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首页> 外文期刊>Polyhedron: The International Journal for Inorganic and Organometallic Chemistry >Exploring competitive metal binding and crystallization of UO22+ and Cu2+ tetrahydrofuran-2,3,4,5-tetracarboxylic acid complexes
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Exploring competitive metal binding and crystallization of UO22+ and Cu2+ tetrahydrofuran-2,3,4,5-tetracarboxylic acid complexes

机译：探索UO22 +和Cu2 +四氢呋喃-2,3,4,5-四羧酸复合物的竞争性金属结合和结晶

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摘要

Solvent extractions are used to separate actinide elements from fission products in nuclear waste streams and the successful isolation of specific species utilize subtle differences in metal ligand binding. Metal ligand binding is also important in crystallization of metal organic materials and herein we explore the importance of competitive binding in the tetrahydrofuran-2,3,4,5-tetracarboxylic acid (THFTCA) system. This ligand has been previously evaluated for the selective extraction of uranium from other lanthanides and actinides and in the current study, we evaluate the crystallization of uranyl-THFTCA complexes in the presence of Cu2+, Sr2+, Th4+, and Ce3+. Three major phases were formed in the crystallization experiments and characterized with single crystal X-ray diffraction, powder X-ray diffraction, thermogravimetric analysis, and Raman spectroscopy. Two of the resulting phases were novel (UTHF1 ((C4H10N2)[UO2(C8H8O9)(2)]center dot 2H(2)O) and UTHF2 (Na[(UO2)(C8H5O9)(H2O)]center dot 3.5 H2O)), whereas the third (CuTHF1) was previously reported in the literature. Raman spectroscopy was utilized to evaluate spectral changes in the mother liquor of UTHF1, UTHF2, and CuTHF1 over time to assess the crystallization process. Further, isothermal titration calorimetry was used to determine the binding constants for UO22+ and Cu2+ to the THFTCA ligand in solution and evaluate the role of competitive metal binding in this system. The thermodynamic parameters and the crystallographic data were used to justify the formation of a weaker UO22+-THFTCA complex. Formation of a weaker UO22+-THFTCA complex supports our findings that UTHF1 only forms in homomeric systems, but suggests that the crystallization of UTHF2 and CuTHF1 is reliant on the presence of additional counter ions and ligands to change the amount of available THFTCA ligand. (C) 2020 Elsevier Ltd. All rights reserved.
机译：溶剂萃取用于从核废物流中的裂变产物中分离锕系元素，并利用金属-配体结合的细微差异成功分离特定物种。金属配体结合在金属有机材料的结晶过程中也很重要，本文探讨了四氢呋喃-2,3,4,5-四羧酸（THFTCA）体系中竞争结合的重要性。该配体之前已被评估用于从其他镧系元素和锕系元素中选择性萃取铀，在当前的研究中，我们评估了在Cu2+、Sr2+、Th4+和Ce3+存在的情况下铀酰-THFTCA络合物的结晶。结晶实验中形成了三个主要相，并用单晶X射线衍射、粉末X射线衍射、热重分析和拉曼光谱对其进行了表征。其中两个相是新的（UTHF1（（C4H10N2）[UO2（C8H8O9）（2）]中心点2H（2）O）和UTHF2（Na[（UO2）（C8H5O9）（H2O）]中心点3.5 H2O）），而第三个相（CuTHF1）之前已在文献中报道过。拉曼光谱用于评估UTHF1、UTHF2和CuTHF1母液随时间的光谱变化，以评估结晶过程。此外，采用等温滴定量热法测定溶液中UO22+和Cu2+与THFTCA配体的结合常数，并评估竞争性金属结合在该体系中的作用。热力学参数和晶体学数据被用来证明较弱的UO22+-THFTCA络合物的形成。较弱的UO22+-THFTCA复合物的形成支持我们的发现，即UTHF1仅在均聚体系中形成，但表明UTHF2和CuTHF1的结晶依赖于额外的反离子和配体的存在来改变可用的THFTCA配体的数量。（C） 2020爱思唯尔有限公司版权所有。

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