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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Probing the difference in covalence by enthalpy measurements: a new heterocyclic N-donor ligand for actinide/lanthanide separation
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Probing the difference in covalence by enthalpy measurements: a new heterocyclic N-donor ligand for actinide/lanthanide separation

机译：通过焓测量探讨共价的差异：用于：系元素/镧系元素分离的新型杂环N供体配体

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摘要

Complexation of Am(III), Nd(III), and Eu(III) with a new heterocyclic nitrogen-donor ligand, 2,9-di(quinazolin-2-yl)-1,10-phenanthroline (denoted as BQPhen in this paper), was studied by thermodynamic measurements and theoretical computations. The stability constants of two successive complexes in dimethylformamide, ML3+ and ML23+ where M stands for Nd, Eu, or Am while L stands for the BQPhen ligand, were determined by absorption spectrophotometry. The enthalpy of complexation was determined by microcalorimetry. Results show that BQPhen forms ten times stronger complexes with Am(III) than Eu(III) or Nd(III) under identical conditions, suggesting that BQPhen could be used as an efficient extractant for the separations of trivalent actinides from lanthanides. The higher binding strength of BQPhen towards Am(III) than Nd(III) or Eu(III) is mainly due to the more favourable enthalpy of complexation for Am(III)/BQPhen complexes, implying a higher degree of covalence in the Am(III)/BQPhen complexes than the lanthanide(III)/BQPhen complexes. The thermodynamic trend was corroborated with computational results and validated by solvent extraction experiments that demonstrated BQPhen preferably extracted Am(III) more than Eu(III), with a separation factor of about 10. Discussions have been made to compare BQPhen with other phenanthroline derivatives such as CyMe4-BTPhen, a bis-triazine-phenanthroline derivative that was reported in the literature. Data suggest that, under identical conditions, BQPhen would form stronger complexes with Am(III), Eu(III), and Nd(III) than CyMe4-BTPhen.
机译：Am（III），Nd（III）和Eu（III）与新的杂环氮供体配体2,9-二（喹唑啉-2-基）-1,10-菲咯啉（在此称为BQPhen）的络合本文通过热力学测量和理论计算进行了研究。通过吸收分光光度法测定了二甲基甲酰胺ML3 +和ML23 +中两个连续的配合物的稳定性常数，其中M代表Nd，Eu或Am，L代表BQPhen配体。络合焓通过微量量热法测定。结果表明，在相同条件下，BQPhen与Am（III）形成的络合物比Eu（III）或Nd（III）形成的络合物强十倍，这表明BQPhen可作为从镧系元素中分离三价valent系元素的有效萃取剂。 BQPhen对Am（III）的结合强度比Nd（III）或Eu（III）高，这主要是由于Am（III）/ BQPhen复合物的络合焓更高，这意味着Am（III）中的共价度更高。 III）/ BQPhen复合物比镧系元素（III）/ BQPhen复合物。计算结果证实了该热力学趋势，并通过溶剂萃取实验进行了验证，该实验表明BQPhen提取的Am（III）比Eu（III）多，分离因子约为10。讨论过将BQPhen与其他菲咯啉衍生物进行比较的讨论。名为CyMe4-BTPhen，一种双三嗪-菲咯啉衍生物，已有文献报道。数据表明，在相同条件下，BQPhen与Am（III），Eu（III）和Nd（III）形成比CyMe4-BTPhen更强的复合物。

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