Complexation of uranyl with chelidamic acid: Crystal structures, binding strength, and electrochemical redoxes

Nuclear Analysis Pub Date : 2022-06-01 DOI:10.1016/j.nucana.2022.100014

Xingliang Li, Wanjun Mu, Baihua Chen, Yao He, Jun Tu, Yuchuan Yang, Yanqiu Yang, Hongyuan Wei, Shuming Peng

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Abstract

Chelidamic acid (denoted as H₃L in this paper) is a naturally occurring derivative of dipicolinic acid that functions as a versatile ligand. The complex formation of chelidamic acid with UO₂²⁺ has been investigated by potentiometry in a 0.1 M NaClO₄ solution. The potentiometry identified 1:1 uranyl–chelidamate complexes (UO₂HL, UO₂L₂⁻), 1:2 uranyl–chelidamate complex (UO₂L₂⁴⁻), and a hydrolytic complex UO₂(OH)₂L²⁻. The possible UO₂H₂L₂²⁻ structure was determine by crystal analysis. Chelidamate molecules coordinate to uranyl mainly through the pyridine–carboxylate chelation pocket (O, N, O), and 4-pyridinol–OH group is protonated. The presence of hydrolysate UO₂(OH)₂L^2– was further confirmed by nuclear magnetic resonance spectroscopy (NMR). In an alkaline aqueous medium under anaerobic conditions, the complex U^VIO₂(OH)₂L²⁻can be electrochemically reduced to pentavalent uranyl.

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螯合酸与铀酰的络合:晶体结构、结合强度和电化学氧化

螯合胺酸(本文用H3L表示)是一种天然存在的二吡啶酸衍生物，是一种多功能配体。用电位法研究了在0.1 M氯化钠溶液中螯合酸与UO22+络合物的形成。电位测定法鉴定了1:1的铀酰螯合物(UO2HL, UO2L2−)，1:2的铀酰螯合物(UO2L24−)和水解物UO2(OH)2L2−。通过晶体分析确定了可能的UO2H2L22−结构。螯合酸分子主要通过吡啶-羧酸螯合袋(O, N, O)与铀酰配合，4-吡啶- oh基团被质子化。核磁共振波谱进一步证实了水解产物UO2(OH)2L2 -的存在。在厌氧条件下的碱性水介质中，络合物UVIO2(OH)2L2−可以电化学还原为五价铀酰。

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来源期刊

Nuclear Analysis

CiteScore

1.70

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0.00%

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