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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >A fluorescence study on the complexation of Sm(III), Eu(III) and Tb(III) with tetraalkyldiglycolamides (TRDGA) in aqueous solution, in solid state, and in solvent extraction
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A fluorescence study on the complexation of Sm(III), Eu(III) and Tb(III) with tetraalkyldiglycolamides (TRDGA) in aqueous solution, in solid state, and in solvent extraction

机译：荧光研究Sm（III），Eu（III）和Tb（III）与四烷基二甘醇酰胺（TRDGA）在水溶液中，固态和溶剂萃取中的络合

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Tetraalkyldiglycolamide (TRDGA) ligands have potential utilization for the separation of actinide and lanthanide ions in the nuclear industry as chelates in aqueous solution if water-soluble or as extractants in organic solvents if water-insoluble. Here, a spectral titration method is extensively applied to investigating the complexation of fluorescent Sm(III), Eu(III), and Tb(III) with TRDGA ligands in aqueous solutions and a solvent extraction system. In aqueous solutions using N, N, N', N'-tetramethyldiglycolamide (TMDGA, L-I) as chelate, three successive complex species of Ln(III), including [LnL(I)](3+), [LnL(2)(I)](3+), and [LnL(3)(I)](3+), are identified for each Ln(III) (Ln = Sm, Eu, and Tb), and their stability constants are determined with fluorescence spectral titration method at 25 degrees C in 1 M NaNO3. The coordination mode in [LnLI 3] 3+ is illustrated by single-crystal structures of the solid compounds LnL(3)(I) (ClO4)(3) (Ln = Sm, Eu, Tb, and L-I = TMDGA) grown from aqueous solutions by slow evaporation. The crystal structures show that in the complexes Ln(III) ions are coordinated by nine oxygen atoms from three tridentate L-I ligands in a distorted tricapped trigonal prism geometry. To provide parallels to solvent extraction chemistry, the extracted Ln(III) complexes with N, N'-dimethyl-N,N'-dioctyldiglycolamide (DMDODGA, L-II, a lipophilic analogue of TMDGA) are prepared, and the fluorescence spectra are collected as well for comparison. The fluorescence spectra of the extracted Ln(III) complexes with LII in an organic phase of 40-60% (v/v) n-octanol-kerosene are nearly identical to the corresponding deconvoluted spectra of [LnL(3)(I)](3+) in aqueous solution. The similarity in fluorescence spectra suggests that Ln(III) ion in the extracted complexes is also coordinated by three tridentate LII ligands and that the nitrate anions acting just as counterions do not directly bond to Ln(III) in the organic phase of solvent extraction.
机译：四烷基二甘醇酰胺（TRDGA）配体具有潜在用途，可用于分离核工业中的in系元素和镧系元素离子（如果是水溶性的话，作为水溶液中的螯合物），或者如果不溶于水的话，作为有机溶剂中的萃取剂。在这里，光谱滴定法被广泛应用于研究荧光Sm（III），Eu（III）和Tb（III）与TRDGA配体在水溶液和溶剂萃取系统中的络合。在使用N，N，N'，N'-四甲基二甘醇酰胺（TMDGA，LI）作为螯合物的水溶液中，Ln（III）的三个连续复杂物种包括[LnL（I）]（3 +），[LnL（2）为每个Ln（III）标识（I）]（3+）和[LnL（3）（I）]（3+）（Ln = Sm，Eu和Tb），并用荧光光谱滴定法在25°C下于1 M NaNO3中进行。 [LnLI 3] 3+中的配位模式由固体化合物LnL（3）（I）（ClO4）（3）（Ln = Sm，Eu，Tb和LI = TMDGA）的单晶结构表示。水溶液通过缓慢蒸发。晶体结构表明，在复合物中，Ln（III）离子由来自三个三齿L-1配体的九个氧原子配成扭曲的三棱柱三角几何形状。为提供与溶剂萃取化学相似的作用，制备了具有N，N'-二甲基-N，N'-二辛基二甘醇酰胺（DMDODGA，L-II，TMDGA的亲脂性类似物）的Ln（III）配合物，并制备了荧光光谱收集并进行比较。萃取的Ln（III）与LII的配合物在40-60％（v / v）正辛醇-煤油的有机相中的荧光光谱与[LnL（3）（I）]的相应解卷积光谱几乎相同（3+）在水溶液中。荧光光谱的相似性表明，提取的络合物中的Ln（III）离子也由三个三齿LII配体协调，而硝酸盐阴离子作为抗衡离子在溶剂提取的有机相中不直接键合至Ln（III）。

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