Leoncini Andrea, Ansari Seraj Ahmad, Mohapatra Prasanta Kumar, Boda Anil, Musharaf Ali Sheikh, Sengupta Arijit, Huskens Jurriaan, Verboom Willem
Molecular Nanofabrication Group, MESA+ Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500 AE Enschede, The Netherlands.
Radiochemistry Division, Bhabha Atomic Research Centre, Mumbai-400085, India.
Dalton Trans. 2017 Jan 31;46(5):1431-1438. doi: 10.1039/c6dt04034a.
Three benzene-centered tripodal diglycolamides (Bz-T-DGAs) were synthesized and evaluated for actinide, lanthanide, and fission product ion extraction. 1,3,5-Triethylbenzene-based tripodal DGA (LI) showed high distribution ratio (D) values for Am and Eu in a mixture of 95% n-dodecane and 5% iso-decanol at 3 M HNO. Eu/Am separation factors, in the range of 8-10, were obtained at 1 M HNO which decreased at higher acidities with the exception of LII which did not show much change. Benzene-1,3,5-triamide-based tripodal DGA (LII) exhibited a high D-value for Pu compared to the other ligands. Slope analysis showed the formation of 1 : 1 or 1 : 2 complexes is dependent on the ligand. The nature of the complexes was further studied with luminescence spectroscopy (Eu complexes) and DFT calculations (Am complexes).
合成了三种以苯为中心的三脚架型二甘醇酰胺(Bz-T-DGAs),并对其进行了锕系元素、镧系元素和裂变产物离子萃取性能评估。基于1,3,5-三乙苯的三脚架型二甘醇酰胺(LI)在3 M硝酸条件下,于95%正十二烷和5%异癸醇的混合体系中对镅和铕显示出较高的分配比(D)值。在1 M硝酸条件下获得的铕/镅分离因子在8 - 10范围内,在较高酸度下该分离因子降低,但LII除外,其变化不大。与其他配体相比,基于苯-1,3,5-三酰胺的三脚架型二甘醇酰胺(LII)对钚显示出较高的D值。斜率分析表明,1∶1或1∶2配合物的形成取决于配体。利用发光光谱(铕配合物)和密度泛函理论计算(镅配合物)进一步研究了配合物的性质。