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Hexadentate β-Dicarbonyl(bis-catecholamine) Ligands for Efficient Uranyl Cation Decorporation: Thermodynamic and Antioxidant Activity Studies
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2019-10-15 , DOI: 10.1021/acs.inorgchem.9b02306 Qingchun Zhang 1 , Bo Jin 1 , Tian Zheng 1 , Xingyan Tang 2 , Zhicheng Guo 3 , Rufang Peng 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2019-10-15 , DOI: 10.1021/acs.inorgchem.9b02306 Qingchun Zhang 1 , Bo Jin 1 , Tian Zheng 1 , Xingyan Tang 2 , Zhicheng Guo 3 , Rufang Peng 1
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The special linear dioxo cation structure of the uranyl cation, which relegates ligand coordination to an equatorial plane perpendicular to the O═U═O vector, poses an unusual challenge for the rational design of efficient chelating agents. Therefore, the planar hexadentate ligand rational design employed in this work incorporates two bidentate catecholamine (CAM) chelating moieties and a flexible linker with a β-dicarbonyl chelating moiety (β-dicarbonyl(CAM)2 ligands). The solution thermodynamics of β-dicarbonyl(CAM)2 with a uranyl cation was investigated by potentiometric and spectrophotometric titrations. The results demonstrated that the pUO22+ values are significantly higher than for the previously reported TMA(2Li-1,2-HOPO)2, and efficient chelation of the uranyl cation was realized by the planar hexadentate β-dicarbonyl(CAM)2. The efficient chelating ability of β-dicarbonyl(CAM)2 was attributed to the presence of the more flexible β-dicarbonyl chelating linker and planar hexadentate structure, which favors the geometric arrangement between ligand and uranyl coordinative preference. Meanwhile, β-dicarbonyl(CAM)2 also exhibits higher antiradical efficiency in comparison to butylated hydroxyanisole. These results indicated that β-dicarbonyl(CAM)2 has potential application prospects as a chelating agent for efficient chelation of a uranyl cation.
中文翻译：
六齿β-二羰基（双-儿茶酚胺）配体，用于高效铀酰阳离子脱附：热力学和抗氧化活性研究
铀酰阳离子的特殊线性二氧羰基阳离子结构将配体配位降低到垂直于O═U═O载体的赤道平面，这对有效螯合剂的合理设计提出了不寻常的挑战。因此，这项工作中采用的平面六齿配体合理设计结合了两个二齿儿茶酚胺（CAM）螯合部分和一个带有β-二羰基螯合部分（β-二羰基（CAM）2配体）的柔性接头。通过电位滴定法和分光光度滴定法研究了带有铀酰阳离子的β-二羰基（CAM）2的溶液热力学。结果表明，pUO 2 2+值显着高于先前报道的TMA（2Li-1,2-HOPO）2，并通过平面六齿β-二羰基（CAM）2实现了铀酰阳离子的有效螯合。β-二羰基（CAM）2的有效螯合能力归因于更灵活的β-二羰基螯合连接基和平面六齿结构的存在，这有利于配体与铀酰配位偏好之间的几何排列。同时，与丁基化羟基茴香醚相比，β-二羰基（CAM）2还表现出更高的抗自由基效率。这些结果表明，β-二羰基（CAM）2作为用于铀酰阳离子的有效螯合的螯合剂具有潜在的应用前景。
更新日期：2019-10-16
中文翻译：
六齿β-二羰基（双-儿茶酚胺）配体，用于高效铀酰阳离子脱附：热力学和抗氧化活性研究
铀酰阳离子的特殊线性二氧羰基阳离子结构将配体配位降低到垂直于O═U═O载体的赤道平面，这对有效螯合剂的合理设计提出了不寻常的挑战。因此，这项工作中采用的平面六齿配体合理设计结合了两个二齿儿茶酚胺（CAM）螯合部分和一个带有β-二羰基螯合部分（β-二羰基（CAM）2配体）的柔性接头。通过电位滴定法和分光光度滴定法研究了带有铀酰阳离子的β-二羰基（CAM）2的溶液热力学。结果表明，pUO 2 2+值显着高于先前报道的TMA（2Li-1,2-HOPO）2，并通过平面六齿β-二羰基（CAM）2实现了铀酰阳离子的有效螯合。β-二羰基（CAM）2的有效螯合能力归因于更灵活的β-二羰基螯合连接基和平面六齿结构的存在，这有利于配体与铀酰配位偏好之间的几何排列。同时，与丁基化羟基茴香醚相比，β-二羰基（CAM）2还表现出更高的抗自由基效率。这些结果表明，β-二羰基（CAM）2作为用于铀酰阳离子的有效螯合的螯合剂具有潜在的应用前景。
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