Derivatives of (2-Carbamoylethyl)diphenylphosphine Oxides: Synthesis and Extraction Properties toward Actinides and Lanthanides

IF 1.8 3区化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR Russian Journal of Inorganic Chemistry Pub Date : 2024-03-11 DOI:10.1134/s0036023623602751

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Abstract

A series of (2-carbamoylethyl)diphenylphosphine oxides (CEPO) has been synthesized from commercially available reagents: chlorodiphenylphosphine and acrylamides. Effect of coordinating fragments Ph₂P(O)(CH₂)₂C(O), nature of oligoyl group that binds these fragments, and the presence of additional coordinating centers in CEPO on extraction properties toward actinides and lanthanides has been studied. It has been found that N,N′-methylene-bis[3-(diphenylphosphoryl)propionamide] (III) containing two diphenylphosphorylpropionyl fragments bound by rigid HNCH₂NH linker shows the highest efficiency in extraction of actinides (recovery extent is ∼73% for U(VI) and ~85% for Th(IV)), whereas ligand V containing the maximum number of such phosphorylcarbonyl groups in conformationally non-rigid nitrogen heterocyclic matrix and CEPO (II) containing additional C=O group in the alkyl fragment at the nitrogen atom of carbamoyl fragment exhibit considerable preference in the extraction of lanthanides (extraction of gadolinium with this compound is close to 92%). Obtained data display that highly efficient and selective extractants for both 4f and 5f elements can be constructed on the basis of (2-carbamoylethyl)diphenylphosphine oxides.

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(2-氨基甲酰乙基)二苯基氧化膦的衍生物：合成及对锕系元素和镧系元素的萃取特性

摘要利用市售试剂氯二苯基膦和丙烯酰胺合成了一系列（2-氨基甲酰基乙基）二苯基膦氧化物（CEPO）。研究了配位片段 Ph2P(O)(CH2)2C(O)、结合这些片段的低聚酰基的性质以及 CEPO 中附加配位中心的存在对锕系元素和镧系元素萃取特性的影响。研究发现，N,N′-亚甲基双[3-（二苯基磷酰）丙酰胺]（III）含有两个二苯基磷酰丙酰基片段，并通过刚性 HNCH2NH 链接结合，在萃取锕系元素时效率最高（对铀（VI）的回收率为 73%，对钍（IV）的回收率为 85%）、而在构象非刚性氮杂环基质中含有最多此类磷酰羰基的配体 V 和在氨基甲酰基片段的氮原子上的烷基片段中含有额外 C=O 基团的 CEPO (II) 则在镧系元素的萃取中表现出相当大的优势（该化合物对钆的萃取率接近 92%）。所获得的数据表明，可以在（2-氨基甲酰基乙基）二苯基膦氧化物的基础上构建出对 4f 和 5f 元素具有高效选择性的萃取剂。

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来源期刊

Russian Journal of Inorganic Chemistry 化学-无机化学与核化学

CiteScore

3.10

自引率

38.10%

发文量

237

审稿时长

3 months

期刊介绍： Russian Journal of Inorganic Chemistry is a monthly periodical that covers the following topics of research: the synthesis and properties of inorganic compounds, coordination compounds, physicochemical analysis of inorganic systems, theoretical inorganic chemistry, physical methods of investigation, chemistry of solutions, inorganic materials, and nanomaterials.