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脂环族取代基对新型1,10-菲咯啉-2,9-二酰胺家族萃取能力的影响。

The impact of alicyclic substituents on the extraction ability of new family of 1,10-phenanthroline-2,9-diamides.

作者信息

Lemport Pavel S, Matveev Petr I, Yatsenko Alexander V, Evsiunina Mariia V, Petrov Valentine S, Tarasevich Boris N, Roznyatovsky Vitaly A, Dorovatovskii Pavel V, Khrustalev Victor N, Zhokhov Sergey S, Solov'ev Vitaly P, Aslanov Leonid A, Petrov Vladimir G, Kalmykov Stepan N, Nenajdenko Valentine G, Ustyniuk Yuri A

机构信息

Chemistry Department, Lomonosov Moscow State University 119991 Moscow Russia

National Research Center "Kurchatov Institute" Russia.

出版信息

RSC Adv. 2020 Jul 10;10(44):26022-26033. doi: 10.1039/d0ra05182a. eCollection 2020 Jul 9.

Abstract

Development of efficient extractants for the separation of actinides and lanthanides in the technologies of nuclear fuel cycle is one of the most urgent and complex tasks in modern nuclear energetics. New family of 4,7-dichloro-1,10-phenanthroline-2,9-dicarboxylic acid diamides based on cyclic amines was synthesized and shown to exhibit high selectivity in the La/Am pair separation (SF (Am/La ≈ 10)) and in the Am/Eu pair separation (SF (Am/Eu ≈ 12)). It was shown that pyrrolidine derived diamide is more efficient extractant for americium, curium and lanthanides from highly acidic HNO solution than its non-cyclic ,,','-tetraalkyl analogues. The structures of synthesized compounds were studied in details by IR, NMR spectroscopy, and single crystal X-ray diffraction. According to spectroscopy data, incorporation of aromatic rings to the amide fragment of ligand leads to complex dynamic behavior in solutions what is believed to strongly affect the extraction ability of synthesized ligands.

摘要

开发用于核燃料循环技术中锕系元素和镧系元素分离的高效萃取剂是现代核能领域最紧迫和复杂的任务之一。基于环胺合成了新型的4,7-二氯-1,10-菲咯啉-2,9-二羧酸二酰胺系列,并显示出在镧/镅对分离(分离因子SF(镅/镧)≈10)和镅/铕对分离(分离因子SF(镅/铕)≈12)中具有高选择性。结果表明,与非环状的N,N,N',N'-四烷基类似物相比,吡咯烷衍生的二酰胺是从高酸性硝酸溶液中萃取镅、锔和镧系元素更有效的萃取剂。通过红外光谱、核磁共振光谱和单晶X射线衍射对合成化合物的结构进行了详细研究。根据光谱数据,在配体的酰胺片段中引入芳环会导致溶液中复杂的动态行为,据信这会强烈影响合成配体的萃取能力。

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