Density functional theoretical modelling was performed to design and screen suitable macrocyclic crown ether functionalized resins for the isotopic enrichment of gadolinium. Theoretical calculations predict the complexation stability order of Gd³⁺ ion as follows: di-cylohexano-18-crown-6 (DCH18C6) > dibenzo-18-crown-6 (DB18C6) > benzo-15-crown-5 (B15C5), which was experimentally verified. The calculated isotopic separation factor value was shown to be the highest for DB18C6. From the theoretical analysis of both the stability and isotopic separation factor, DB18C6 is predicted to be the most promising candidate for isotopic separation of gadolinium. Hence, DB18C6 was functionalized with chloromethylated polystyrene (CMPS) resin. Subsequently, CMPS-grafted DB18C6 resin was synthesized and characterized. Furthermore, isotopic enrichment of gadolinium was carried out by performing column chromatographic experiments using CMPS-DB18C6 resin. The absorption capacity of the novel CMPS-DB18C6 resin for gadolinium was found to be 1 mg g⁻¹. The separation coefficient, ε × 10³, was found to be 6.3, 8.9, 3.4, and 9.7 for Gd-155/158, Gd-156/158, Gd-157/158, and Gd-155/160 isotopic pairs, respectively, and thus hold promise for future isotopic enrichment technology.

中文翻译：

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用于crown同位素富集的功能化冠醚树脂的分子工程：从计算机到柱色谱法†

进行了密度泛函理论建模，以设计和筛选适用于macro同位素富集的大环冠醚官能化树脂。理论计算可预测Gd ³⁺的络合稳定性顺序离子如下：二环己基-18-冠-6（DCH18C6）>二苯并-18-冠-6（DB18C6）>苯并-15-冠-5（B15C5），已通过实验验证。计算出的同位素分离因子值对于DB18C6最高。从稳定性和同位素分离因子的理论分析来看，DB18C6有望成为g同位素分离的最有希望的候选者。因此，DB18C6用氯甲基化的聚苯乙烯（CMPS）树脂进行了功能化。随后，合成并表征了CMPS接枝的DB18C6树脂。此外，通过使用CMPS-DB18C6树脂进行柱色谱实验来进行iso的同位素富集。发现新型CMPS-DB18C6树脂对g的吸收能力为1 mg g ^-1。发现Gd-155 / 158，Gd-156 / 158，Gd-157 / 158和Gd-155 / 160同位素对的分离系数ε ×10 ³分别为6.3、8.9、3.4和9.7 ，因此对未来的同位素富集技术有希望。