Bin Li, Ludi Wang, Yu Kang, Hong Cao, Yaoyang Liu, Qiange He, Zhongfeng Li, Xiaoyan Tang, Jing Chen, Li Wang* and Chao Xu*,
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引用次数: 0
摘要
亲水性锕系元素掩蔽剂被认为是一种有效的替代品,可以避免在核废料管理的液液萃取过程中通常使用的大量有害有机溶剂/稀释剂。然而,亲水配体的实际应用在合成/纯化程序方面面临着巨大挑战,更重要的是配体本身的耐酸性。在本文中,我们证明了菲罗啉二亚胺框架与组氨酸侧翼部分的生物特征相结合,可以在超过 1 M HNO3 的高酸度条件下实现三价镧系元素/锕系元素(也包括锕系元素/锕系元素)的高效分离。这种方法利用了 N、O-杂化配体的软硬配位特性,以及在能量上有利于金属配位的酰亚胺和组氨酸的多重质子化。这些因素共同促成了一种易于获得、水溶性强、选择性高且耐酸的 Am(III)掩蔽剂的合成。因此,我们在本文中表明,通过将合成的 N、O-杂化配体与氨基酸适当结合,可以以更可持续的方式有效实现三价镧系和锕系元素的分离。
Amino Acid Decorated Phenanthroline Diimide as Sustainable Hydrophilic Am(III) Masking Agent with High Acid Resistance
Hydrophilic actinide masking agents are believed to be efficient alternatives to circumvent the extensive hazardous organic solvents/diluents typically employed in the liquid–liquid extraction for nuclear waste management. However, the practical application of hydrophilic ligands faces significant challenges in both synthetic/purification procedures and, more importantly, the acid resistance of the ligands themselves. Herein, we have demonstrated the combination of phenanthroline diimide framework with a biomotif of histidine flanking parts could achieve efficient separation of trivalent lanthanides/actinides (also actinides/actinides) under high acidity of over 1 M HNO3. This approach leverages the soft–hard coordination properties of N, O-hybrid ligands, as well as the energetically favored imides for metal coordination and the multiple protonation of histidine. These factors collectively contribute to the synthesis of an easily accessible, highly water-soluble, superior selective, and acid-resistant Am(III) masking agent. Thus, we have shown in this paper, by proper combination of synthetic N, O-hybrid ligand with amino acid, trivalent lanthanide and actinide separation could be efficiently fulfilled in a more sustainable manner.