧原子（酰胺，醚和/或羧酸氧）通过赤道平面与线性UO22 +离子配位。稳定常数，焓和络合熵均以ODA> DMOGA> TMOGA的顺序降低，表明络合是熵驱动的，而羧酸根基团被酰胺基取代会降低与U-VI的络合强度，这是由于络合熵的降低。配合物的热力学稳定性的趋势与通过单晶X射线衍射，FT-IR光谱获得的结构和光谱数据非常相关。和激光诱导发光光谱。

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